Carbonaceous materials have drawn much attention in potassium-ion batteries (PIBs) due to their low price and superior physicochemical properties. However, the application of carbonaceous materials in PIB anodes is hi...Carbonaceous materials have drawn much attention in potassium-ion batteries (PIBs) due to their low price and superior physicochemical properties. However, the application of carbonaceous materials in PIB anodes is hindered by sluggish kinetics and large volume expansion. Herein, N/S co-doped carbon nanocapsule (NSCN) is constructed for superior K+ storage. The NSCN possesses 3D nanocapsule framework with abundant meso/macropores, which guarantees structural robustness and accelerates ions/electrons transportation. The high-level N/S co-doping in carbon matrix not only generates ample defects and active sites for K+ adsorption, but also expands interlayer distance for facile K+ intercalation/deintercalation. As a result, the NSCN electrode delivers a high reversible capacity (408 mAh g^(−1) at 0.05 A g^(−1)), outstanding rate capability (149 mAh g^(−1) at 5 A g^(−1)) and favorable cycle stability (150m Ah g^(−1) at 2 A g^(−1) after 2000 cycles). Ex situ TEM, Raman and XPS measurements demonstrate the excellent stability and reversibility of NSCN electrode during potassiation/depotassiation process. This work provides inspiration for the optimization of energy storage materials by structure and doping engineering.展开更多
Seven-day-old maize (Zea mays) plants were grown hydroponically for ten days in deprived nutrient solutions against the corresponding control grown under full nutrition;the effects of S-, N- or P-deprivation on lamina...Seven-day-old maize (Zea mays) plants were grown hydroponically for ten days in deprived nutrient solutions against the corresponding control grown under full nutrition;the effects of S-, N- or P-deprivation on laminas’ mean stomatal conductance (gs), transpiration rate (E) and photosynthetic rate (A) were monitored, along with the impact on the laminas’ total dry mass (DM), water amount (W), length and surface area (Sa). Furthermore, a time series analysis of each parameter’s response ratios (Rr), i.e. the treatment’s value divided by the corresponding control’s one, was performed. Under S-deprivation, the Rr of laminas’ mean gs, E, and A presented oscillations within a ±15% fluctuation zone, notably the “control” zone, whilst those of laminas’ total DM, water amount, surface area, and length included oscillation during the first days and deviation later on, presenting deviation during d10. Under the N-deprivation conditions all Rr time courses except the A one, included early deviations from the control zone without recovering. The deviation from the control zone appeared at d4. Under P-deprivation, all Rr time courses represented oscillations within the control zone. P-deprivation’s patterns resembled those of S-deprivation. Compared to the one of the S-deprivation, the P-one’s oscillations took place within a broader zone. Linear relationships among the various Rr patterns were found between gs-E, gs-A, E-A, DM-W and DM-Sa. In conclusion, the impact of P-deprivation appeared in an early stage and included an alleviation action, the one of N-deprivation appeared early with no alleviation action, whilst that of S-deprivation appeared later, being rather weaker when compared to the impact of the P-deprivation’s impact.展开更多
The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in seconda...Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.展开更多
Plant biomass, primary production and mineral cycling in the beech forest (Fagus sylvatica L.), Hestehave in Jutland, Denmark were studied over a 50-year period. The role of the forest as a carbon sink was also assess...Plant biomass, primary production and mineral cycling in the beech forest (Fagus sylvatica L.), Hestehave in Jutland, Denmark were studied over a 50-year period. The role of the forest as a carbon sink was also assessed. Aboveground tree biomass was 226 t·ha-1 in 1970 and after a 50-year 539 t·ha-1 in 2014, an unexpected increase with 313 t·ha-1. Annual production at those two points in time was 13.4 and 20.5 t·ha-1, respectively. It was apparent that the tree biomass was still acting as a sink for carbon, which was the dominant element in the aboveground parts. The concentration of other elements (N > K > Mg > P > S > Na > Mn > Zn > Fe > Cu) ranged from 495 to 0.4 kg·ha-1. Annual litterfall restored 3.2 t·ha-1 to the soil as organic matter or 1.6 t·ha-1 as carbon. Over the year 53% of the litterfall was decomposed. A pH decrease of 0.95 units in the soil was observed between 1968 and 1993. This was attributed to fallout from a neighbouring thermal heating station affecting sulfur deposition and increasing soil acidification. After 1993, when filters were fitted in the heating station, the pH decrease in the soil was smaller, only 0.09 pH-units up to 2011. The increased tree growth is an additional, likely explanation for the observed soil acidification. Deposition of the growth-limiting element nitrogen increased during later years and is now, most likely around 20 kg·ha-1 per annum, which may partly contribute to the increased production.展开更多
The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple ...The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.展开更多
Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hier...Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.展开更多
Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples w...Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.展开更多
The development of highly efficient non-precious-metal-based electrocatalysts for the hydrogen evolution reaction is imperative for promoting the large-scale application of electrochemical water splitting.Herein,nitro...The development of highly efficient non-precious-metal-based electrocatalysts for the hydrogen evolution reaction is imperative for promoting the large-scale application of electrochemical water splitting.Herein,nitrogen/phosphorus co-doped carbon nanorods encapsulated Mo_(2)C nanoparticles(Mo_(2)C@PNc)have been prepared by pre-phosphating treatment in combination of the coordination with polydopamine and the subsequent pyrolysis.The phosphating temperature has a significant effect on the content of phosphorus within the resultant Mo_(2)C@PNC,and the optimal catalyst delivers superior HER activity with the low overpotential of 104 mV at a current density of 10 mAcm^(-2) and good stability for 8 h,which has been theoretically demonstrated to originate from the synergistic effect between P doping and Mo_(2)C induced electron redistribution of nitrogen-doped carbon layer.展开更多
In this paper,we investigate sufficient and necessary conditions such that generalized Forelli-Rudin type operators T_(λ,τ,k),S_(λ,τ,k),Q_(λ,τ,k)and R_(λ,τ,k)are bounded between Lebesgue type spaces.In order t...In this paper,we investigate sufficient and necessary conditions such that generalized Forelli-Rudin type operators T_(λ,τ,k),S_(λ,τ,k),Q_(λ,τ,k)and R_(λ,τ,k)are bounded between Lebesgue type spaces.In order to prove the main results,we first give some bidirectional estimates for several typical integrals.展开更多
Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dend...Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dendritic Li formation,dramatical volume variation and serious pulverization.Herein,manganese dioxide (MnO_(2)) nanosheet modified nitrogen (N),phosphorus (P) co-doping carbon nanofibers(NPC) on carbon cloth (CC)(MnO_(2)@NPC-CC) is successfully fabricated through electrodeposition approach and further treated with Li by the molten-infusion method to prepare Li based Mn@NPC-CC(Li-Mn@NPC-CC) electrode.The synergy of MnO_(2) and NPC obviously increases the reaction rate between MnO_(2)@NPC-CC and Li and guides even Li distribution over infusion process.Additionally,theoretical calculation,simulation and experimental results further indicate that N,P,Mn multi-doping effectively improves the superior lithiophilicity of Li-Mn@NPC-CC,which induces uniform Li deposition/dissolution to suppress dendrite growth over cycles.Moreover,conductive and porous NPC matrix not only effectively improves the stability of Li-Mn@NPC-CC,but also provides abundant spaces to accelerate the transfer of ion/electron and buffer electrode dimension variation during cycling.Hence,Li-Mn@NPC-CC-based symmetric cells exhibit extra-long cycling life (over 2200 h) with small hysteresis of 20 mV.When the LiMn@NPC-CC anode couples with air,Li iron phosphate (LiFePO_(4)),or hard carbon (C) cathode,the assembled full cells exhibit outstanding performance with low hysteresis and stable cycling properties.Especially,the corresponding pouch-typed Li–air cells also exhibit good performance at different bending angles and even power a series of electronic devices.展开更多
Plant biomass, primary production and mineral cycling were studied in a mixed deciduous forest (Quercus robur L., Tilia cordata L. and Corylus avellana L.) in southern Sweden. Plant biomass amount above and below grou...Plant biomass, primary production and mineral cycling were studied in a mixed deciduous forest (Quercus robur L., Tilia cordata L. and Corylus avellana L.) in southern Sweden. Plant biomass amount above and below ground was 201 and 37 t·ha-1, respectively. Primary production above and below ground was an estimated 13.3 and 2.3 t·ha-1, respectively. Carbon was the dominant element in the forest ecosystem, comprising 133 t·ha-1. Other major elements were: N > Ca > K > Si > Mg > S > Mn > P > Fe and Na (range 1123 to 18 kg·ha-1), followed by some trace elements. Yearly litterfall restored 6.0 t·ha-1 organic matter or 2.3 t·ha-1 carbon. Approximately 45% decomposed and returned to the soil during the year. Monitoring of other elements revealed that the ecosystem received inputs through dry and wet deposition, in particular 34.4 kg·ha-1 S and 9.4 kg·ha-1 of N yearly as throughfall. Determination of yearly biomass increase showed that the oak forest ecosystem was still in an aggradation or accumulation phase.展开更多
Neutron capture therapy with Sulfur-33, similar to boron neutron capture therapy with Boron-10, is effective in treating some types of tumors including ocular melanoma. The key point in sulfur neutron capture therapy ...Neutron capture therapy with Sulfur-33, similar to boron neutron capture therapy with Boron-10, is effective in treating some types of tumors including ocular melanoma. The key point in sulfur neutron capture therapy is whether the neutron beam flux and the resonance capture cross section of ^(33)S(n;α)^(30) Si reaction at 13.5 keV can achieve the requirements of radiotherapy. In this research,the authors investigated the production of 13.5 keV neutron production and moderation based on an accelerator neutron source. A lithium glass detector was used to measure the neutron flux produced via near threshold^7 Li(p,n)~7 Be reaction using the time-of-flight method. Furthermore, the moderation effects of different kinds of materials were investigated using Monte Carlo simulation.展开更多
The development of aqueous zinc-ion batteries (AZIBs) marks a significant advancement in the field of sustainable and environmentally friendly energy storage.To address the challenges faced by singlephase vanadium-bas...The development of aqueous zinc-ion batteries (AZIBs) marks a significant advancement in the field of sustainable and environmentally friendly energy storage.To address the challenges faced by singlephase vanadium-based oxides,such as poor conductivity and dissolution in electrolytes,this study introduces vacuum S/N doping to fabricate V_(2)O_(3)/VO_(2)@S/N-C nanofibers,improving the cycling stability and enhancing the capacity.The V_(2)O_(3)/VO_(2)@S/N-C electrode exhibits exceptional cyclic stability,retaining a capacity of 133.3 m A h g^(-1)after 30,000 cycles at a high current density of 100 A g^(-1)and a capacity retention of 81.8%after 150,000 cycles at 200 A g^(-1).Characterizations using ex-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy reveal co-intercalation of H^(+)and Zn^(2+)in the V_(2)O_(3)/VO_(2)@S/N-C electrode.Due to the presence of S_(2)^(2-),more phases changed to V_(10)O_(24).12H_(2)O,making the V_(2)O_(3)/VO_(2)@S/N-C electrode better reversible.By elucidating the zinc storage mechanism and demonstrating the stable performance of the doped electrode,this work contributes valuable insights into the optimization of the electrode materials for future energy storage solutions.展开更多
Developing highly efficient and stable platinum-based electrocatalyst for oxygen reduction reaction(ORR) is critical to expediting commercialization of fuel cells.Herein,several PtCu alloy nanocatalysts supported on N...Developing highly efficient and stable platinum-based electrocatalyst for oxygen reduction reaction(ORR) is critical to expediting commercialization of fuel cells.Herein,several PtCu alloy nanocatalysts supported on N,P co-doped carbon(PtCu/NPC) were prepared by microbial-sorption and carbonization-reduction.Among them,PtCu/NPC-700 ℃ exhibits excellent catalytic performance for ORR with a mass activity of 0.895 A mg_(pt)^(-1)(@0.9 V) which is 8.29 folds of commercial Pt/C.Additionally,the ECSA and MA of PtCu/NPC-700℃ only decrease by 14.2% and 18.7% respectively,while Pt/C decreases by 35.2% and 52.8% after 10,000 cycles of ADT test.Moreover,the PtCu/NPC-700℃ catalyst emanates a maximum power density of 715 mW cm^(-2) and only 11.1% loss of maximum power density after 10,000 ADTs in single-cell test,indicating PtCu/NPC-700℃ also manifests higher activity and durability in actual single-cell operation than Pt/C.This research provides an easy and novel strategy for developing highly active and durable Pt-based alloy catalyst.展开更多
We report the performances of a chalcopyrite Cu(In, Ga)Se<sub>2 </sub>CIGS-based thin-film solar cell with a newly employed high conductive n-Si layer. The data analysis was performed with the help of the ...We report the performances of a chalcopyrite Cu(In, Ga)Se<sub>2 </sub>CIGS-based thin-film solar cell with a newly employed high conductive n-Si layer. The data analysis was performed with the help of the 1D-Solar Cell Capacitance Simulator (1D-SCAPS) software program. The new device structure is based on the CIGS layer as the absorber layer, n-Si as the high conductive layer, i-In<sub>2</sub>S<sub>3</sub>, and i-ZnO as the buffer and window layers, respectively. The optimum CIGS bandgap was determined first and used to simulate and analyze the cell performance throughout the experiment. This analysis revealed that the absorber layer’s optimum bandgap value has to be 1.4 eV to achieve maximum efficiency of 22.57%. Subsequently, output solar cell parameters were analyzed as a function of CIGS layer thickness, defect density, and the operating temperature with an optimized n-Si layer. The newly modeled device has a p-CIGS/n-Si/In<sub>2</sub>S<sub>3</sub>/Al-ZnO structure. The main objective was to improve the overall cell performance while optimizing the thickness of absorber layers, defect density, bandgap, and operating temperature with the newly employed optimized n-Si layer. The increase of absorber layer thickness from 0.2 - 2 µm showed an upward trend in the cell’s performance, while the increase of defect density and operating temperature showed a downward trend in solar cell performance. This study illustrates that the proposed cell structure shows higher cell performances and can be fabricated on the lab-scale and industrial levels.展开更多
Limited lithium resources have promoted the exploration of new battery technologies.Among them,potassium-ion batteries are considered as promising alternatives.At present,commercial graphite and other carbon-based mat...Limited lithium resources have promoted the exploration of new battery technologies.Among them,potassium-ion batteries are considered as promising alternatives.At present,commercial graphite and other carbon-based materials have shown good prospects as anodes for potassium-ion batteries.However,the volume expansion and structural collapse caused by periodic K+insertion/extraction have severely restricted further development and application of potassium-ion batteries.A hollow biomass carbon ball(NOP-PB)ternarily doped with N,O,and P was synthesized and used as the negative electrode of a potassium-ion battery.X-ray photoelectron spectroscopy,Fourier‐transform infrared spectroscopy,and transmission electron microscopy confirmed that the hollow biomass carbon spheres were successfully doped with N,O,and P.Further analysis proved that N,O,and P ternary doping expands the interlayer distance of the graphite surface and introduces more defect sites.DFT calculations simultaneously proved that the K adsorption energy of the doped structure is greatly improved.The solid hollow hierarchical porous structure buffers the volume expansion of the potassium insertion process,maintains the original structure after a long cycle and promotes the transfer of potassium ions and electrons.Therefore,the NOP‐PB negative electrode shows extremely enhanced electrochemical performance,including high specific capacity,excellent long‐term stability,and good rate stability.展开更多
This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)w...This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)with different content(mCu-xNP/AC)were manufactured and applied in the acetylene hydrochlorination reaction.It was found that the doping of carriers N and P induced the transformation of Cu^(2+)to Cu^(+),and the catalytic activity was markedly improved.Under the optimal reaction temperature of 220℃,the gas hourly space velocity(GHSV)of C_(2)H_(2)was 90 h^(-1)and V_(HCl):V_(C_(2)H_(2))was 1.15.The initial activity of the 5%Cu-30 NP/AC catalyst reached 95.59%.Through some characterization methods showed the addition of N and P improved the dispersion of Cu in carbon,which increased the ratio of Cu^+/Cu^(2+).The measurement results confirmed that the chemisorption capacity of mCu-xNP/AC for C_(2)H_(2)decreased slightly,and the chemisorption capacity for HCl increased significantly,which was the reason for the increased activity of the catalyst.The conclusion provides a reference for the development of acetylene hydrochlorination Cu catalyst.展开更多
基金the financial supports from the National Natural Science Foundation of China(Grant Nos.51872005,U1508201,52072002)。
文摘Carbonaceous materials have drawn much attention in potassium-ion batteries (PIBs) due to their low price and superior physicochemical properties. However, the application of carbonaceous materials in PIB anodes is hindered by sluggish kinetics and large volume expansion. Herein, N/S co-doped carbon nanocapsule (NSCN) is constructed for superior K+ storage. The NSCN possesses 3D nanocapsule framework with abundant meso/macropores, which guarantees structural robustness and accelerates ions/electrons transportation. The high-level N/S co-doping in carbon matrix not only generates ample defects and active sites for K+ adsorption, but also expands interlayer distance for facile K+ intercalation/deintercalation. As a result, the NSCN electrode delivers a high reversible capacity (408 mAh g^(−1) at 0.05 A g^(−1)), outstanding rate capability (149 mAh g^(−1) at 5 A g^(−1)) and favorable cycle stability (150m Ah g^(−1) at 2 A g^(−1) after 2000 cycles). Ex situ TEM, Raman and XPS measurements demonstrate the excellent stability and reversibility of NSCN electrode during potassiation/depotassiation process. This work provides inspiration for the optimization of energy storage materials by structure and doping engineering.
文摘Seven-day-old maize (Zea mays) plants were grown hydroponically for ten days in deprived nutrient solutions against the corresponding control grown under full nutrition;the effects of S-, N- or P-deprivation on laminas’ mean stomatal conductance (gs), transpiration rate (E) and photosynthetic rate (A) were monitored, along with the impact on the laminas’ total dry mass (DM), water amount (W), length and surface area (Sa). Furthermore, a time series analysis of each parameter’s response ratios (Rr), i.e. the treatment’s value divided by the corresponding control’s one, was performed. Under S-deprivation, the Rr of laminas’ mean gs, E, and A presented oscillations within a ±15% fluctuation zone, notably the “control” zone, whilst those of laminas’ total DM, water amount, surface area, and length included oscillation during the first days and deviation later on, presenting deviation during d10. Under the N-deprivation conditions all Rr time courses except the A one, included early deviations from the control zone without recovering. The deviation from the control zone appeared at d4. Under P-deprivation, all Rr time courses represented oscillations within the control zone. P-deprivation’s patterns resembled those of S-deprivation. Compared to the one of the S-deprivation, the P-one’s oscillations took place within a broader zone. Linear relationships among the various Rr patterns were found between gs-E, gs-A, E-A, DM-W and DM-Sa. In conclusion, the impact of P-deprivation appeared in an early stage and included an alleviation action, the one of N-deprivation appeared early with no alleviation action, whilst that of S-deprivation appeared later, being rather weaker when compared to the impact of the P-deprivation’s impact.
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金financially supported by the Shenzhen Science and Technology Program(JCYJ20220530141012028),ChinaThe National Natural Science Foundation of China(22005178),China+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01),ChianThe fellowship of China Postdoctoral Science Foundation(2022M722333),Chianthe Jiangsu Funding Program for Excellent Postdoctoral Talent,Chian。
文摘Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.
文摘Plant biomass, primary production and mineral cycling in the beech forest (Fagus sylvatica L.), Hestehave in Jutland, Denmark were studied over a 50-year period. The role of the forest as a carbon sink was also assessed. Aboveground tree biomass was 226 t·ha-1 in 1970 and after a 50-year 539 t·ha-1 in 2014, an unexpected increase with 313 t·ha-1. Annual production at those two points in time was 13.4 and 20.5 t·ha-1, respectively. It was apparent that the tree biomass was still acting as a sink for carbon, which was the dominant element in the aboveground parts. The concentration of other elements (N > K > Mg > P > S > Na > Mn > Zn > Fe > Cu) ranged from 495 to 0.4 kg·ha-1. Annual litterfall restored 3.2 t·ha-1 to the soil as organic matter or 1.6 t·ha-1 as carbon. Over the year 53% of the litterfall was decomposed. A pH decrease of 0.95 units in the soil was observed between 1968 and 1993. This was attributed to fallout from a neighbouring thermal heating station affecting sulfur deposition and increasing soil acidification. After 1993, when filters were fitted in the heating station, the pH decrease in the soil was smaller, only 0.09 pH-units up to 2011. The increased tree growth is an additional, likely explanation for the observed soil acidification. Deposition of the growth-limiting element nitrogen increased during later years and is now, most likely around 20 kg·ha-1 per annum, which may partly contribute to the increased production.
基金supported by the National Natural Science Foundation of China(52374301 and 22279030)the Fundamental Research Funds for the Central Universities(N2223037)+1 种基金Hebei Key Laboratory of Dielectric and Electrolyte Functional Material,Northeastern University at Qinhuangdao(HKDEFM2021201)the Performance subsidy fund for the Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(22567627H)。
文摘The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.
基金financial support from the National Natural Science Foundation of China (21773111, 21473089, 21573107 and 51571110)the National Key Research and Development Program of China (2017YFA0206503, 2018YFA0209103)+1 种基金Priority Academic Program Development of Jiangsu Higher Education Institutions, Fundamental Research Funds for the Central Universitiesthe program B for outstanding PhD candidate of Nanjing University (201702B049)
文摘Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.
文摘Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.
基金financially supported by Fundamental Research Funds for the Central Universities(No.531118010232 and No.202044011)the Natural Science Foundation of Changsha(No.KQ2202146 and No.KQ2208259)the"Young Talent Support Plan"of Xi'an Jiaotong University.
文摘The development of highly efficient non-precious-metal-based electrocatalysts for the hydrogen evolution reaction is imperative for promoting the large-scale application of electrochemical water splitting.Herein,nitrogen/phosphorus co-doped carbon nanorods encapsulated Mo_(2)C nanoparticles(Mo_(2)C@PNc)have been prepared by pre-phosphating treatment in combination of the coordination with polydopamine and the subsequent pyrolysis.The phosphating temperature has a significant effect on the content of phosphorus within the resultant Mo_(2)C@PNC,and the optimal catalyst delivers superior HER activity with the low overpotential of 104 mV at a current density of 10 mAcm^(-2) and good stability for 8 h,which has been theoretically demonstrated to originate from the synergistic effect between P doping and Mo_(2)C induced electron redistribution of nitrogen-doped carbon layer.
基金supported by the Natural Science Foundation of Hunan Province of China(2022JJ30369)the Education Department Important Foundation of Hunan Province in China(23A0095)。
文摘In this paper,we investigate sufficient and necessary conditions such that generalized Forelli-Rudin type operators T_(λ,τ,k),S_(λ,τ,k),Q_(λ,τ,k)and R_(λ,τ,k)are bounded between Lebesgue type spaces.In order to prove the main results,we first give some bidirectional estimates for several typical integrals.
基金funding support from the National Natural Science Foundation of China (21905151 and 51772162)the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China (2019KJC004)+1 种基金the Outstanding Youth Foundation of Shandong Province, China (ZR2019JQ14)the Taishan Scholar Young Talent Program, Major Scientific and Technological Innovation Project (2019JZZY020405)。
文摘Lithium (Li) metal batteries have attracted much attention owing to its ultra-high energy density.However,as important part of Li metal batteries,Li anodes still face many challenges,mainly including uncontrolled dendritic Li formation,dramatical volume variation and serious pulverization.Herein,manganese dioxide (MnO_(2)) nanosheet modified nitrogen (N),phosphorus (P) co-doping carbon nanofibers(NPC) on carbon cloth (CC)(MnO_(2)@NPC-CC) is successfully fabricated through electrodeposition approach and further treated with Li by the molten-infusion method to prepare Li based Mn@NPC-CC(Li-Mn@NPC-CC) electrode.The synergy of MnO_(2) and NPC obviously increases the reaction rate between MnO_(2)@NPC-CC and Li and guides even Li distribution over infusion process.Additionally,theoretical calculation,simulation and experimental results further indicate that N,P,Mn multi-doping effectively improves the superior lithiophilicity of Li-Mn@NPC-CC,which induces uniform Li deposition/dissolution to suppress dendrite growth over cycles.Moreover,conductive and porous NPC matrix not only effectively improves the stability of Li-Mn@NPC-CC,but also provides abundant spaces to accelerate the transfer of ion/electron and buffer electrode dimension variation during cycling.Hence,Li-Mn@NPC-CC-based symmetric cells exhibit extra-long cycling life (over 2200 h) with small hysteresis of 20 mV.When the LiMn@NPC-CC anode couples with air,Li iron phosphate (LiFePO_(4)),or hard carbon (C) cathode,the assembled full cells exhibit outstanding performance with low hysteresis and stable cycling properties.Especially,the corresponding pouch-typed Li–air cells also exhibit good performance at different bending angles and even power a series of electronic devices.
文摘Plant biomass, primary production and mineral cycling were studied in a mixed deciduous forest (Quercus robur L., Tilia cordata L. and Corylus avellana L.) in southern Sweden. Plant biomass amount above and below ground was 201 and 37 t·ha-1, respectively. Primary production above and below ground was an estimated 13.3 and 2.3 t·ha-1, respectively. Carbon was the dominant element in the forest ecosystem, comprising 133 t·ha-1. Other major elements were: N > Ca > K > Si > Mg > S > Mn > P > Fe and Na (range 1123 to 18 kg·ha-1), followed by some trace elements. Yearly litterfall restored 6.0 t·ha-1 organic matter or 2.3 t·ha-1 carbon. Approximately 45% decomposed and returned to the soil during the year. Monitoring of other elements revealed that the ecosystem received inputs through dry and wet deposition, in particular 34.4 kg·ha-1 S and 9.4 kg·ha-1 of N yearly as throughfall. Determination of yearly biomass increase showed that the oak forest ecosystem was still in an aggradation or accumulation phase.
文摘Neutron capture therapy with Sulfur-33, similar to boron neutron capture therapy with Boron-10, is effective in treating some types of tumors including ocular melanoma. The key point in sulfur neutron capture therapy is whether the neutron beam flux and the resonance capture cross section of ^(33)S(n;α)^(30) Si reaction at 13.5 keV can achieve the requirements of radiotherapy. In this research,the authors investigated the production of 13.5 keV neutron production and moderation based on an accelerator neutron source. A lithium glass detector was used to measure the neutron flux produced via near threshold^7 Li(p,n)~7 Be reaction using the time-of-flight method. Furthermore, the moderation effects of different kinds of materials were investigated using Monte Carlo simulation.
基金financially supported by the Natural Science Foundation of China (Grant No. 52272063)the Jiangxi Provincial Natural Science Foundation (No. 20224BAB214037, 20232BAB204022, 20232BAB204019)。
文摘The development of aqueous zinc-ion batteries (AZIBs) marks a significant advancement in the field of sustainable and environmentally friendly energy storage.To address the challenges faced by singlephase vanadium-based oxides,such as poor conductivity and dissolution in electrolytes,this study introduces vacuum S/N doping to fabricate V_(2)O_(3)/VO_(2)@S/N-C nanofibers,improving the cycling stability and enhancing the capacity.The V_(2)O_(3)/VO_(2)@S/N-C electrode exhibits exceptional cyclic stability,retaining a capacity of 133.3 m A h g^(-1)after 30,000 cycles at a high current density of 100 A g^(-1)and a capacity retention of 81.8%after 150,000 cycles at 200 A g^(-1).Characterizations using ex-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy reveal co-intercalation of H^(+)and Zn^(2+)in the V_(2)O_(3)/VO_(2)@S/N-C electrode.Due to the presence of S_(2)^(2-),more phases changed to V_(10)O_(24).12H_(2)O,making the V_(2)O_(3)/VO_(2)@S/N-C electrode better reversible.By elucidating the zinc storage mechanism and demonstrating the stable performance of the doped electrode,this work contributes valuable insights into the optimization of the electrode materials for future energy storage solutions.
基金supported by funding from the National Natural Science Foundation of China (12074435 and 52001335)the Science and Technology Innovation Program of Hunan Province (2021RC4001)the Natural Science Foundation of Yunnan Province (202201AT070259)。
文摘Developing highly efficient and stable platinum-based electrocatalyst for oxygen reduction reaction(ORR) is critical to expediting commercialization of fuel cells.Herein,several PtCu alloy nanocatalysts supported on N,P co-doped carbon(PtCu/NPC) were prepared by microbial-sorption and carbonization-reduction.Among them,PtCu/NPC-700 ℃ exhibits excellent catalytic performance for ORR with a mass activity of 0.895 A mg_(pt)^(-1)(@0.9 V) which is 8.29 folds of commercial Pt/C.Additionally,the ECSA and MA of PtCu/NPC-700℃ only decrease by 14.2% and 18.7% respectively,while Pt/C decreases by 35.2% and 52.8% after 10,000 cycles of ADT test.Moreover,the PtCu/NPC-700℃ catalyst emanates a maximum power density of 715 mW cm^(-2) and only 11.1% loss of maximum power density after 10,000 ADTs in single-cell test,indicating PtCu/NPC-700℃ also manifests higher activity and durability in actual single-cell operation than Pt/C.This research provides an easy and novel strategy for developing highly active and durable Pt-based alloy catalyst.
文摘We report the performances of a chalcopyrite Cu(In, Ga)Se<sub>2 </sub>CIGS-based thin-film solar cell with a newly employed high conductive n-Si layer. The data analysis was performed with the help of the 1D-Solar Cell Capacitance Simulator (1D-SCAPS) software program. The new device structure is based on the CIGS layer as the absorber layer, n-Si as the high conductive layer, i-In<sub>2</sub>S<sub>3</sub>, and i-ZnO as the buffer and window layers, respectively. The optimum CIGS bandgap was determined first and used to simulate and analyze the cell performance throughout the experiment. This analysis revealed that the absorber layer’s optimum bandgap value has to be 1.4 eV to achieve maximum efficiency of 22.57%. Subsequently, output solar cell parameters were analyzed as a function of CIGS layer thickness, defect density, and the operating temperature with an optimized n-Si layer. The newly modeled device has a p-CIGS/n-Si/In<sub>2</sub>S<sub>3</sub>/Al-ZnO structure. The main objective was to improve the overall cell performance while optimizing the thickness of absorber layers, defect density, bandgap, and operating temperature with the newly employed optimized n-Si layer. The increase of absorber layer thickness from 0.2 - 2 µm showed an upward trend in the cell’s performance, while the increase of defect density and operating temperature showed a downward trend in solar cell performance. This study illustrates that the proposed cell structure shows higher cell performances and can be fabricated on the lab-scale and industrial levels.
基金The authors are grateful for support from the National Natural Science Foundation of China(No.21671160).
文摘Limited lithium resources have promoted the exploration of new battery technologies.Among them,potassium-ion batteries are considered as promising alternatives.At present,commercial graphite and other carbon-based materials have shown good prospects as anodes for potassium-ion batteries.However,the volume expansion and structural collapse caused by periodic K+insertion/extraction have severely restricted further development and application of potassium-ion batteries.A hollow biomass carbon ball(NOP-PB)ternarily doped with N,O,and P was synthesized and used as the negative electrode of a potassium-ion battery.X-ray photoelectron spectroscopy,Fourier‐transform infrared spectroscopy,and transmission electron microscopy confirmed that the hollow biomass carbon spheres were successfully doped with N,O,and P.Further analysis proved that N,O,and P ternary doping expands the interlayer distance of the graphite surface and introduces more defect sites.DFT calculations simultaneously proved that the K adsorption energy of the doped structure is greatly improved.The solid hollow hierarchical porous structure buffers the volume expansion of the potassium insertion process,maintains the original structure after a long cycle and promotes the transfer of potassium ions and electrons.Therefore,the NOP‐PB negative electrode shows extremely enhanced electrochemical performance,including high specific capacity,excellent long‐term stability,and good rate stability.
基金supported by the Taishan Scholars Program of Shandong Province(tsqn202103051)the Project of Scientific Research in Shihezi University(CXFZ202205)。
文摘This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)with different content(mCu-xNP/AC)were manufactured and applied in the acetylene hydrochlorination reaction.It was found that the doping of carriers N and P induced the transformation of Cu^(2+)to Cu^(+),and the catalytic activity was markedly improved.Under the optimal reaction temperature of 220℃,the gas hourly space velocity(GHSV)of C_(2)H_(2)was 90 h^(-1)and V_(HCl):V_(C_(2)H_(2))was 1.15.The initial activity of the 5%Cu-30 NP/AC catalyst reached 95.59%.Through some characterization methods showed the addition of N and P improved the dispersion of Cu in carbon,which increased the ratio of Cu^+/Cu^(2+).The measurement results confirmed that the chemisorption capacity of mCu-xNP/AC for C_(2)H_(2)decreased slightly,and the chemisorption capacity for HCl increased significantly,which was the reason for the increased activity of the catalyst.The conclusion provides a reference for the development of acetylene hydrochlorination Cu catalyst.