All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for t...All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for the next-generation energy storage systems.However,interfacial issues between SSEs and Nirich oxide cathode materials,attributed to space charge layer,interfacial side reactions,and mechanical contact failure,significantly restrict the performances of ASSBs.The interface degradation is closely related to the components of the composite cathode and the process of electrode fabrication.Focusing on the influencing factors of interface compatibility between SSEs and Ni-rich oxide cathode,this article systematically discusses how cathode active materials(CAMs),electrolytes,conductive additives,binders,and electrode fabrication impact the interface compatibility.In addition,the strategies for the compatibility modification are reviewed.Furthermore,the challenges and prospects of intensive research on the degradation and modification of the SSE/Ni-rich cathode material interface are discussed.This review is intended to inspire the development of high-energy-density and high-safety all-solid-state batteries.展开更多
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an...The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.展开更多
Sulfide all-solid-state lithium batteries(SASSLBs)with a single-crystal nickel-rich layered oxide cathode(LiNix-CoyMn_(1-x-y)O_(2),x≥0.8)are highly desirable for advanced power batteries owing to their excellent ener...Sulfide all-solid-state lithium batteries(SASSLBs)with a single-crystal nickel-rich layered oxide cathode(LiNix-CoyMn_(1-x-y)O_(2),x≥0.8)are highly desirable for advanced power batteries owing to their excellent energy density and safety.Nevertheless,the cathode material's cracking issue and its severe interfacial problem with sulfide solid electrolytes have hindered the further development.This study proposes to employ surface modification engineering to produce B-NCM cathode materials coated with boride nanostructure stabilizer in situ by utilizing NCM encapsulated with residual lithium.This approach enhances the electrochemical performance of SASSLBs by effectively inhibiting electrochemical-mechanical degradation of the NCM cathode material on cycling and reducing deleterious side reactions with the solid sulfide electrolyte.The B-NCM/LPSCl/Gr SASSLBs demonstrate impressive cycling stability,retaining 84.19%of its capacity after 500 cycles at 0.2 C,which represents a 30.13%increase vs.NCM/LPSCl/Gr.It also exhibits a specific capacity of 170.4 mAh/g during its first discharge at 0.1 C.This work demonstrates an effective surface engineering strategy for enhancing capacity and cycle life,providing valuable insights into solving interfacial problems in SASSLBs.展开更多
Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
With an increase in global aging,the number of people affected by cerebrovascular diseases is also increasing,and the incidence of vascular dementia-closely related to cerebrovascular risk-is increasing at an epidemic...With an increase in global aging,the number of people affected by cerebrovascular diseases is also increasing,and the incidence of vascular dementia-closely related to cerebrovascular risk-is increasing at an epidemic rate.However,few therapeutic options exist that can markedly improve the cognitive impairment and prognosis of vascular dementia patients.Similarly in Alzheimer’s disease and other neurological disorders,synaptic dysfunction is recognized as the main reason for cognitive decline.Nitric oxide is one of the ubiquitous gaseous cellular messengers involved in multiple physiological and pathological processes of the central nervous system.Recently,nitric oxide has been implicated in regulating synaptic plasticity and plays an important role in the pathogenesis of vascular dementia.This review introduces in detail the emerging role of nitric oxide in physiological and pathological states of vascular dementia and summarizes the diverse effects of nitric oxide on different aspects of synaptic dysfunction,neuroinflammation,oxidative stress,and blood-brain barrier dysfunction that underlie the progress of vascular dementia.Additionally,we propose that targeting the nitric oxide-sGC-cGMP pathway using certain specific approaches may provide a novel therapeutic strategy for vascular dementia.展开更多
Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expre...Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expressed.NO can serve different purposes:As a vasoactive molecule,as a neurotransmitter or as an immunomodulator.It plays a key role in cerebral ischemia/reperfusion injury(CIRI).Hypoxic episodes simulate the production of oxygen free radicals,leading to mitochondrial and phospholipid damage.Upon reperfusion,increased levels of oxygen trigger oxide synthases;whose products are associated with neuronal damage by promoting lipid peroxidation,nitrosylation and excitotoxicity.Molecular pathways in CIRI can be altered by NOS.Neuroprotective effects are observed with eNOS activity.While nNOS interplay is prone to endothelial inflammation,oxidative stress and apoptosis.Therefore,nNOS appears to be detrimental.The interaction between NO and other free radicals develops peroxynitrite;which is a cytotoxic agent.It plays a main role in the likelihood of hemorrhagic events by tissue plasminogen activator(t-PA).Peroxynitrite scavengers are currently being studied as potential targets to prevent hemorrhagic transformation in CIRI.展开更多
Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In t...Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In this study,a flake-like nickel cobaltate/re-duced graphene oxide/melamine-derived carbon foam(FNC/RGO/MDCF)was successfully fabricated through a combination of solvo-thermal treatment and high-temperature pyrolysis.Results indicated that RGO was evenly distributed in the MDCF skeleton,providing ef-fective support for the load growth of FNC on its surface.Sample S3,the FNC/RGO/MDCF composite prepared by solvothermal method for 16 h,exhibited a minimum reflection loss(RL_(min))of-66.44 dB at a thickness of 2.29 mm.When the thickness was reduced to 1.50 mm,the optimal effective absorption bandwidth was 3.84 GHz.Analysis of the absorption mechanism of FNC/RGO/MDCF revealed that its excellent absorption performance was primarily attributed to the combined effects of conduction loss,multiple reflection,scattering,in-terface polarization,and dipole polarization.展开更多
Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether ...Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.展开更多
Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,gr...Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,graphene oxide modified asphalt was prepared and characteristics was studied including the high deformation resistance performance and the self-healing property of modified asphalt.Functional groups and morphology of graphene oxide modified asphalt were described by Fourier transform infrared spectroscopy.The high deformation resistance performance and self-healing effect of asphalt samples were obtained through dynamic slear rheometer(DSR)test.Results shows that graphene oxide dispersions improve the performance of asphalt relatively well compared to graphene oxide powder.There is no chemical reaction between graphene oxide and asphalt,but physical connection.The addition of graphene oxide improved the high deformation resistance of modified asphalt and expedited the self-healing ability of asphalt under fatigue load.展开更多
Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SO...Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SOECs with Zr-rich electrolyte,called Zr-rich side P-SOECs,possess high thermodynamically stability under high steam concentrations but the large reaction resistances and the current leakage,thus the inferior performances.In this study,an efficient functional interlayer Ba_(0.95)La_(0.05)Fe_(0.8)Zn_(0.2)O_(3-δ)(BLFZ)in-between the anode and the electrolyte is developed.The electrochemical performances of P-SOECs are greatly enhanced because the BLFZ can greatly increase the interface contact,boost anode reaction kinetics,and increase proton injection into electrolyte.As a result,the P-SOEC yields high current density of 0.83 A cm^(-2) at 600℃ in 1.3 Vamong all the reported Zr-rich side cells.This work not only offers an efficient functional interlayer for P-SOECs but also holds the potential to achieve P-SOECs with high performances and long-term stability.展开更多
Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-p...Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.展开更多
Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poi...Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.展开更多
Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intend...Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intends to study the photocatalytic production of hydrogen from D-(+)-Glucose by using different groups of catalysts that have been prepared (M2+ = Zn, Mg and Ni) M2+/Ti4+ Al3+-LDHs (layered double hydroxides). It is then loaded Pd on the catalyst, and the effect of the composite catalyst, layered double hydroxides, is measured. After calcining, the catalyst for the conversion of Layered Double Hydroxides (LDHs) to Layered Double Oxides (LDOs) is used to produce hydrogen gas from glucose. Photocatalytic reforming of glucose-derived compounds is an efficient method for the production of hydrogen. The purpose is to study the effect of metal ions on layered double oxide (LDO) materials by loading Pd and investigate hydrogen production from glucose. The metal cations in the layer were distributed through the preparation of the catalyst process by ion and atom scale between the layers, which were dispersed systematically, as well as the controlled component catalysis. This process shows that ZnTiAl-LDO had the best effect as a catalyst in producing hydrogen compared to NiTiAl-LDO and MgTiAl-LDO.展开更多
Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage p...Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.展开更多
Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))aroun...Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))around the oxygen vacancies.The origin of the enhanced catalytic activity of ZrO_(2)with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study.Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface,which directly attacked the C-H bond in propane.The involvement of localized electrons activates the C-H bond via back-donation to the antibonding orbital on the defective surface;conversely,charge is transferred from propane to the pristine surfaces.The barrier for the first C-H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces,which verifies the superior activity of Zr_(cus).Notably,however,the desorption of both propene and hydrogen molecules from Zr_(cus)is more difficult due to strong binding.The calculated turnover frequency(TOF)for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures,whereas the defective surfaces have a larger TOF at high temperatures.However,the rate-determining step and reaction order on the defective surface differ from those on the pristine surface,which corroborates that the catalysts follow different mechanisms.A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide.展开更多
Conventional Fe-C alloy parts used in mechanical transmission and braking systems exposed to the external environment often suffer from wear and corrosion failures.Surface coating strengthening technologies have been ...Conventional Fe-C alloy parts used in mechanical transmission and braking systems exposed to the external environment often suffer from wear and corrosion failures.Surface coating strengthening technologies have been explored to improve the surface performance and prolong service life of these parts.Among these technologies,laser cladding has shown promise in producing Fe-based alloy coatings with superior interfacial bonding properties to the Fe-C alloy substrate.Additionally,the microstructure of the Fe-based alloy coating is more uniform and the grain size is finer than that of surfacing welding,thermal spraying,and plasma cladding,and the oxide film of alloying elements on the coating surface can improve the coating performance.However,Fe-based alloy coatings produced by laser cladding typically exhibit lower hardness,lower wear resistance,corrosion resistance,and oxidation resistance compared to coatings based on Co and Ni alloys.Moreover,these coatings are susceptible to defects such as pores and cracks.To address these limitations,the incorporation of rare-earth oxides through doping in the laser cladding process has garnered significant attention.This approach has demonstrated substantial improvements in the microstructure and properties of Fe-based alloy coatings.This paper reviewed recent research on the structure and properties of laser-cladded Fe-based alloy coatings doped with various rare earth oxides,including La_(2)O_(3),CeO_(2),and Y_(2)O_(3).Specifically,it discussed the effects of rare earth oxides and their concentrations on the structure,hardness,friction,wear,corrosion,and oxidation characteristics of these coatings.Furthermore,the mechanisms by which rare earth oxides influence the coating’s structure and properties were summarized.This review aimed to serve as a valuable reference for the application and advancement of laser cladding technology for rare earth modified Fe-based alloy coatings.展开更多
Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impa...Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.展开更多
Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived f...Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.展开更多
The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly unders...The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates.In this study,we prepared two Zn-Al spinel oxide catalysts via coprecipitation(ZnAl-C)and hydrothermal(ZnAl-H)methods,and conducted a comparative investigation in the CO_(2)hydrogenation reaction.Surprisingly,under similar conditions,ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H.Comprehensive characterizations using X-ray diffraction(XRD),Raman spectroscopy and electron paramagnetic resonance(EPR)unveiled that ZnAl-C catalyst had abundant ZnO species on its surface,and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies,which are crucial for CO_(2)adsorption and activation.Additionally,state-of-the-art solid-state nuclear magnetic resonance(NMR)techniques,including ex-situ and in-situ NMR analyses,confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species,which was readily hydrogenated to methanol and DME.These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO_(2)-to-methanol hydrogenation reaction,which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst.These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.展开更多
Amorphous RuO_(x)(a-RuO_(x)) with disordered atomic arrangement and abundant coordinatively unsaturated Ru sites possesses high intrinsic electrocatalytic activity for oxygen evolution reaction (OER).However,the a-RuO...Amorphous RuO_(x)(a-RuO_(x)) with disordered atomic arrangement and abundant coordinatively unsaturated Ru sites possesses high intrinsic electrocatalytic activity for oxygen evolution reaction (OER).However,the a-RuO_(x)is prone to fast corrosion during OER in strong acid.Here we realized the stabilization of an ultrathin a-RuO_(x)layer via constructing heterointerface with crystalline a-MnO_(2)nanorods array (MnO_(2)@aRuO_(x)).Benefiting from the strong electronic interfacial interaction,the as-formed MnO_(2)@a-RuO_(x)electrocatalyst display an ultralow overpotential of 128 mV to reach 10 mA cm^(-2)and stable operation for over 100 h in 0.1 mol L^(-1)HClO_(4).The assembled proton exchange membrane(PEM) water electrolyzer reach 1 A cm^(-2)at applied cell voltage of 1.71 V.Extensive characterizations indicate the MnO_(2)substrate work as an electron donor pool to prevent the overoxidation of Ru sites and the OER proceeds in adsorbent evolution mechanism process without involving lattice oxygen.Our work provides a promising route to construct robust amorphous phase electrocatalysts.展开更多
基金financially supported by the National Natural Science Foundation of China(52072036,52272187)the China Petroleum&Chemical Corporation(SINOPEC)project(223128).
文摘All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for the next-generation energy storage systems.However,interfacial issues between SSEs and Nirich oxide cathode materials,attributed to space charge layer,interfacial side reactions,and mechanical contact failure,significantly restrict the performances of ASSBs.The interface degradation is closely related to the components of the composite cathode and the process of electrode fabrication.Focusing on the influencing factors of interface compatibility between SSEs and Ni-rich oxide cathode,this article systematically discusses how cathode active materials(CAMs),electrolytes,conductive additives,binders,and electrode fabrication impact the interface compatibility.In addition,the strategies for the compatibility modification are reviewed.Furthermore,the challenges and prospects of intensive research on the degradation and modification of the SSE/Ni-rich cathode material interface are discussed.This review is intended to inspire the development of high-energy-density and high-safety all-solid-state batteries.
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
基金support from the National Natural Science Foundation of China(Grant No.52374407)is gratefully acknowledged.
文摘Sulfide all-solid-state lithium batteries(SASSLBs)with a single-crystal nickel-rich layered oxide cathode(LiNix-CoyMn_(1-x-y)O_(2),x≥0.8)are highly desirable for advanced power batteries owing to their excellent energy density and safety.Nevertheless,the cathode material's cracking issue and its severe interfacial problem with sulfide solid electrolytes have hindered the further development.This study proposes to employ surface modification engineering to produce B-NCM cathode materials coated with boride nanostructure stabilizer in situ by utilizing NCM encapsulated with residual lithium.This approach enhances the electrochemical performance of SASSLBs by effectively inhibiting electrochemical-mechanical degradation of the NCM cathode material on cycling and reducing deleterious side reactions with the solid sulfide electrolyte.The B-NCM/LPSCl/Gr SASSLBs demonstrate impressive cycling stability,retaining 84.19%of its capacity after 500 cycles at 0.2 C,which represents a 30.13%increase vs.NCM/LPSCl/Gr.It also exhibits a specific capacity of 170.4 mAh/g during its first discharge at 0.1 C.This work demonstrates an effective surface engineering strategy for enhancing capacity and cycle life,providing valuable insights into solving interfacial problems in SASSLBs.
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
基金supported by the National Key R&D Program of China,No.2019YFE0121200(to LQZ)the National Natural Science Foundation of China,Nos.82325017(to LQZ),82030032(to LQZ),82261138555(to DL)+2 种基金the Natural Science Foundation of Hubei Province,No.2022CFA004(to LQZ)the Natural Science Foundation of Jiangxi Province,No.20224BAB206040(to XZ)Research Project of Cognitive Science and Transdisciplinary Studies Center of Jiangxi Province,No.RZYB202201(to XZ).
文摘With an increase in global aging,the number of people affected by cerebrovascular diseases is also increasing,and the incidence of vascular dementia-closely related to cerebrovascular risk-is increasing at an epidemic rate.However,few therapeutic options exist that can markedly improve the cognitive impairment and prognosis of vascular dementia patients.Similarly in Alzheimer’s disease and other neurological disorders,synaptic dysfunction is recognized as the main reason for cognitive decline.Nitric oxide is one of the ubiquitous gaseous cellular messengers involved in multiple physiological and pathological processes of the central nervous system.Recently,nitric oxide has been implicated in regulating synaptic plasticity and plays an important role in the pathogenesis of vascular dementia.This review introduces in detail the emerging role of nitric oxide in physiological and pathological states of vascular dementia and summarizes the diverse effects of nitric oxide on different aspects of synaptic dysfunction,neuroinflammation,oxidative stress,and blood-brain barrier dysfunction that underlie the progress of vascular dementia.Additionally,we propose that targeting the nitric oxide-sGC-cGMP pathway using certain specific approaches may provide a novel therapeutic strategy for vascular dementia.
文摘Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expressed.NO can serve different purposes:As a vasoactive molecule,as a neurotransmitter or as an immunomodulator.It plays a key role in cerebral ischemia/reperfusion injury(CIRI).Hypoxic episodes simulate the production of oxygen free radicals,leading to mitochondrial and phospholipid damage.Upon reperfusion,increased levels of oxygen trigger oxide synthases;whose products are associated with neuronal damage by promoting lipid peroxidation,nitrosylation and excitotoxicity.Molecular pathways in CIRI can be altered by NOS.Neuroprotective effects are observed with eNOS activity.While nNOS interplay is prone to endothelial inflammation,oxidative stress and apoptosis.Therefore,nNOS appears to be detrimental.The interaction between NO and other free radicals develops peroxynitrite;which is a cytotoxic agent.It plays a main role in the likelihood of hemorrhagic events by tissue plasminogen activator(t-PA).Peroxynitrite scavengers are currently being studied as potential targets to prevent hemorrhagic transformation in CIRI.
基金support of the Key Science Research Project in Colleges and Universities of Anhui Province,China(No.2022AH050813)the Medical Special Cultivation Project of Anhui University of Science and Technology,China(No.YZ2023H2A002).
文摘Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In this study,a flake-like nickel cobaltate/re-duced graphene oxide/melamine-derived carbon foam(FNC/RGO/MDCF)was successfully fabricated through a combination of solvo-thermal treatment and high-temperature pyrolysis.Results indicated that RGO was evenly distributed in the MDCF skeleton,providing ef-fective support for the load growth of FNC on its surface.Sample S3,the FNC/RGO/MDCF composite prepared by solvothermal method for 16 h,exhibited a minimum reflection loss(RL_(min))of-66.44 dB at a thickness of 2.29 mm.When the thickness was reduced to 1.50 mm,the optimal effective absorption bandwidth was 3.84 GHz.Analysis of the absorption mechanism of FNC/RGO/MDCF revealed that its excellent absorption performance was primarily attributed to the combined effects of conduction loss,multiple reflection,scattering,in-terface polarization,and dipole polarization.
基金financially supported by the Natural Science Foundation of Jiangsu Province(Grant No.BK20241181)the State Key Laboratory of AnalyticalChemistry for Life Science,School of Chemistry and Chemical Engineering,Nanjing University(Grant No.SKLACLS2419)。
文摘Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.
基金supported by Gansu Provincial Science and Technology Plan(23CXGA0195)Longnan Science and Technology Plan(2024CX03)。
文摘Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,graphene oxide modified asphalt was prepared and characteristics was studied including the high deformation resistance performance and the self-healing property of modified asphalt.Functional groups and morphology of graphene oxide modified asphalt were described by Fourier transform infrared spectroscopy.The high deformation resistance performance and self-healing effect of asphalt samples were obtained through dynamic slear rheometer(DSR)test.Results shows that graphene oxide dispersions improve the performance of asphalt relatively well compared to graphene oxide powder.There is no chemical reaction between graphene oxide and asphalt,but physical connection.The addition of graphene oxide improved the high deformation resistance of modified asphalt and expedited the self-healing ability of asphalt under fatigue load.
基金financial support from the JSPS KAKENHI Grant-in-Aid for Scientific Research(B),No.21H02035KAKENHI Grant-in-Aid for Challenging Research(Exploratory),No.21K19017+2 种基金KAKENHI Grant-in-Aid for Transformative Research Areas(B),No.21H05100National Natural Science Foundation of China,No.22409033 and No.22409035Basic and Applied Basic Research Foundation of Guangdong Province,No.2022A1515110470.
文摘Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SOECs with Zr-rich electrolyte,called Zr-rich side P-SOECs,possess high thermodynamically stability under high steam concentrations but the large reaction resistances and the current leakage,thus the inferior performances.In this study,an efficient functional interlayer Ba_(0.95)La_(0.05)Fe_(0.8)Zn_(0.2)O_(3-δ)(BLFZ)in-between the anode and the electrolyte is developed.The electrochemical performances of P-SOECs are greatly enhanced because the BLFZ can greatly increase the interface contact,boost anode reaction kinetics,and increase proton injection into electrolyte.As a result,the P-SOEC yields high current density of 0.83 A cm^(-2) at 600℃ in 1.3 Vamong all the reported Zr-rich side cells.This work not only offers an efficient functional interlayer for P-SOECs but also holds the potential to achieve P-SOECs with high performances and long-term stability.
基金supported by National Key R&D Program of China(2021YFB4001401)National Natural Science Foundation of China(52272190,22178023).
文摘Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.
基金supported by National Natural Science Foundation of China(22279018)National Natural Science Foundation of China(22005055)Natural Science Foundation of Fujian Province(2022J01085).
文摘Solid oxide cells(SOCs)are emerging devices for efficient energy storage and conversion.However,during SOC operation,gaseous chromium(Cr)species released from Fe-Cr alloy interconnect can lead to Cr deposition and poisoning of air electrodes,causing substantial degradation in electrochemical performance and compromising the longterm stability of SOCs.This mini-review examines the mechanism of Cr deposition and poisoning in air electrodes under both fuel-cell and electrolysis modes.Furthermore,emphasis is placed on the recent advancements in strategies to mitigate Cr poisoning,offering insights into the rational design and development of active and Cr-tolerant air electrodes for SOCs.
文摘Hydrogen (H2) production from renewable biomass resources plays a significant role in solving the shortage of fossil energy;hence, there is an interest in investigating alternative, cleaner processes. This work intends to study the photocatalytic production of hydrogen from D-(+)-Glucose by using different groups of catalysts that have been prepared (M2+ = Zn, Mg and Ni) M2+/Ti4+ Al3+-LDHs (layered double hydroxides). It is then loaded Pd on the catalyst, and the effect of the composite catalyst, layered double hydroxides, is measured. After calcining, the catalyst for the conversion of Layered Double Hydroxides (LDHs) to Layered Double Oxides (LDOs) is used to produce hydrogen gas from glucose. Photocatalytic reforming of glucose-derived compounds is an efficient method for the production of hydrogen. The purpose is to study the effect of metal ions on layered double oxide (LDO) materials by loading Pd and investigate hydrogen production from glucose. The metal cations in the layer were distributed through the preparation of the catalyst process by ion and atom scale between the layers, which were dispersed systematically, as well as the controlled component catalysis. This process shows that ZnTiAl-LDO had the best effect as a catalyst in producing hydrogen compared to NiTiAl-LDO and MgTiAl-LDO.
基金supported by Fundamental Research Funds for the Central Universities(2023KYJD1008)the Science Research Projects of the Anhui Higher Education Institutions of China(2022AH051582).
文摘Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.
文摘Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))around the oxygen vacancies.The origin of the enhanced catalytic activity of ZrO_(2)with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study.Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface,which directly attacked the C-H bond in propane.The involvement of localized electrons activates the C-H bond via back-donation to the antibonding orbital on the defective surface;conversely,charge is transferred from propane to the pristine surfaces.The barrier for the first C-H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces,which verifies the superior activity of Zr_(cus).Notably,however,the desorption of both propene and hydrogen molecules from Zr_(cus)is more difficult due to strong binding.The calculated turnover frequency(TOF)for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures,whereas the defective surfaces have a larger TOF at high temperatures.However,the rate-determining step and reaction order on the defective surface differ from those on the pristine surface,which corroborates that the catalysts follow different mechanisms.A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide.
基金supported by the Jiangxi Provincial Natural Science Foundation of China(Grant number 20224BAB204049)the National Natural Science Foundation of China(Grant number 52205194)the Fund Project of Jiangxi Provincial Department of Education(Grant number GJJ2200602)。
文摘Conventional Fe-C alloy parts used in mechanical transmission and braking systems exposed to the external environment often suffer from wear and corrosion failures.Surface coating strengthening technologies have been explored to improve the surface performance and prolong service life of these parts.Among these technologies,laser cladding has shown promise in producing Fe-based alloy coatings with superior interfacial bonding properties to the Fe-C alloy substrate.Additionally,the microstructure of the Fe-based alloy coating is more uniform and the grain size is finer than that of surfacing welding,thermal spraying,and plasma cladding,and the oxide film of alloying elements on the coating surface can improve the coating performance.However,Fe-based alloy coatings produced by laser cladding typically exhibit lower hardness,lower wear resistance,corrosion resistance,and oxidation resistance compared to coatings based on Co and Ni alloys.Moreover,these coatings are susceptible to defects such as pores and cracks.To address these limitations,the incorporation of rare-earth oxides through doping in the laser cladding process has garnered significant attention.This approach has demonstrated substantial improvements in the microstructure and properties of Fe-based alloy coatings.This paper reviewed recent research on the structure and properties of laser-cladded Fe-based alloy coatings doped with various rare earth oxides,including La_(2)O_(3),CeO_(2),and Y_(2)O_(3).Specifically,it discussed the effects of rare earth oxides and their concentrations on the structure,hardness,friction,wear,corrosion,and oxidation characteristics of these coatings.Furthermore,the mechanisms by which rare earth oxides influence the coating’s structure and properties were summarized.This review aimed to serve as a valuable reference for the application and advancement of laser cladding technology for rare earth modified Fe-based alloy coatings.
基金National Natural Science Foundation of China (NSFC)(52273266, U2001216)Shenzhen Science and Technology Innovation Committee (20231121102401001)+2 种基金Shenzhen Key Laboratory Project (ZDSYS201602261933302)GuangdongHong Kong-Macao Joint Laboratory on Micro-Nano Manufacturing Technology (2021LSYS004)SUSTech high level special funds (G03050K002)。
文摘Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.
基金supported by the National Natural Science Foundation of China(22279026)the National Key Research and Development Program of China(2022YFE0138900)+2 种基金the Young Elite Scientist sponsorship program by CAST(no.20200148)the Natural Science Funds of Heilongjiang Province(YQ2021B003)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process.Herein,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes.Density functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating ability.Molecular dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion interaction.The unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO anodes.Micro-CT further detects the inhibiting effect on the SiO volume expansion.As a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based electrolytes.This work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.
基金financially National Key R&D Program of China(No.2022YFA1504800)National Natural Science Foundation of China(Grant No.22325405,22372160,22321002)+1 种基金Liaoning Revitalization Talents Program(XLYC1807207)DICP I202104。
文摘The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates.In this study,we prepared two Zn-Al spinel oxide catalysts via coprecipitation(ZnAl-C)and hydrothermal(ZnAl-H)methods,and conducted a comparative investigation in the CO_(2)hydrogenation reaction.Surprisingly,under similar conditions,ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H.Comprehensive characterizations using X-ray diffraction(XRD),Raman spectroscopy and electron paramagnetic resonance(EPR)unveiled that ZnAl-C catalyst had abundant ZnO species on its surface,and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies,which are crucial for CO_(2)adsorption and activation.Additionally,state-of-the-art solid-state nuclear magnetic resonance(NMR)techniques,including ex-situ and in-situ NMR analyses,confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species,which was readily hydrogenated to methanol and DME.These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO_(2)-to-methanol hydrogenation reaction,which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst.These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.
基金supported by the Fundamental Research Funds for the Central Universities (2232024Y-01)the National Natural Science Foundation of China (52225204, 52272289, 52173233 and 52402231)+3 种基金the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-03-E00109)the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Natural Science Foundation of Shanghai (23ZR1479200)“Shuguang Program” supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission (20SG33)the DHU Distinguished Young Professor Program (LZA2022001)。
文摘Amorphous RuO_(x)(a-RuO_(x)) with disordered atomic arrangement and abundant coordinatively unsaturated Ru sites possesses high intrinsic electrocatalytic activity for oxygen evolution reaction (OER).However,the a-RuO_(x)is prone to fast corrosion during OER in strong acid.Here we realized the stabilization of an ultrathin a-RuO_(x)layer via constructing heterointerface with crystalline a-MnO_(2)nanorods array (MnO_(2)@aRuO_(x)).Benefiting from the strong electronic interfacial interaction,the as-formed MnO_(2)@a-RuO_(x)electrocatalyst display an ultralow overpotential of 128 mV to reach 10 mA cm^(-2)and stable operation for over 100 h in 0.1 mol L^(-1)HClO_(4).The assembled proton exchange membrane(PEM) water electrolyzer reach 1 A cm^(-2)at applied cell voltage of 1.71 V.Extensive characterizations indicate the MnO_(2)substrate work as an electron donor pool to prevent the overoxidation of Ru sites and the OER proceeds in adsorbent evolution mechanism process without involving lattice oxygen.Our work provides a promising route to construct robust amorphous phase electrocatalysts.
