Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few...Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.展开更多
The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuni...The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.展开更多
Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective stra...Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective strategy to in situ grow a layer of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)composite on the nickel foam(NF)collector,where Ti_(3)C_(2)T_(x)is not only a conductive component,but also a catalyst that accelerates the oxidation of NF to Ni(OH)_(2).Detailed analysis reveals that the crystallinity,morphology,and electronic structure of the integrated electrode can be tuned via the electrochemical activation,which is beneficial for improving electrical conductivity and redox activity.As expected,the integrated electrode shows a specific capacity of 1.09 C cm^(-2)at 1 mA cm^(-2)after three custom activation cycles and maintains 92.4%of the initial capacity after 1500 cycles.Moreover,a hybrid supercapacitor composed of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)/NF cathode and activated carbon anode provides an energy density of 0.1 mWh cm^(-2)at a power density of 0.97 mW cm^(-2),and excellent cycling stability with about 110%capacity retention rate after 5000 cycles.This work would afford an economical and convenient method to steer commercial Ni foam into advanced Ni(OH)_(2)-based composite materials as binder-free electrodes for hybrid supercapacitors.展开更多
Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamic...Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamics and kinetic properties pose major challenges for their engineering applications.Herein,we review the recent progress in improving their thermodynamics and kinetics,with an emphasis on the models and the influence of various parameters in the calculated models.Subsequently,the impact of alloying,composite,and nanocrystallization on both thermodynamics and dynamics are discussed in detail.In particular,the correlation between various modification strategies and the hydrogen capacity,dehydrogenation enthalpy and temperature,hydriding/dehydriding rates are summarized.In addition,the mechanism of hydrogen storage processes of Mg-based materials is discussed from the aspect of classical kinetic theories and microscope hydrogen transferring behavior.This review concludes with an outlook on the remaining challenge issues and prospects.展开更多
Exploring highly active and stable transition metal-based bifunctional electrocatalysts has recently attracted extensive research interests for achieving high inherent activity, abundant exposed active sites, rapid ma...Exploring highly active and stable transition metal-based bifunctional electrocatalysts has recently attracted extensive research interests for achieving high inherent activity, abundant exposed active sites, rapid mass transfer, and strong structure stability for overall water splitting. Herein, an interface engineering coupled with shell-protection strategy was applied to construct three-dimensional(3D) core-shell NixSy@MnOxHy heterostructure nanorods grown on nickel foam(NixSy@MnOxHy/NF) as a bifunctional electrocatalyst. NixSy@MnOxHy/NF was synthesized via a facile hydrothermal reaction followed by an electrodeposition process. The X-ray absorption fine structure spectra reveal that abundant Mn-S bonds connect the heterostructure interfaces of N ixSy@MnOxHy, leading to a strong electronic interaction, which improves the intrinsic activities of hydrogen evolution reaction and oxygen evolution reaction(OER). Besides, as an efficient protective shell, the MnOxHy dramatically inhibits the electrochemical corrosion of the electrocatalyst at high current densities, which remarkably enhances the stability at high potentials. Furthermore, the 3D nanorod structure not only exposes enriched active sites, but also accelerates the electrolyte diffusion and bubble desorption. Therefore, NixSy@MnOxHy/NF exhibits exceptional bifunctional activity and stability for overall water splitting, with low overpotentials of 326 and 356 mV for OER at 100 and 500 mA cm^(–2), respectively, along with high stability of 150 h at 100 mA cm^(–2). Furthermore, for overall water splitting, it presents a low cell voltage of 1.529 V at 10 mA cm^(–2), accompanied by excellent stability at 100 mA cm^(–2) for 100 h. This work sheds a light on exploring highly active and stable bifunctional electrocatalysts by the interface engineering coupled with shell-protection strategy.展开更多
Hydrogen,a renewable and outstanding energy carrier with zero carbon dioxide emission,is regarded as the best alternative to fossil fuels.The most preferred route to large-scale production of hydrogen is by water elec...Hydrogen,a renewable and outstanding energy carrier with zero carbon dioxide emission,is regarded as the best alternative to fossil fuels.The most preferred route to large-scale production of hydrogen is by water electrolysis from the intermittent sources(e.g.,wind,solar,hydro,and tidal energy).However,the efficiency of water electrolysis is very much dependent on the activity of electrocatalysts.Thus,designing high-effective,stable,and cheap materials for hydrogen evolution reaction(HER)could have a substantial impact on renewable energy technologies.Recently,single-atom catalysts(SACs)have emerged as a new frontier in catalysis science,because SACs have maximum atom-utilization efficiency and excellent catalytic reaction activity.Various synthesis methods and analytical techniques have been adopted to prepare and characterize these SACs.In this review,we discuss recent progress on SACs synthesis,characterization methods,and their catalytic applications.Particularly,we highlight their unique electrochemical characteristics toward HER.Finally,the current key challenges in SACs for HER are pointed out and some potential directions are proposed as well.展开更多
Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bif...Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.展开更多
Compared with commercial lithium batteries with liquid electrolytes,all-solidstate lithium batteries(ASSLBs)possess the advantages of higher safety,better electrochemical stability,higher energy density,and longer cyc...Compared with commercial lithium batteries with liquid electrolytes,all-solidstate lithium batteries(ASSLBs)possess the advantages of higher safety,better electrochemical stability,higher energy density,and longer cycle life;therefore,ASSLBs have been identified as promising candidates for next-generation safe and stable high-energy-storage devices.The design and fabrication of solid-state electrolytes(SSEs)are vital for the future commercialization of ASSLBs.Among various SSEs,solid polymer composite electrolytes(SPCEs)consisting of inorganic nanofillers and polymer matrix have shown great application prospects in the practice of ASSLBs.The incorporation of inorganic nanofillers into the polymer matrix has been considered as a crucial method to achieve high ionic conductivity for SPCE.In this review,the mechanisms of Li+transport variation caused by incorporating inorganic nanofillers into the polymer matrix are discussed in detail.On the basis of the recent progress,the respective contributions of polymer chains,passive ceramic nanofillers,and active ceramic nanofillers in affecting the Li+transport process of SPCE are reviewed systematically.The inherent relationship between the morphological characteristics of inorganic nanofillers and the ionic conductivity of the resultant SPCE is discussed.Finally,the challenges and future perspectives for developing high-performance SPCE are put forward.This review aims to provide possible strategies for the further improvement of ionic conductivity in inorganic nanoscale filler-reinforced SPCE and highlight their inspiration for future research directions.展开更多
The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity...The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.展开更多
Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble m...Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble metal‐based hybrid catalyst which consists of binary FeNi alloy/nitride nanocrystals with graphitic‐shell and biomass‐derived N‐doped carbon(NC)(FexNiyN@C/NC).This novel nanostructure exhibits superior performance for ORR/OER,which can be attributed to the strong interactions between the graphitic‐shell encapsulated FeNi alloy/nitride nanocrystals and the N‐doped porous carbon substrate.The X‐ray absorption spectroscopy technique was employed to reveal the underlying mechanisms for the excellent performance.The assembled Zn‐air battery device exhibits outstanding charging/discharging performance and cycling stability,indicating the great potential of this type of novel catalysts.展开更多
Perforin is a pore-forming protein engaged mainly in mediating target T cell death and is employed by cytotoxic T lymphocytes （CTLs） and natural killer cells. However, whether it also plays a role in conventional C...Perforin is a pore-forming protein engaged mainly in mediating target T cell death and is employed by cytotoxic T lymphocytes （CTLs） and natural killer cells. However, whether it also plays a role in conventional CD4^＋ T cell function remains unclear. Here we report that in perforin-deficient （PKO） mice, CD4^＋ T cells are hyperproliferative in response to T cell receptor （TCR） stimulation. This feature of hyperproliferation is accompanied by the enhancement both in cell division and in IL-2 secretion. It seems that the perforin deficiency does not influence T cell development in thymus spleen and lymph node. In vivo, perforin deficiency results in increased antigen-specific T cell proliferation and antibody production. Furthermore, PKO mice are more susceptible to experimental autoimmune uveitis. To address the molecular mechanism, we found that after TCR stimulation, CD4^＋ T cells from PKO mice display an increased intracellular calcium flux and subsequently enhance activation of transcription factor NFAT1. Our results indicate that perforin plays a negative role in regulating CD4^＋ T cell activation and immune response by affecting TCR-dependent Ca^2＋ signaling.展开更多
Oxygen reduction reaction(ORR)is an important electrochemical process for renewable energy conversion and storage applications such as fuel cells and metal-air batteries.ORR is sluggish in kinetics and requires a larg...Oxygen reduction reaction(ORR)is an important electrochemical process for renewable energy conversion and storage applications such as fuel cells and metal-air batteries.ORR is sluggish in kinetics and requires a large amount of platinum group metal(PGM)-based catalysts to facilitate its slow reaction rate.Application of precious metals raises the cost and decreases the competitivity of these devices in the market.To address this challenge,PGM-free ORR catalysts have been intensively investigated as an alternative to replace the PGM-based catalysts and to promote the deployment of ORR-related applications.In particular,the biomass holds promising potential to be used as the precursor material for PGM-free ORR catalysts.This pathway has gained more and more attention in recent years.In this review,recent advances regarding biomass-derived ORR catalysts are summarized with a focus on the rational design of both active sites and porous structures which are the two key factors in determining ORR performance of catalysts.At the end,the perspectives of development of biomass-derived catalysts is discussed.展开更多
Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement.Unlike the previously reported singleatom or dual-atom configura...Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement.Unlike the previously reported singleatom or dual-atom configurations,we designed a new type of binary-atom catalyst,through engineering Fe-N_(4)electronic structure with adjacent Co-N_(2)C_(2)and nitrogen-coordinated Co nanoclusters,as oxygen electrocatalysts.The resultant optimized electronic structure of the Fe-N_(4)active center favors the binding capability of intermediates and enhances oxygen reduction reaction(ORR)activity in both alkaline and acid conditions.In addition,anchoring M-N-C atomic sites on highly graphitized carbon supports guarantees of efficient charge-and mass-transports,and escorts the high bifunctional catalytic activity of the entire catalyst.Further,through the combination of electrochemical studies and in-situ X-ray absorption spectroscopy analyses,the ORR degradation mechanisms under highly oxidative conditions during oxygen evolution reaction processes were revealed.This work developed a new binary-atom catalyst and systematically investigates the effect of highly oxidative environments on ORR electrochemical behavior.It demonstrates the strategy for facilitating oxygen electrocatalytic activity and stability of the atomically dispersed M-N-C catalysts.展开更多
It is important to understand the pathogenesis of asthma induced by natural allergens, which could exclude the interference of artificial adjuvant and provide insights of natural immune response in the disease. In the...It is important to understand the pathogenesis of asthma induced by natural allergens, which could exclude the interference of artificial adjuvant and provide insights of natural immune response in the disease. In the present study, we show that Trichosanthin （TCS） could induce airway inflammation even without the help of alum. Furthermore, TCS appeared capable of replacing alum to promote OVA-specific airway inflammation. TCS induced accumulation of IL-4-producing eosinophils in peritoneum at an early stage and the adjuvant function of TCS was eliminated by blockage of IL-4 at this stage. Finally, the eosinophils triggered by TCS from WT mice, but not from IL-4- deficient mice were shown to function as adjuvant for the induction of OVA-specific Th2 responses. Our data indicate that TCS is not only an allergen, but also a Th2-typc adjuvant modulating the switching of immune responses to a Th2 pathway. This chain of events results from IL-4 production by eosinophils at an early stage of TCS-priming. In conclusion, TCS may be useful as a Th2 adjuvant, and innate immune cells, such as eosinophils, may be a good target to study the initiation of Th2 response.展开更多
Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivit...Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.展开更多
Atomic scale engineering of materials and interfaces has become increasingly important in material manufacturing.Atomic layer deposition(ALD)is a technology that can offer many unique properties to achieve atomic-scal...Atomic scale engineering of materials and interfaces has become increasingly important in material manufacturing.Atomic layer deposition(ALD)is a technology that can offer many unique properties to achieve atomic-scale material manufacturing controllability.Herein,we discuss this ALD technology for its applications,attributes,technology status and challenges.We envision that the ALD technology will continue making significant contributions to various industries and technologies in the coming years.展开更多
Cathode catalysts for direct alcohol fuel cells(DAFCs) must have high catalytic activity for the oxy-gen reduction reaction(ORR), low cost, and high tolerance to the presence of methanol or ethanol. Pt is the benchmar...Cathode catalysts for direct alcohol fuel cells(DAFCs) must have high catalytic activity for the oxy-gen reduction reaction(ORR), low cost, and high tolerance to the presence of methanol or ethanol. Pt is the benchmark catalyst for this application owing to its excellent electrocatalytic activity, but its high cost and low tolerance to the organic fuel permeating through the membrane have hindered the commercialization of DAFCs. Herein we present a facile synthesis route to obtain organic fuel-tolerant Zr- and Ta-based catalysts supported on carbon. This method consists of a simple precipitation of metal precursors followed by a heat treatment. X-ray diffraction analyses confirmed that the obtained samples were crystalline ZrO 2-x and Na2Ta8O21-x having crystallite sizes of 26 and 32 nm, respectively. The thermal treatment effectively increased the activity of the catalysts to-wards the ORR, although further optimization is necessary. Both catalysts exhibited a high tolerance to the presence of methanol with only a moderate reduction in ORR activity even at high methanol concentration(0.5 mol/L).展开更多
When I read the paper“Electrolytes enriched by potassium perfluorinated sulfonates for lithium metal batteries”from Prof.Jianmin Ma’s group,which was published in Science Bulletin(doi.org/10.1016/j.scib.2020.09.018...When I read the paper“Electrolytes enriched by potassium perfluorinated sulfonates for lithium metal batteries”from Prof.Jianmin Ma’s group,which was published in Science Bulletin(doi.org/10.1016/j.scib.2020.09.018),I felt excited as presented a multi-factor principle for applying potassium perfluorinated sulfonates to suppress the dendrite growth and protect the cathode from the viewpoint of electrolyte additives.The effects of these additives are revealed through experimental results,molecular dynamics simulations and first-principle calculations.Specifically,it involves the influence of additives on Li^(+)solvation structure,solid electrolyte interphase(SEI),Li growth and nucleation.Following the guidance of the multi-factor principle,every part of the additive molecule should be utilized to regulate electrolytes.This multifactor principle for electrolyte additive molecule design(EAMD)offers a unique insight on understanding the electrochemical behavior of iontype electrolyte additives on both the Li metal anode and high-voltage cathode.In these regards,I would be delighted to write a highlight for this innovative work and,hopefully,it may raise more interest in the areas of electrolyte additives.展开更多
Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel ce...Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.展开更多
Aging increases the risk ofliver diseases and systemic susceptibility to aging-related diseases.However,cell type-specific changes and the underlying mechanism of liver aging in higher vertebrates remain incompletely ...Aging increases the risk ofliver diseases and systemic susceptibility to aging-related diseases.However,cell type-specific changes and the underlying mechanism of liver aging in higher vertebrates remain incompletely characterized.Here,we constructed the first single-nucleus transcriptomic landscape of primate liver aging,in which we resolved cell type-specific gene expression fluctuation in hepatocytes across three liver zonations and detected aberrant cell-cell interactions between hepatocytes and niche cells.Upon in-depth dissection of this rich dataset,we identifed impaired lipid metabolism and upregulation of chronic inflammation-related genes prominently associated with declined liver functions during aging.In particular,hyperactivated sterol regulatory element-binding protein(SREBP)signaling was a hallmark of the aged liver,and consequently,forced activation of SREBP2 in human primary hepatocytes recapitulated in vivo aging phenotypes,manifesting as impaired detoxification and accelerated cellular senescence.This study expands our knowledge of primate liver aging and informs the development of diagnostics and therapeutic interventions for liver aging and associated diseases.展开更多
基金Natural Sciences and Engineering Research Council of Canada (NSERC)Fonds de Recherche du Québec-Nature et Technologies (FRQNT)+3 种基金Centre Québécois sur les Materiaux Fonctionnels (CQMF)Institut National de la Recherche Scientifique (INRS)École de Technologie Supérieure (ÉTS)King Abdullah University of Science and Technology (KAUST)。
文摘Ammonia serves as a crucial chemical raw material and hydrogen energy carrier.Aqueous electrocatalytic nitrogen reduction reaction(NRR),powered by renewable energy,has attracted tremendous interest during the past few years.Although some achievements have been revealed in aqueous NRR,significant challenges have also been identified.The activity and selectivity are fundamentally limited by nitrogen activation and competitive hydrogen evolution.This review focuses on the hurdles of nitrogen activation and delves into complementary strategies,including materials design and system optimization(reactor,electrolyte,and mediator).Then,it introduces advanced interdisciplinary technologies that have recently emerged for nitrogen activation using high-energy physics such as plasma and triboelectrification.With a better understanding of the corresponding reaction mechanisms in the coming years,these technologies have the potential to be extended in further applications.This review provides further insight into the reaction mechanisms of selectivity and stability of different reaction systems.We then recommend a rigorous and detailed protocol for investigating NRR performance and also highlight several potential research directions in this exciting field,coupling with advanced interdisciplinary applications,in situ/operando characterizations,and theoretical calculations.
基金supported by the National Natural Science Foundation of China (52173286, 52207249)Major basic research project of Natural Science Foundation of Shandong Province (ZR2023ZD12)+1 种基金the State Key Laboratory of Marine Resource Utilization in South China Sea (Hainan University) (MRUKF2023013)Open Program of Guangxi Key Laboratory of Information Materials (221024-K)。
文摘The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.
基金supported by the NSF of China(Nos.21971143,21805165,22209098)the 111 Project(D20015)+1 种基金the major research and development project of Hubei Three Gorges Laboratory(2022-3)the Natural Science Foundation of Hubei Province(2022CFB326)
文摘Exploring a novel strategy for large-scale production of battery-type Ni(OH)_(2)-based composites,with excellent capacitive performance,is still greatly challenging.Herein,we developed a facile and cost-effective strategy to in situ grow a layer of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)composite on the nickel foam(NF)collector,where Ti_(3)C_(2)T_(x)is not only a conductive component,but also a catalyst that accelerates the oxidation of NF to Ni(OH)_(2).Detailed analysis reveals that the crystallinity,morphology,and electronic structure of the integrated electrode can be tuned via the electrochemical activation,which is beneficial for improving electrical conductivity and redox activity.As expected,the integrated electrode shows a specific capacity of 1.09 C cm^(-2)at 1 mA cm^(-2)after three custom activation cycles and maintains 92.4%of the initial capacity after 1500 cycles.Moreover,a hybrid supercapacitor composed of Ni(OH)_(2)/Ti_(3)C_(2)T_(x)/NF cathode and activated carbon anode provides an energy density of 0.1 mWh cm^(-2)at a power density of 0.97 mW cm^(-2),and excellent cycling stability with about 110%capacity retention rate after 5000 cycles.This work would afford an economical and convenient method to steer commercial Ni foam into advanced Ni(OH)_(2)-based composite materials as binder-free electrodes for hybrid supercapacitors.
基金supported by the Chongqing Special Key Project of Technology Innovation and Application Development,China(cstc2019jscx-dxwt B0029)the National Natural Science Foundation of China(51871143)+5 种基金the Science and Technology Committee of Shanghai(19010500400)the Shanghai Rising-Star Program(21QA1403200)Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2019jcyj-msxm X0306)the Start-up Funds of Chongqing University(02110011044171)the Senior Talent Start-up Funds of Jiangsu University(4111310024)the Independent Research Project of State Key Laboratory of Mechanical Transmissions(SKLMT-ZZKT-2021M11)
文摘Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamics and kinetic properties pose major challenges for their engineering applications.Herein,we review the recent progress in improving their thermodynamics and kinetics,with an emphasis on the models and the influence of various parameters in the calculated models.Subsequently,the impact of alloying,composite,and nanocrystallization on both thermodynamics and dynamics are discussed in detail.In particular,the correlation between various modification strategies and the hydrogen capacity,dehydrogenation enthalpy and temperature,hydriding/dehydriding rates are summarized.In addition,the mechanism of hydrogen storage processes of Mg-based materials is discussed from the aspect of classical kinetic theories and microscope hydrogen transferring behavior.This review concludes with an outlook on the remaining challenge issues and prospects.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021A1515110859)the Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province+2 种基金the Natural Sciences and Engineering Research Council of Canada(NSERC)Institut National de la Recherche Scientifique(INRS)。
文摘Exploring highly active and stable transition metal-based bifunctional electrocatalysts has recently attracted extensive research interests for achieving high inherent activity, abundant exposed active sites, rapid mass transfer, and strong structure stability for overall water splitting. Herein, an interface engineering coupled with shell-protection strategy was applied to construct three-dimensional(3D) core-shell NixSy@MnOxHy heterostructure nanorods grown on nickel foam(NixSy@MnOxHy/NF) as a bifunctional electrocatalyst. NixSy@MnOxHy/NF was synthesized via a facile hydrothermal reaction followed by an electrodeposition process. The X-ray absorption fine structure spectra reveal that abundant Mn-S bonds connect the heterostructure interfaces of N ixSy@MnOxHy, leading to a strong electronic interaction, which improves the intrinsic activities of hydrogen evolution reaction and oxygen evolution reaction(OER). Besides, as an efficient protective shell, the MnOxHy dramatically inhibits the electrochemical corrosion of the electrocatalyst at high current densities, which remarkably enhances the stability at high potentials. Furthermore, the 3D nanorod structure not only exposes enriched active sites, but also accelerates the electrolyte diffusion and bubble desorption. Therefore, NixSy@MnOxHy/NF exhibits exceptional bifunctional activity and stability for overall water splitting, with low overpotentials of 326 and 356 mV for OER at 100 and 500 mA cm^(–2), respectively, along with high stability of 150 h at 100 mA cm^(–2). Furthermore, for overall water splitting, it presents a low cell voltage of 1.529 V at 10 mA cm^(–2), accompanied by excellent stability at 100 mA cm^(–2) for 100 h. This work sheds a light on exploring highly active and stable bifunctional electrocatalysts by the interface engineering coupled with shell-protection strategy.
基金financially supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)Institut National de la Recherche Scientifique(INRS)the National Natural Science Foundation of China(516722040)
文摘Hydrogen,a renewable and outstanding energy carrier with zero carbon dioxide emission,is regarded as the best alternative to fossil fuels.The most preferred route to large-scale production of hydrogen is by water electrolysis from the intermittent sources(e.g.,wind,solar,hydro,and tidal energy).However,the efficiency of water electrolysis is very much dependent on the activity of electrocatalysts.Thus,designing high-effective,stable,and cheap materials for hydrogen evolution reaction(HER)could have a substantial impact on renewable energy technologies.Recently,single-atom catalysts(SACs)have emerged as a new frontier in catalysis science,because SACs have maximum atom-utilization efficiency and excellent catalytic reaction activity.Various synthesis methods and analytical techniques have been adopted to prepare and characterize these SACs.In this review,we discuss recent progress on SACs synthesis,characterization methods,and their catalytic applications.Particularly,we highlight their unique electrochemical characteristics toward HER.Finally,the current key challenges in SACs for HER are pointed out and some potential directions are proposed as well.
基金This work is supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)Centre Québéco is sur les Materiaux Fonctionnels(CQMF),Fonds de Recherche du Québec-Nature et Technologies(FRQNT)+2 种基金Institut National de la Recherche Scientifique(INRS)This work is also supported by the National Natural Science Foundation of China(21972017)the“Scientific and Technical Innovation Action Plan”Hong Kong,Macao and Taiwan Science&Technology Cooperation Project of Shanghai Science and Technology Committee(19160760600).F.Dong gratefully acknowledges scholarships from the China Scholarship Council(CSC).
文摘Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.
基金the National Natural Science Foundation of China(Grant No.21673051)the Department of Science and Technology of Guangdong Province,China(No.2019A050510043).
文摘Compared with commercial lithium batteries with liquid electrolytes,all-solidstate lithium batteries(ASSLBs)possess the advantages of higher safety,better electrochemical stability,higher energy density,and longer cycle life;therefore,ASSLBs have been identified as promising candidates for next-generation safe and stable high-energy-storage devices.The design and fabrication of solid-state electrolytes(SSEs)are vital for the future commercialization of ASSLBs.Among various SSEs,solid polymer composite electrolytes(SPCEs)consisting of inorganic nanofillers and polymer matrix have shown great application prospects in the practice of ASSLBs.The incorporation of inorganic nanofillers into the polymer matrix has been considered as a crucial method to achieve high ionic conductivity for SPCE.In this review,the mechanisms of Li+transport variation caused by incorporating inorganic nanofillers into the polymer matrix are discussed in detail.On the basis of the recent progress,the respective contributions of polymer chains,passive ceramic nanofillers,and active ceramic nanofillers in affecting the Li+transport process of SPCE are reviewed systematically.The inherent relationship between the morphological characteristics of inorganic nanofillers and the ionic conductivity of the resultant SPCE is discussed.Finally,the challenges and future perspectives for developing high-performance SPCE are put forward.This review aims to provide possible strategies for the further improvement of ionic conductivity in inorganic nanoscale filler-reinforced SPCE and highlight their inspiration for future research directions.
基金This work is supported financially by the Natural Sciences and Engineering Research Council of Canada(NSERC),the Fonds de Recherche du Québec-Nature et Technologies(FRQNT)Centre Québécois sur les Materiaux Fonctionnels(CQMF),the Canada Foundation for Innovation(CFI)+1 种基金Institut National de la Recherche Scientifique(INRS).The XAS characterizations were performed at the Canadian Light Source(CLS),which is financially supported by NSERC,CFIthe University of Saskatchewan,the Government of Saskatchewan,Western Economic Diversification Canada,the National Research Council of Canada,and the Canadian Institutes of Health Research。
文摘The electroreduction reaction of CO_(2)(ECO_(2)RR)requires high-performance catalysts to convert CO_(2)into useful chemicals.Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO_(2)RR.This work presents a series of atomically dispersed Co,Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework(C-Fe-Co-ZIF)for the syngas generation from ECO_(2)RR.The synergistic effect of the bimetallic catalyst promotes CO production.Compared to the pure C-Co-ZiF,C-Fe-Co-ZIF facilitates CO production with a CO Faradaic efficiency(FE)boost of 10%,with optimal FE_(CO)of 51.9%,FE_(H_(2))of 42.4%at-0.55 V,and CO current density of 8.0 mA cm^(-2)at-0.7 V versus reversible hydrogen electrode(RHE).The H_(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of-0.35 to-0.8 V versus RHE.The total FE_(CO+H_(2))maintains as high as 93%over 10 h.The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe,which is essential for the enhancement of the CO production in ECO_(2)RR.The positive impacts of Cu-Co and Ni-Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO_(2)RR.
基金This study was supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)the National Natural Science Foundation of China(21972017)+2 种基金Canada Foundation for Innovation(CFI)Centre Québécois sur les Materiaux Fonctionnels,Fondsde Recherche du Québec‐Nature et TechnologiesInstitut National de la Recherche Scientifique.Mingjie Wu gratefully acknowledges the scholarships from the China Scholarship Council.
文摘Oxygen reduction/evolution reactions(ORR/OERs)catalysts play a key role in the metal‐air battery and water‐splitting process.Herein,we developed a facile template‐free method to fabricate a new type of non–noble metal‐based hybrid catalyst which consists of binary FeNi alloy/nitride nanocrystals with graphitic‐shell and biomass‐derived N‐doped carbon(NC)(FexNiyN@C/NC).This novel nanostructure exhibits superior performance for ORR/OER,which can be attributed to the strong interactions between the graphitic‐shell encapsulated FeNi alloy/nitride nanocrystals and the N‐doped porous carbon substrate.The X‐ray absorption spectroscopy technique was employed to reveal the underlying mechanisms for the excellent performance.The assembled Zn‐air battery device exhibits outstanding charging/discharging performance and cycling stability,indicating the great potential of this type of novel catalysts.
基金Acknowledgments We thank Drs Hua Gu （Columbia University, USA）, Weiguo Zhang （Duke University Medical Center, USA）, and Youhai H Chen （University of Pennsylvania, USA） for reviewing the manuscript and for suggestions, and Dr Ilia Voskoboinik （Peter MacCallum Cancer Centre, Australia） for providing the mouse perforin cDNA in pKS（＋） Bluescript. Ragl^-/- mice were gifts from Xiaolong Liu （Shanghai Institutes for Biological Sciences, China）. This work was supported by grants from the National Natural Science Foundation of China （30325018, 30530700, 30623003, and 30421005） and CAS project （KSCX1-YW-R-43）, grants from the National Key Project 973 （2006CB504300 and 2007CB512404）, grants from the Technology Commission of Shanghai Municipality （04DZ14902, 04DZ19108, 06DZ22032, 04DZ19112, 07XD14033, and 07DZ22916）, 863 key project （2006AA02A247）, and a grant from the E-institutes of Shanghai Universities Immunology Division.
文摘Perforin is a pore-forming protein engaged mainly in mediating target T cell death and is employed by cytotoxic T lymphocytes （CTLs） and natural killer cells. However, whether it also plays a role in conventional CD4^＋ T cell function remains unclear. Here we report that in perforin-deficient （PKO） mice, CD4^＋ T cells are hyperproliferative in response to T cell receptor （TCR） stimulation. This feature of hyperproliferation is accompanied by the enhancement both in cell division and in IL-2 secretion. It seems that the perforin deficiency does not influence T cell development in thymus spleen and lymph node. In vivo, perforin deficiency results in increased antigen-specific T cell proliferation and antibody production. Furthermore, PKO mice are more susceptible to experimental autoimmune uveitis. To address the molecular mechanism, we found that after TCR stimulation, CD4^＋ T cells from PKO mice display an increased intracellular calcium flux and subsequently enhance activation of transcription factor NFAT1. Our results indicate that perforin plays a negative role in regulating CD4^＋ T cell activation and immune response by affecting TCR-dependent Ca^2＋ signaling.
基金This study is financially supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)the Fonds de Recherche du Québec—Nature et Technologies(FRQNT),Centre Québécois sur les Materiaux Fonctionnels(CQMF)+3 种基金Institut National de la Recherche Scientifique(INRS)National Natural Science Foundation of China(Grant No.21805064)SS acknowledges the ECS-Toyota Young Investigator Fellowship.LD acknowledges the scholarship under the International Postdoctoral Exchange Fellowship Program by the Office of China Postdoctoral Council(Grant No.20180072)FRQNT for the Postdoctoral scholarship(V2,file number:274384)in Quebec Canada.
文摘Oxygen reduction reaction(ORR)is an important electrochemical process for renewable energy conversion and storage applications such as fuel cells and metal-air batteries.ORR is sluggish in kinetics and requires a large amount of platinum group metal(PGM)-based catalysts to facilitate its slow reaction rate.Application of precious metals raises the cost and decreases the competitivity of these devices in the market.To address this challenge,PGM-free ORR catalysts have been intensively investigated as an alternative to replace the PGM-based catalysts and to promote the deployment of ORR-related applications.In particular,the biomass holds promising potential to be used as the precursor material for PGM-free ORR catalysts.This pathway has gained more and more attention in recent years.In this review,recent advances regarding biomass-derived ORR catalysts are summarized with a focus on the rational design of both active sites and porous structures which are the two key factors in determining ORR performance of catalysts.At the end,the perspectives of development of biomass-derived catalysts is discussed.
基金funded by the National Natural Science Foundation of China (22208331, 52003300)the Natural Sciences and Engineering Research Council of Canada (NSERC)+4 种基金the Fonds de Recherche du Québec-Nature et Technologies (FRQNT)Centre Québécois sur les Materiaux Fonctionnels (CQMF), McGill Universityécole de Technologie Supérieure (éTS)Institut National de la Recherche Scientifique (INRS)the support from the Marcelle-Gauvreau Engineering Research Chair program
文摘Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement.Unlike the previously reported singleatom or dual-atom configurations,we designed a new type of binary-atom catalyst,through engineering Fe-N_(4)electronic structure with adjacent Co-N_(2)C_(2)and nitrogen-coordinated Co nanoclusters,as oxygen electrocatalysts.The resultant optimized electronic structure of the Fe-N_(4)active center favors the binding capability of intermediates and enhances oxygen reduction reaction(ORR)activity in both alkaline and acid conditions.In addition,anchoring M-N-C atomic sites on highly graphitized carbon supports guarantees of efficient charge-and mass-transports,and escorts the high bifunctional catalytic activity of the entire catalyst.Further,through the combination of electrochemical studies and in-situ X-ray absorption spectroscopy analyses,the ORR degradation mechanisms under highly oxidative conditions during oxygen evolution reaction processes were revealed.This work developed a new binary-atom catalyst and systematically investigates the effect of highly oxidative environments on ORR electrochemical behavior.It demonstrates the strategy for facilitating oxygen electrocatalytic activity and stability of the atomically dispersed M-N-C catalysts.
基金Acknowledgments We thank ProfYongjun Liu, Dangsheng Li and Yangxin Fu for helpful comments and Dr Sheri Skinner for reviewing the manuscript and for constructive suggestions. This work was supported by grants from the National Natural Science Foundation of China （30530700, 30623003, 30600568, 30721065, 90713044, 30600308, 30801011, 30870126） and CAS project （KSCX1-YW-R-43）, grant from SIBS project （2007KIP301）, grants from the Ministry of Science and Technology （2006CB504300, 2007CB512404, 2006AA02A247, 20072714）, the Technology Commission of Shanghai Municipality （88014199, 07DZ22916, 07XD14033, 064319034, 08431903004, 2008ZX10206, 08DZ2291703）, EU project （FP6-2005-SSP-5-B, SP5B-CT-2006-044161） and from the E-institutes of Shanghai Universities Immunology Division.
文摘It is important to understand the pathogenesis of asthma induced by natural allergens, which could exclude the interference of artificial adjuvant and provide insights of natural immune response in the disease. In the present study, we show that Trichosanthin （TCS） could induce airway inflammation even without the help of alum. Furthermore, TCS appeared capable of replacing alum to promote OVA-specific airway inflammation. TCS induced accumulation of IL-4-producing eosinophils in peritoneum at an early stage and the adjuvant function of TCS was eliminated by blockage of IL-4 at this stage. Finally, the eosinophils triggered by TCS from WT mice, but not from IL-4- deficient mice were shown to function as adjuvant for the induction of OVA-specific Th2 responses. Our data indicate that TCS is not only an allergen, but also a Th2-typc adjuvant modulating the switching of immune responses to a Th2 pathway. This chain of events results from IL-4 production by eosinophils at an early stage of TCS-priming. In conclusion, TCS may be useful as a Th2 adjuvant, and innate immune cells, such as eosinophils, may be a good target to study the initiation of Th2 response.
基金supported by the Natural Science Foundation of China(91963202 and 52072372)the Key Research Program of Frontier Sciences(CAS,Grant,QYZDJ-SSW-SLH046)the CAS/SAFEA International Partnership Program for Creative Research Teams,and the Hefei Institutes of Physical Science,Chinese Academy of Sciences Director’s Fund(YZJ ZX202018)
文摘Transition metal oxides are regarded as promising candidates of anode for next-generation lithium-ion batteries(LIBs)due to their ultrahigh theoretical capacity and low cost,but are restricted by their low conductivity and large volume expansion during Li^(+)intercalation.Herein,we designed and constructed a structurally integrated 3D carbon tube(3D-CT)grid film with Mn_(3)O_(4)nanoparticles(Mn_(3)O_(4)-NPs)and carbon nanotubes(CNTs)filled in the inner cavity of CTs(denoted as Mn_(3)O_(4)-NPs/CNTs@3D-CT)as high-performance free-standing anode for LIBs.The Mn_(3)O_(4)-NPs/CNTs@3D-CT grid with Mn_(3)O_(4)-NPs filled in the inner cavity of 3D-CT not only afford sufficient space to overcome the damage caused by the volume expansion of Mn_(3)O_(4)-NPs during charge and discharge processes,but also achieves highly efficient channels for the fast transport of both electrons and Li+during cycling,thus offering outstanding electrochemical performance(865 mAh g^(-1)at 1 A g^(-1)after 300 cycles)and excellent rate capability(418 mAh g^(-1)at 4 A g^(-1))based on the total mass of electrode.The unique 3D-CT framework structure would open up a new route to the highly stable,high-capacity,and excellent cycle and high-rate performance free-standing electrodes for highperformance Li-ion storage.
基金the support from Guangdong Basic and Applied Basic Research Foundation (2020B1515120039)Guangdong Technology Center for Oxide Semiconductor Devices+2 种基金the support from National Key R&D Program of China (2022YFF1500400)the National Natural Science Foundation of China (51835005)the support from the Natural Sciences and Engineering Research Council of Canada (NSERC)
文摘Atomic scale engineering of materials and interfaces has become increasingly important in material manufacturing.Atomic layer deposition(ALD)is a technology that can offer many unique properties to achieve atomic-scale material manufacturing controllability.Herein,we discuss this ALD technology for its applications,attributes,technology status and challenges.We envision that the ALD technology will continue making significant contributions to various industries and technologies in the coming years.
基金the "Mobility project Italy-Canada (Québec) n° QU13MO7"the financial support of the EU through the DURAMET Project 278054+1 种基金funding from the European Community’s Seventh Framework Programme (FP7/2011–2014) for the Fuel Cells and Hydrogen Joint Technology Initiative under grant agreement DURAMET no. 278054""Fonds de Recherche du Québec-Nature et Technologies (FQRNT)" for financial support
文摘Cathode catalysts for direct alcohol fuel cells(DAFCs) must have high catalytic activity for the oxy-gen reduction reaction(ORR), low cost, and high tolerance to the presence of methanol or ethanol. Pt is the benchmark catalyst for this application owing to its excellent electrocatalytic activity, but its high cost and low tolerance to the organic fuel permeating through the membrane have hindered the commercialization of DAFCs. Herein we present a facile synthesis route to obtain organic fuel-tolerant Zr- and Ta-based catalysts supported on carbon. This method consists of a simple precipitation of metal precursors followed by a heat treatment. X-ray diffraction analyses confirmed that the obtained samples were crystalline ZrO 2-x and Na2Ta8O21-x having crystallite sizes of 26 and 32 nm, respectively. The thermal treatment effectively increased the activity of the catalysts to-wards the ORR, although further optimization is necessary. Both catalysts exhibited a high tolerance to the presence of methanol with only a moderate reduction in ORR activity even at high methanol concentration(0.5 mol/L).
基金financial support from the Natural Sciences and Engineering Research Council of Canada(NSERC)Institut National de la Recherche Scientifique(INRS)
文摘When I read the paper“Electrolytes enriched by potassium perfluorinated sulfonates for lithium metal batteries”from Prof.Jianmin Ma’s group,which was published in Science Bulletin(doi.org/10.1016/j.scib.2020.09.018),I felt excited as presented a multi-factor principle for applying potassium perfluorinated sulfonates to suppress the dendrite growth and protect the cathode from the viewpoint of electrolyte additives.The effects of these additives are revealed through experimental results,molecular dynamics simulations and first-principle calculations.Specifically,it involves the influence of additives on Li^(+)solvation structure,solid electrolyte interphase(SEI),Li growth and nucleation.Following the guidance of the multi-factor principle,every part of the additive molecule should be utilized to regulate electrolytes.This multifactor principle for electrolyte additive molecule design(EAMD)offers a unique insight on understanding the electrochemical behavior of iontype electrolyte additives on both the Li metal anode and high-voltage cathode.In these regards,I would be delighted to write a highlight for this innovative work and,hopefully,it may raise more interest in the areas of electrolyte additives.
基金supported by the National Key Research and Development Program of China(2017YFB0102900 and 2016YFB0101201)the National Natural Science Foundation of China(51971094,21476088 and 21776104)the Guangdong Provincial Department of Science and Technology(2015A030312007)。
文摘Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.
基金supported by the National Key Research and Development Program of China (Grant Nos.2022YFA1103700,2020YFA0804000,2020YFA0112200,2021YFF1201000,2022YFA1103800,2021YFA1101401,the STI2030-Major Projects-2021ZD0202400)the National Natural Science Foundation of China (Grant Nos.92049116,81921006,82125011,92149301,92168201,91949209,92049304,32121001,82192863,82122024,82071588,32000500,82271600)+9 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA16000000)CAS Project for Young Scientists in Basic Research (YSBR-076,YSBR-012)the Program of the Beijing Natural Science Foundation (Z190019)the Pilot Project for Public Welfare Development and Reform of Beijing-affiliated Medical Research Institutes (No.11000022T000000461062)Youth Innovation Promotion Association of CAS (E1CAZW0401,2023092,2022083)Young Elite Scientists Sponsorship Program by CAST (YESS20200012,YESS20210002)the Informatization Plan of Chinese Academy of Sciences (CAS-WX2021SF-0301,CAS-WX2022SDC-XK14,CAS-WX2021SF-0101)New Cormerstone Science Foundation through the XPLORER PRIZE (2021-1045)Excellent Young Talents Program of Capital Medical University (No.12300927)Excellent Young Talents Training Program for the Construction of Beijing Municipal University Teacher Team (BPHR202203105).
文摘Aging increases the risk ofliver diseases and systemic susceptibility to aging-related diseases.However,cell type-specific changes and the underlying mechanism of liver aging in higher vertebrates remain incompletely characterized.Here,we constructed the first single-nucleus transcriptomic landscape of primate liver aging,in which we resolved cell type-specific gene expression fluctuation in hepatocytes across three liver zonations and detected aberrant cell-cell interactions between hepatocytes and niche cells.Upon in-depth dissection of this rich dataset,we identifed impaired lipid metabolism and upregulation of chronic inflammation-related genes prominently associated with declined liver functions during aging.In particular,hyperactivated sterol regulatory element-binding protein(SREBP)signaling was a hallmark of the aged liver,and consequently,forced activation of SREBP2 in human primary hepatocytes recapitulated in vivo aging phenotypes,manifesting as impaired detoxification and accelerated cellular senescence.This study expands our knowledge of primate liver aging and informs the development of diagnostics and therapeutic interventions for liver aging and associated diseases.
