Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen e...Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.展开更多
The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow...The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow charge transfer dynamics and severe charge recombination at the interface.Herein,a novel“killing two birds with one stone”approach was discovered by employing CoPi as an interface mediator,which shifts its charge transfer behavior from conventional hole storage or passivation to hole transporter.The optimized BiVO_(4)/CoPi/FeOOH photoanode achieves a noteworthy photocurrent density of 5.4 mA/cm^(2) and exhibits long term stability(13 h).The dynamic analysis and electrochemical characterization reveal that CoPi can rapidly and directly transfer more photogenerated holes to the surface of OEC in comparison to traditional slow holes transfer behavior,resulting in highly efficient interface charge separation.Interestingly,the strong interfacial interactions can also be extended to OEC/electrolyte interface,specifically by promoting the surface reaction dynamics.Moreover,this innovative approach of altering behavior of CoPi can also be utilized to design other photoanodes,like BiVO_(4)/CoPi/NiOOH,aimed at efficient PEC water splitting.This finding affords a smart strategy to develop highly efficient and stable photoelectrodes for water splitting.展开更多
The aim of this article is to study the structures of arbitrary split δ-Jordan Lie triple systems, which are a generalization of split Lie triple systems. By developing techniques of connections of roots for this kin...The aim of this article is to study the structures of arbitrary split δ-Jordan Lie triple systems, which are a generalization of split Lie triple systems. By developing techniques of connections of roots for this kind of triple systems, we show that any of such δ-Jordan Lie triple systems T with a symmetric root system is of the form T=U+∑[α]∈■1/~I[α] with U a subspace of T0 and any I[α] a well described ideal of T, satisfying{I[α],T,I[β]}={I[α],I[β],T}={T,I[α],I[β]}=0 if [α]≠[β] .展开更多
Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by ...Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.展开更多
This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abun...This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.展开更多
The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use e...The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use efficiency and enhancing crop stress resistance.Nevertheless,the precise interaction between soil warming(SW)and SN remains unclear.In order to ascertain the impact of SW on maize growth and whether SN can improve the tolerance of maize to SW,a two-year field experiment was conducted(2022-2023).The aim was to examine the influence of two SW ranges(MT,warming 1.40℃;HT,warming 2.75℃)and two nitrogen application methods(N1,one-time basal application of nitrogen fertilizer;N2,one third of base nitrogen fertilizer+two thirds of jointing stage supplemental nitrogen fertilizer)on maize root growth,photosynthetic characteristics,nitrogen use efficiency,and yield.The results demonstrated that SW impeded root growth and precipitated the premature aging of maize leaves following anthesis,particularly in the HT,which led to a notable reduction in maize yield.In comparison to N1,SN has been shown to increase root length density by 8.54%,root bleeding rate by 8.57%,and enhance root distribution ratio in the middle soil layers(20-60 cm).The interaction between SW and SN had a notable impact on maize growth and yield.The SN improved the absorption and utilization efficiency of nitrogen by promoting root development and downward canopy growth,thus improving the tolerance of maize to SW at the later stage of growth.In particular,the N2HT resulted in a 14.51%increase in the photosynthetic rate,a 18.58%increase in nitrogen absorption efficiency,and a 18.32%increase in maize yield compared with N1HT.It can be posited that the SN represents a viable nitrogen management measure with the potential to enhance maize tolerance to soil high-temperature stress.展开更多
Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the ...Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.展开更多
The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplore...The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplored challenge of substantial electrochemical overpotential,surface reconstruction has emerged as a necessary strategy.Focusing on key aspects such as Janus structures,overflow effects,the d-band center displacement hypothesis,and interface coupling related to electrochemical reactions is essential for water electrolysis.Emerging as frontrunners among next-generation electrocatalysts,Mott-Schottky(M-S)catalysts feature a heterojunction formed between a metal and a semiconductor,offering customizable and predictable interfacial synergy.This review offers an in-depth examination of the processes driving the hydrogen and oxygen evolution reactions(HER and OER),highlighting the benefits of employing nanoscale transition metal nitrides,carbides,oxides,and phosphides in M-S heterointerface catalysts.Furthermore,the challenges,limitations,and future prospects of employing M-S heterostructured catalysts for water splitting are thoroughly discussed.展开更多
The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical chal...The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical challenges in industrial alkaline electrolysis,particularly elucidating hydrogen and oxygen evolution reaction(HER/OER)mechanisms while addressing the persistent activity-stability trade-off.This review summarizes their decade-long progress in developing advanced electrodes,analyzing the origins of sluggish alkaline HER kinetics and OER stability limitations.Professor Wei proposes a unifying"12345 Principle"as an optimization framework.For HER electrocatalysts,they have identified that metal/metal oxide interfaces create synergistic"chimney effect"and"local electric field enhancement effect",enhancing selective intermediate adsorption,interfacial water enrichment/reorientation,and mass transport under industrial high-polarization conditions.Regarding OER,innovative strategies,including dual-ligand synergistic modulation,lattice oxygen suppression,and self-repairing surface construction,are demonstrated to balance oxygen species adsorption,optimize spin states,and dynamically reinforce metal-oxygen bonds for concurrent activity-stability enhancement.The review concludes by addressing remaining challenges in long-term industrial durability and suggesting future research priorities.展开更多
Transition metal phosphides(TMPs),with tunable electronic structures and diverse compositions,are promising candidates for electrocatalytic water splitting.However,their unsatisfactory electrical conductivity and tend...Transition metal phosphides(TMPs),with tunable electronic structures and diverse compositions,are promising candidates for electrocatalytic water splitting.However,their unsatisfactory electrical conductivity and tendency to aggregate during reactions result in structural instability,ultimately hindering further improvement of their electrocatalytic performance.To address these issues,a bamboo-leaf-like FeCoP/MXene heterojunction was synthesized by hydrothermal and thermal treatments,utilizing highly conductive MXene as the substrate.Density functional theory(DFT)calculations and experimental characterization reveal that strong Ti-O-Co/Fe covalent bond are formed between MXene and FeCoP through hybridization of O 2p and Co/Fe 3d orbitals,which enhance the structural stability of the interface and facilitate the effective anchoring of FeCoP on the MXene surface.Consequently,the structural stability and electrical conductivity of the catalyst are improved simultaneously.Additionally,interfacial charge redistribution optimizes the Gibbs free energy of hydrogen adsorption at the Co,Fe,and Ti sites while promoting the adsorption and activation of water molecules.These factors interact synergistically,leading to enhanced bi-functional electrocatalytic performance for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In a FeCoP/MXene(+‖-)two-electrode system,the catalyst achieves a current density of 10 mA cm^(-2)at a potential of 1.5 V,which is superior to the RuO_(2)(+)‖Pt/C(-)system.The assembled water splitting device exhibits long-term stability for up to 100 h at a current density of 100 mA cm^(-2).Furthermore,an anion exchange membrane water electrolyzer(AEMWE)equipped with FeCoP/MXene as both anode and cathode achieves an industrial-grade current density of 500 mA cm^(-2)at 1.83 V.These results highlight the critical role of interfacial engineering in enhancing the electrocatalytic performance of TMPs for water splitting and provide valuable insights for the design of novel bifunctional TMP catalysts.展开更多
Developing BiVO_(4)photoanode with efficient carrier transfer and fast water oxidation kinetics is the permanent pursuit to achieve the state-of-art solar-driven photoelectrochemical(PEC)water splitting.The capacity t...Developing BiVO_(4)photoanode with efficient carrier transfer and fast water oxidation kinetics is the permanent pursuit to achieve the state-of-art solar-driven photoelectrochemical(PEC)water splitting.The capacity to increase the PEC activity of BiVO_(4)by loading oxygen evolution co-catalysts(OECs)has been proven,however it suffers from sluggish charge carriers dynamics brought on by the complicated interface between BiVO_(4)and OECs as well as poor long-term durability.Herein,we connected OECs(NiFeOx)and photoanode with a Al-O bridge for bettering the PEC performance of BiVO_(4).The Al-O bridge served as a channel to extract hole from BiVO_(4)to Ni Fe Ox,thus boosting charge carriers separation and preventing BiVO_(4) from photo-corrosion.The Al-O bridging photoanode(NiFeO_(x)/Al_(2)O_(3)/BiVO_(4))demonstrated a high photocurrent density of 5.87 m A/cm^(2)at 1.23 V vs.RHE and long-term photostability in comparison to Ni Fe Ox/BiVO_(4)photoanode.This study proposes a unique technique to boost charge carriers separation between BiVO_(4) and OECs for high-efficiency solar-driven PEC water splitting.展开更多
CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport e...CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport efficiency of photogenerated carriers.To address the above issues,a cost-effective ternary Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode was designed.Firstly,a thin Cu:NiO_(X)film was inserted between CuBi_(2)O_(4)and FTO conducting substrate as a hole-selective layer,which promotes the transmission of photogenerated holes to the FTO substrate effectively.Furthermore,the modification of CuO film on the CuBi_(2)O_(4)electrode not only increases the absorption of sunlight and generates more photogenerated carriers,but also constitutes a heterojunction with CuBi_(2)O_(4),creating a built-in electric field,which facilitates the separation of electrons and holes,and accelerates the electrons transfer to electrode–electrolyte interface.The fabricated Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode exhibits a surprisingly high photocurrent density of−1.51 mA·cm^(−2)at 0.4 V versus RHE,which is 2.6 times that of the pristine CuBi_(2)O_(4)photocathode.The improved PEC performance is attributed to the synergy effect of the Cu:NiO_(X)hole-selective layer and the CuBi_(2)O_(4)/CuO heterojunction.Moreover,the combination with the BiVO_(4)/CoS,an unbiased overall water splitting was achieved,which has a photocurrent of 0.193 mA·cm^(−2).展开更多
Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high pr...Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high production costs and energy consumption.The key is to develop highly efficient electrochemical water splitting catalysts.In recent years,the preparation of electrocatalysts via plasma treatment has gained recognition for its rapid,eco-friendly,and controllable properties,especially in the optimization of nano-microstructure.This review comprehensively summarizes the impact of plasma treatment on the nano-microstructure of water electrolysis catalysts,encompassing dispersion enhancement,morphology modulation,surface functionalization,defect construction,and element doping.These impacts on the nano-microstructure increase the surface area,modify the pore structure,introduce active sites,and regulate the electronic environment,thereby promoting the water splitting performance of electrocatalysts.Finally,the remaining challenges and potential opportunities are discussed for the future development of plasma treatment.This review would be a valuable reference for plasmaassisted electrocatalyst synthesis and mechanism understanding in plasma impact on nano-microstructure.展开更多
The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were...The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework(NiCo-MOF)as source of nickel and cobalt.Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO_(3).The prepared SrTiO_(3)loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting,achieving an apparent quantum yield of 11.9%at 350±10 nm.Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni,reducing the free energy of H adsorption.The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability.This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.展开更多
Conventional flat-plate photovoltaic-thermal(PV-T)collectors generate electricity and heat simultaneously;however,the outlet temperature of the latter is typically below 60℃,limiting their widespread application.The ...Conventional flat-plate photovoltaic-thermal(PV-T)collectors generate electricity and heat simultaneously;however,the outlet temperature of the latter is typically below 60℃,limiting their widespread application.The use of optical concentration can enable higher-temperature heat to be generated,but this can also lead to a rise in the operating temperature of the PV cells in the collector and,in turn,to a deterioration in their electrical performance.To overcome this challenge,an optical spectral-splitting filter that absorbs the infrared and transmits the visible portion of the solar spectrum can be used,such that wavelengths below the bandgap are sent to the cells for electricity generation,while those above it are sent to a thermally decoupled absorber for the generation of heat at a temperature that is considerably higher than that of the cells.In this study,a triangular primary PV-T channel,wherein the primary heat transfer fluid(water)flows,is integrated into a parabolic trough concentrator of geometrical concentration ratio~10,while a secondary liquid filter(water,AgSiO_(2)-eg or Therminol-66)is introduced for spectral splitting.Optical,electrical and thermal-fluid(sub-)models are developed and coupled to study the performance of this collector.Each sub-model is individually checked against results taken from the literature with maximum deviations under 10%.Subsequently,the optical and electrical models are coupled with a 3-D thermal-fluid CFD model(using COMSOL Multiphysics 6.1)to predict the electrical and thermal performance of the collector.Results show that when water is used as the optical filter,the maximum overall thermal(filter channel plus primary channel)and electrical efficiencies of the collector reach~45%and 15%,respectively.A comparison between water,AgSiO_(2)-eg and Therminol-66 reveals that AgSiO_(2)-eg improves the thermal efficiency of the filter channel by~25%(absolute)compared to Therminol-66 and water,however,this improvement–which arises from the thermal performance of the filter–comes at an expense of a~5%electrical efficiency loss.展开更多
基金Supported by the National Natural Science Foundation of China(No.52273056)the Science and Technology Development Program of Jilin Province,China(No.YDZJ202501ZYTS305)。
文摘Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.
基金the National Natural Science Foundation of China(Nos.22202126,52273186,51873100,and 62105194)San Qin Scholars Innovation Teams in Shaanxi Province,China,International Joint Research Center of Shaanxi Province for Photoelectric Materials Science,and International Science and Technology Cooperation Project of Shaanxi Province,China(No.2021KW-20).
文摘The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow charge transfer dynamics and severe charge recombination at the interface.Herein,a novel“killing two birds with one stone”approach was discovered by employing CoPi as an interface mediator,which shifts its charge transfer behavior from conventional hole storage or passivation to hole transporter.The optimized BiVO_(4)/CoPi/FeOOH photoanode achieves a noteworthy photocurrent density of 5.4 mA/cm^(2) and exhibits long term stability(13 h).The dynamic analysis and electrochemical characterization reveal that CoPi can rapidly and directly transfer more photogenerated holes to the surface of OEC in comparison to traditional slow holes transfer behavior,resulting in highly efficient interface charge separation.Interestingly,the strong interfacial interactions can also be extended to OEC/electrolyte interface,specifically by promoting the surface reaction dynamics.Moreover,this innovative approach of altering behavior of CoPi can also be utilized to design other photoanodes,like BiVO_(4)/CoPi/NiOOH,aimed at efficient PEC water splitting.This finding affords a smart strategy to develop highly efficient and stable photoelectrodes for water splitting.
基金Supported by the National Natural Science Foundation of China(Grant No.11801121)the Natural Science Foundation of Heilongjiang Province(Grant No.QC2018006)the Fundamental Research Fundation for Universities of Heilongjiang Province(Grant No.LGYC2018JC002).
文摘The aim of this article is to study the structures of arbitrary split δ-Jordan Lie triple systems, which are a generalization of split Lie triple systems. By developing techniques of connections of roots for this kind of triple systems, we show that any of such δ-Jordan Lie triple systems T with a symmetric root system is of the form T=U+∑[α]∈■1/~I[α] with U a subspace of T0 and any I[α] a well described ideal of T, satisfying{I[α],T,I[β]}={I[α],I[β],T}={T,I[α],I[β]}=0 if [α]≠[β] .
基金support from the Czech Science Foundation,project EXPRO,No 19-27454Xsupport by the European Union under the REFRESH—Research Excellence For Region Sustainability and High-tech Industries project number CZ.10.03.01/00/22_003/0000048 via the Operational Programme Just Transition from the Ministry of the Environment of the Czech Republic+1 种基金Horizon Europe project EIC Pathfinder Open 2023,“GlaS-A-Fuels”(No.101130717)supported from ERDF/ESF,project TECHSCALE No.CZ.02.01.01/00/22_008/0004587).
文摘Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.
基金National Programs for NanoKey Project(2022YFA1504002)National Natural Science Foundation of China(22078233)。
文摘This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.
基金supported by the Natural Science Fund of China(31771724)the Key Research and Development Project of Shaanxi Province(2024NC-ZDCYL-01-10).
文摘The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use efficiency and enhancing crop stress resistance.Nevertheless,the precise interaction between soil warming(SW)and SN remains unclear.In order to ascertain the impact of SW on maize growth and whether SN can improve the tolerance of maize to SW,a two-year field experiment was conducted(2022-2023).The aim was to examine the influence of two SW ranges(MT,warming 1.40℃;HT,warming 2.75℃)and two nitrogen application methods(N1,one-time basal application of nitrogen fertilizer;N2,one third of base nitrogen fertilizer+two thirds of jointing stage supplemental nitrogen fertilizer)on maize root growth,photosynthetic characteristics,nitrogen use efficiency,and yield.The results demonstrated that SW impeded root growth and precipitated the premature aging of maize leaves following anthesis,particularly in the HT,which led to a notable reduction in maize yield.In comparison to N1,SN has been shown to increase root length density by 8.54%,root bleeding rate by 8.57%,and enhance root distribution ratio in the middle soil layers(20-60 cm).The interaction between SW and SN had a notable impact on maize growth and yield.The SN improved the absorption and utilization efficiency of nitrogen by promoting root development and downward canopy growth,thus improving the tolerance of maize to SW at the later stage of growth.In particular,the N2HT resulted in a 14.51%increase in the photosynthetic rate,a 18.58%increase in nitrogen absorption efficiency,and a 18.32%increase in maize yield compared with N1HT.It can be posited that the SN represents a viable nitrogen management measure with the potential to enhance maize tolerance to soil high-temperature stress.
基金support by National Key Research and Development Program of China(2022YFB3803502)National Natural Science Foundation of China(52103076)+5 种基金Science and Technology Commission of Shanghai Municipality(23ZR1400300)special fund of Beijing Key Laboratory of Indoor Air Quality Evaluat ion and Control(NO.BZ0344KF21-02)State Key Laboratory of Electrical Insulation and Power Equipment(EIPE22203)JLF is a member of LSRE-LCM–Laboratory of Separation and Reaction Engineering-Laboratory of Catalysis and Materials,supported by national funds through FCT/MCTES(PIDDAC):LSRE-LCM,UIDB/50020/2020(DOI:10.54499/UIDB/50020/2020)UIDP/50020/2020(DOI:10.54499/UIDP/50020/2020)ALiCE,LA/P/0045/2020(DOI:10.54499/LA/P/0045/2020).
文摘Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.
基金sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
基金supported by the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2021L574)the Guizhou Provincial Science and Technology Foundation([2024]ZK General 425 and 438)+1 种基金the National Natural Science Foundation of China(22309033)the Academic Young Talent Foundation of Guizhou Normal University([2022]B05 and B06)。
文摘The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplored challenge of substantial electrochemical overpotential,surface reconstruction has emerged as a necessary strategy.Focusing on key aspects such as Janus structures,overflow effects,the d-band center displacement hypothesis,and interface coupling related to electrochemical reactions is essential for water electrolysis.Emerging as frontrunners among next-generation electrocatalysts,Mott-Schottky(M-S)catalysts feature a heterojunction formed between a metal and a semiconductor,offering customizable and predictable interfacial synergy.This review offers an in-depth examination of the processes driving the hydrogen and oxygen evolution reactions(HER and OER),highlighting the benefits of employing nanoscale transition metal nitrides,carbides,oxides,and phosphides in M-S heterointerface catalysts.Furthermore,the challenges,limitations,and future prospects of employing M-S heterostructured catalysts for water splitting are thoroughly discussed.
基金the National Key R&D Program of China(2021YFB4000300)National Natural Science Foundation of China(21822803,22408030,22072009,91534205,51072239)National Program on Key Basic Research Project(973 Program,2012CB720303).
文摘The unavailability of high-performance and cost-effective electrocatalysts has impeded the large-scale deployment of alkaline water electrolyzers.Professor Zidong Wei's group has focused on resolving critical challenges in industrial alkaline electrolysis,particularly elucidating hydrogen and oxygen evolution reaction(HER/OER)mechanisms while addressing the persistent activity-stability trade-off.This review summarizes their decade-long progress in developing advanced electrodes,analyzing the origins of sluggish alkaline HER kinetics and OER stability limitations.Professor Wei proposes a unifying"12345 Principle"as an optimization framework.For HER electrocatalysts,they have identified that metal/metal oxide interfaces create synergistic"chimney effect"and"local electric field enhancement effect",enhancing selective intermediate adsorption,interfacial water enrichment/reorientation,and mass transport under industrial high-polarization conditions.Regarding OER,innovative strategies,including dual-ligand synergistic modulation,lattice oxygen suppression,and self-repairing surface construction,are demonstrated to balance oxygen species adsorption,optimize spin states,and dynamically reinforce metal-oxygen bonds for concurrent activity-stability enhancement.The review concludes by addressing remaining challenges in long-term industrial durability and suggesting future research priorities.
基金financially supported by the National Natural Science Foundation of China(No.22279030)the Natural Science Fund for Distinguished Young Scholars of Heilongjiang Province(No.JQ2024B003)+1 种基金Fundamental Research Funds for the Undergraduate Universities of Heilongjiang Province(No.2024-KYYWF-0122)the Project of Key Laboratory of Superlight Materials and Surface Technology of Harbin Engineering University
文摘Transition metal phosphides(TMPs),with tunable electronic structures and diverse compositions,are promising candidates for electrocatalytic water splitting.However,their unsatisfactory electrical conductivity and tendency to aggregate during reactions result in structural instability,ultimately hindering further improvement of their electrocatalytic performance.To address these issues,a bamboo-leaf-like FeCoP/MXene heterojunction was synthesized by hydrothermal and thermal treatments,utilizing highly conductive MXene as the substrate.Density functional theory(DFT)calculations and experimental characterization reveal that strong Ti-O-Co/Fe covalent bond are formed between MXene and FeCoP through hybridization of O 2p and Co/Fe 3d orbitals,which enhance the structural stability of the interface and facilitate the effective anchoring of FeCoP on the MXene surface.Consequently,the structural stability and electrical conductivity of the catalyst are improved simultaneously.Additionally,interfacial charge redistribution optimizes the Gibbs free energy of hydrogen adsorption at the Co,Fe,and Ti sites while promoting the adsorption and activation of water molecules.These factors interact synergistically,leading to enhanced bi-functional electrocatalytic performance for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In a FeCoP/MXene(+‖-)two-electrode system,the catalyst achieves a current density of 10 mA cm^(-2)at a potential of 1.5 V,which is superior to the RuO_(2)(+)‖Pt/C(-)system.The assembled water splitting device exhibits long-term stability for up to 100 h at a current density of 100 mA cm^(-2).Furthermore,an anion exchange membrane water electrolyzer(AEMWE)equipped with FeCoP/MXene as both anode and cathode achieves an industrial-grade current density of 500 mA cm^(-2)at 1.83 V.These results highlight the critical role of interfacial engineering in enhancing the electrocatalytic performance of TMPs for water splitting and provide valuable insights for the design of novel bifunctional TMP catalysts.
基金financially supported by the National Natural Science Foundation of China(No.52173277)the Fundamental Research Funds for the Central Universities of Chang’an University(No.300102299304)+1 种基金the Innovative Research Team for Science and Technology of Shaanxi Province(No.2022TD-04)the open program of Key Laboratories of Fine Chemicals and Surfactants in Sichuan Provincial Universities(No.2023JXZ03)。
文摘Developing BiVO_(4)photoanode with efficient carrier transfer and fast water oxidation kinetics is the permanent pursuit to achieve the state-of-art solar-driven photoelectrochemical(PEC)water splitting.The capacity to increase the PEC activity of BiVO_(4)by loading oxygen evolution co-catalysts(OECs)has been proven,however it suffers from sluggish charge carriers dynamics brought on by the complicated interface between BiVO_(4)and OECs as well as poor long-term durability.Herein,we connected OECs(NiFeOx)and photoanode with a Al-O bridge for bettering the PEC performance of BiVO_(4).The Al-O bridge served as a channel to extract hole from BiVO_(4)to Ni Fe Ox,thus boosting charge carriers separation and preventing BiVO_(4) from photo-corrosion.The Al-O bridging photoanode(NiFeO_(x)/Al_(2)O_(3)/BiVO_(4))demonstrated a high photocurrent density of 5.87 m A/cm^(2)at 1.23 V vs.RHE and long-term photostability in comparison to Ni Fe Ox/BiVO_(4)photoanode.This study proposes a unique technique to boost charge carriers separation between BiVO_(4) and OECs for high-efficiency solar-driven PEC water splitting.
基金supported by the National Natural Science Foundation of China(No.61804039)the University Natural Sciences Research Project of Anhui Province(No.2022AH010096)+1 种基金the Talent Research Fund of Hefei University(No.20RC35)the Natural Science Foundation of Anhui Higher Education Institution of China(No.2023AH040160).
文摘CuBi_(2)O_(4)is identified as a promising photocathode in photoelectrochemical(PEC)water splitting systems.However,the PEC performance of CuBi_(2)O_(4)is far from expected due to the limited separation and transport efficiency of photogenerated carriers.To address the above issues,a cost-effective ternary Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode was designed.Firstly,a thin Cu:NiO_(X)film was inserted between CuBi_(2)O_(4)and FTO conducting substrate as a hole-selective layer,which promotes the transmission of photogenerated holes to the FTO substrate effectively.Furthermore,the modification of CuO film on the CuBi_(2)O_(4)electrode not only increases the absorption of sunlight and generates more photogenerated carriers,but also constitutes a heterojunction with CuBi_(2)O_(4),creating a built-in electric field,which facilitates the separation of electrons and holes,and accelerates the electrons transfer to electrode–electrolyte interface.The fabricated Cu:NiO_(X)/CuBi_(2)O_(4)/CuO composite photocathode exhibits a surprisingly high photocurrent density of−1.51 mA·cm^(−2)at 0.4 V versus RHE,which is 2.6 times that of the pristine CuBi_(2)O_(4)photocathode.The improved PEC performance is attributed to the synergy effect of the Cu:NiO_(X)hole-selective layer and the CuBi_(2)O_(4)/CuO heterojunction.Moreover,the combination with the BiVO_(4)/CoS,an unbiased overall water splitting was achieved,which has a photocurrent of 0.193 mA·cm^(−2).
基金supported by the National Key Research and Development Program of China(2021YFB4000405).
文摘Hydrogen is a critical renewable energy source in the energy transition.However,water electrolysis,which is the primary technique for achieving large-scale and low-carbon hydrogen production,still suffers from high production costs and energy consumption.The key is to develop highly efficient electrochemical water splitting catalysts.In recent years,the preparation of electrocatalysts via plasma treatment has gained recognition for its rapid,eco-friendly,and controllable properties,especially in the optimization of nano-microstructure.This review comprehensively summarizes the impact of plasma treatment on the nano-microstructure of water electrolysis catalysts,encompassing dispersion enhancement,morphology modulation,surface functionalization,defect construction,and element doping.These impacts on the nano-microstructure increase the surface area,modify the pore structure,introduce active sites,and regulate the electronic environment,thereby promoting the water splitting performance of electrocatalysts.Finally,the remaining challenges and potential opportunities are discussed for the future development of plasma treatment.This review would be a valuable reference for plasmaassisted electrocatalyst synthesis and mechanism understanding in plasma impact on nano-microstructure.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(No.52488201)the National Natural Science Foundation of China(No.52376209)+1 种基金the China Postdoctoral Science Foundation(Nos.2020T130503 and 2020M673386)China Fundamental Research Funds for the Central Universities.
文摘The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting.In this study,NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework(NiCo-MOF)as source of nickel and cobalt.Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO_(3).The prepared SrTiO_(3)loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting,achieving an apparent quantum yield of 11.9%at 350±10 nm.Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni,reducing the free energy of H adsorption.The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability.This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.
基金supported by the UK Engineering and Physical Sciences Research Council(EPSRC)(Grant No.EP/R045518/1)the Royal Society under an International Collaboration Award 2020(Grant No.ICA\R1\201302)+2 种基金UK company Solar Flow Ltd.This work has also been funded by the European Union under the SPECTRUM project(Grant Agreement No.101172891)support for this research was provided by Tecnologico de Monterrey Challenge-Based Research Funding Programsupporting this publication can be obtained on request from cep-laboratory@imperial.ac.uk.For the purpose of Open Access,the authors have applied a CC BY public copyright license to any Author Accepted Manuscript version arising from this submission.
文摘Conventional flat-plate photovoltaic-thermal(PV-T)collectors generate electricity and heat simultaneously;however,the outlet temperature of the latter is typically below 60℃,limiting their widespread application.The use of optical concentration can enable higher-temperature heat to be generated,but this can also lead to a rise in the operating temperature of the PV cells in the collector and,in turn,to a deterioration in their electrical performance.To overcome this challenge,an optical spectral-splitting filter that absorbs the infrared and transmits the visible portion of the solar spectrum can be used,such that wavelengths below the bandgap are sent to the cells for electricity generation,while those above it are sent to a thermally decoupled absorber for the generation of heat at a temperature that is considerably higher than that of the cells.In this study,a triangular primary PV-T channel,wherein the primary heat transfer fluid(water)flows,is integrated into a parabolic trough concentrator of geometrical concentration ratio~10,while a secondary liquid filter(water,AgSiO_(2)-eg or Therminol-66)is introduced for spectral splitting.Optical,electrical and thermal-fluid(sub-)models are developed and coupled to study the performance of this collector.Each sub-model is individually checked against results taken from the literature with maximum deviations under 10%.Subsequently,the optical and electrical models are coupled with a 3-D thermal-fluid CFD model(using COMSOL Multiphysics 6.1)to predict the electrical and thermal performance of the collector.Results show that when water is used as the optical filter,the maximum overall thermal(filter channel plus primary channel)and electrical efficiencies of the collector reach~45%and 15%,respectively.A comparison between water,AgSiO_(2)-eg and Therminol-66 reveals that AgSiO_(2)-eg improves the thermal efficiency of the filter channel by~25%(absolute)compared to Therminol-66 and water,however,this improvement–which arises from the thermal performance of the filter–comes at an expense of a~5%electrical efficiency loss.
