A series of CoS_(2-x)Se_(x)(x=0.05,0.1,0.2,0.3,and 2)composite catalysts were synthesized on carbon fiber paper via the hydrothermal method with Se doping.By precisely controlling the reaction temperature and Se dopin...A series of CoS_(2-x)Se_(x)(x=0.05,0.1,0.2,0.3,and 2)composite catalysts were synthesized on carbon fiber paper via the hydrothermal method with Se doping.By precisely controlling the reaction temperature and Se doping level,a hollow spherical catalyst structure composed of CoSSe was successfully synthesized,which exhibited exceptional activity for hydrogen evolution in acidic solutions.The influences of Se doping on the microstructure and catalytic mechanism of hydrogen evolution reaction(HER)of these composites were systematically investigated.The experimental results reveal that the hollow spherical sample displays an overpotential value of 143 mV along with a Tafel slope value of 69.8 mV·dec^(-1)at a current density of 10 mA·cm^(-2)in an acid aqueous solution.Furthermore,it demonstrates remarkable cycling stability after undergoing 3000 cycles.The comprehensive analysis indicates that Se doping optimizes the electronic structure and enhances conductivity,meanwhile the unique hollow spherical architecture increases active sites for HER and significantly improves overall electrocatalytic performance.展开更多
Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to thei...Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.展开更多
The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts ...The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts in recent years.The hydrogen and oxygen evolution reactions during alkaline water electrolysis and the oxygen electro-reduction taking place in fuel cells are of particular importance.There is no universal theory explaining all the details of the AM cation effect in electrocatalysis.For example,it remains unclear how“spectator”AM-cations can change the kinetics of electrocatalytic reactions often more significantly than the modifications of the elec-trode structure and composition.This situation originates partly from a lack of systematic experimental and theoretical studies of this phenomenon.The present work exploits impedance spectroscopy to investigate the influence of the AM cations on the mechanism of the hydrogen evolution reaction at Pt microelectrodes.The activity follows the trend:Li^(+)≥Na^(+)≥K^(+)≥Cs^(+),where the highest activity corresponds to 0.1 M LiOH electrolytes at low overpotentials.We demonstrate that the nature of the AM cations also changes the relative contribution of the Volmer–Heyrovsky and Volmer–Tafel mechanisms to the overall reaction,with the former being more important for LiOH electrolytes.Our density functional theory-based thermodynamics and molecular dynamics calculations support these findings.展开更多
Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a...Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a series of Schreibersite-type intermetallic compounds,particularly Mo_(2)Fe_(0.8)Ru_(0.2)P,are synthesized through high-temperature solid-phase synthesis.Experimental results demonstrate that the integration of Ru significantly improves the kinetics of proton adsorption and desorption during the hydrogen evolution reaction(HER).Additionally,density functional theory(DFT)calculations and X-ray absorption near edge structure(XANES)analyses effectively corroborate the pronounced d-orbital hybridization of Fe within the structure,which facilitates the transfer of hydroxide ions and the maintenance of material durability during alkaline HER processes.Remarkably,Mo_(2)Fe_(0.8)Ru_(0.2)P exhibits superior alkaline HER activity,characterized by an overpotential of merely 48 mV at a current density of 10 mA cm^(-2).After prolonged operation of 1000 h at high current densities(1.1 A cm^(-2)),the activity decline remains minimal,under 4%(with overpotential increasing from 258 mV to 268 mV).These results demonstrate the potential of strategically combining metallic elements to design high-performance industrial-grade electrocatalysts.展开更多
Transition metal carbides,known as MXenes,particularly Ti_(3)C_(2)T_(x),have been extensively explored as promising materials for electrochemical reactions.However,transition metal carbonitride MXenes with high nitrog...Transition metal carbides,known as MXenes,particularly Ti_(3)C_(2)T_(x),have been extensively explored as promising materials for electrochemical reactions.However,transition metal carbonitride MXenes with high nitrogen content for electrochemical reactions are rarely reported.In this work,transition metal carbonitride MXenes incorporated with Pt-based electrocatalysts,ranging from single atoms to sub-nanometer dimensions,are explored for hydrogen evolution reaction(HER).The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared to the single-atom-incorporated MXene and commercial Pt/C catalyst in both acidic and alkaline electrolytes.The optimized sample shows low overpotentials of 28,65,and 154 mV at a current densities of 10,100,and 500 m A cm^(-2),a small Tafel slope of 29 m V dec^(-1),a high mass activity of 1203 mA mgPt^(-1)and an excellent turnover frequency of 6.1 s^(-1)in the acidic electrolyte.Density functional theory calculations indicate that this high performance can be attributed to the enhanced active sites,increased surface functional groups,faster charge transfer dynamics,and stronger electronic interaction between Pt and MXene,resulting in optimized hydrogen absorption/desorption toward better HER.This work demonstrates that MXenes with a high content of nitrogen may be promising candidates for various catalytic reactions by incorporating single atoms or clusters.展开更多
High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of...High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of phosphides.Herein,electrospinning and in situ phosphating were employed to prepare three-dimensional(3D)networks of self-supporting HEMP nanofibers with varying degrees of phosphate content.Comprehensive characterizations via X-ray diffraction and X-ray photoelectron spectroscopy,as well as density functional theory calculations,demonstrate that the introduction of phosphorus(P)atoms to HEMP carbon nanofibers mediates their electronic structure,leads to lattice expansion,which in turn enhances their catalytic performance in the hydrogen evolution reaction(HER).Moreover,the formation of metal-P bonds weakens metal-metal interaction and decreases the free energy of hydrogen adsorption,contributing to the exceptional activity observed in the HEMP catalyst.Electrochemical measurements demonstrate that the HEMP-0.75 catalyst with an ultralow loading of 1.22 wt%ruthenium(Ru)exhibits the highest HER catalytic activity and stability in a 1 M KOH electrolyte,achieving a minimal overpotential of 26 mV at a current density of 10 mA·cm^(-2)and Tafel slope of 50.9 mV·dec^(-1).展开更多
Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this s...Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.展开更多
The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their pot...The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications.However,the unsatisfied cyclic stability and electrochemical activity limit their further application.In this work,nickel-molybdenum(Ni-Mo)alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition,thermal annealing,and electrochemical activation.Owing to the synergistic interaction of molybdenum trinickelide(Ni_(3)Mo)and molybdenum dioxide(MoO_(2))in Ni-Mo alloy,the catalyst display superior overall electrochemical properties.A low overpotential of 86 mV at 10 mA/cm^(2)and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H_(2)SO_(4)solution can be achieved.Notably,remarkable stability with negligible performance degradation even after 100 h could be maintained.This work presents a novel and effective strategy for the design and fabrication of high-performance,non-precious metal electrocatalysts for acidic water electrolysis.展开更多
Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional th...Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.展开更多
An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-...An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-doped CoP electrocatalysts in the alkaline hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The introduction of Br modulates the electronic structure of the Co site,endowing Br-CoP with a more metallic character.In addition,P ion leaching promotes the in situ reconstruction of Br-CoOOH,which is the real active site for the OER reaction.Meanwhile,the HER situation is different.On the basis of P ion leaching,the leaching of Br ions promotes the formation of CoP-Co(OH)_(2) active species.In addition,Br doping enhances the adsorption of^(*)H,showing excellent H adsorption free energy,thereby greatly improving the HER activity.Simultaneously,it also enhances the adsorption of OOH^(*),effectively facilitating the occurrence of OER reactions.Br-CoP only needs 261 and 76 mV overpotential to drive the current density of 20 mA cm^(-2) and 10 mA^(-2),which can be maintained unchanged for 100 h.This study provides new insights into anion doping strategies and catalyst reconstruction mechanisms.展开更多
Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru ...Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.展开更多
Constructing clus ter heterostructures with strongly coupled interfaces is of great importance to accelerating the catalytic reactions that involve multiple intermediates.Herein,a strongly coupled cluster heterostruct...Constructing clus ter heterostructures with strongly coupled interfaces is of great importance to accelerating the catalytic reactions that involve multiple intermediates.Herein,a strongly coupled cluster heterostructure composed of platinum and molybdenum carbide(Pt@Mo_(2)C)derived from polyoxometalate clusters is designed to achieve excellent alkaline hydrogen evolution reaction.The Pt@Mo_(2)C cluster exhibits strong electronic interactions between Pt and Mo_(2)C,working together to facilitate the H_(2)O dissociation by concurrently binding intermediates(Pt-H*and Mo-OH*),thus accelerating the kinetics of the rate-determining Volmer step.Theoptimized Pt@Mo_(2)C exhibits a high mass activity of12.1 A·mgpt^(-1),19.2 times higher than that of 20%Pt/C in alkaline media.Moreover,it can be stabilized at a current density of 100 mA·cm^(-2)for more than 200 h.This work demonstrated the superiority of the cluster heterostructures and co-catalytic effect towards the development of highly efficient electrocatalysts.展开更多
The structural modulation of metal-based heterostructure plays a vital role in achieving enhanced performances for highly efficient electrocatalysis.Here we design submonolayered Ru-modified Pd mesoporous nanosheets(P...The structural modulation of metal-based heterostructure plays a vital role in achieving enhanced performances for highly efficient electrocatalysis.Here we design submonolayered Ru-modified Pd mesoporous nanosheets(Pd-Ru MNSs)with the exposure of both Pd and Ru active sites as well as the high atomic utilization of two-dimensional structure.The obtained Pd-Ru MNSs can act as a highly efficient multifunctional catalyst for hydrogen evolution reaction(HER)and alcohol oxidation reactions including ethylene glycol oxidation(EGOR)and ethanol oxidation(EOR),offering new opportunities towards the alcohol oxidation assisted hydrogen production.Specifically,Pd-Ru MNSs demonstrate excellent HER performance in alkaline electrolyte,requiring an overpotential of only 16mV to reach 10mAcm^(−2),significantly outperforming Pd mesoporous nanosheets and commercial catalysts.Density functional theory calculations reveal that the Ru sites in Pd-Ru MNSs could facilitate the water adsorption,accelerate the water dissociation,and optimize the hydrogen desorption,leading to the superior HER activity.Pd-Ru MNSs also exhibit high mass activities of 11.19 A mg^(−1)Pd for EGOR and 8.84 A mg^(−1)Pd for EOR,which is 7.8 and 9.6 times than that of commercial Pd/C,respectively.The EGOR reaction pathway over Pd-Ru MNSs was further investigated by using in situ Fourier-transform infrared spectroscopy.展开更多
As a clean energy source,hydrogen plays a critical role in the global mission to achieve carbon neutrality.Among varied hydrogen production techniques,water electrolysis driven by clean energy,such as solar or wind en...As a clean energy source,hydrogen plays a critical role in the global mission to achieve carbon neutrality.Among varied hydrogen production techniques,water electrolysis driven by clean energy,such as solar or wind energy,is the most promising and viable option,with the advantages of celerity,high efficiency,cleanliness,and sustainability.However,this process necessitates a highly active and durable hydrogen evolution reaction(HER)catalyst to enhance the overall reaction efficiency.This article thoroughly reviews the recent development of electrocatalysts exhibiting high-performance HER.In particular,a comprehensive look at noble metals platinum(Pt),ruthenium(Ru),iridium(Ir),and non-noble metals,including sulfides,carbides,nitrides and phosphides is taken.Synthesis strategies,methods for enhancing performance,and the correlation between structure,composition,and catalytic performance are discussed.We also pay particular attention to density functional theory(DFT)calculations to reveal the mechanisms behind the improvement of HER performance.Finally,the critical challenges associated with electrochemical water splitting and propose coping strategies are presented.展开更多
Exploring platinum single-atom electrocatalysts(SACs)is of great significance for effectively catalyzing the hydrogen evolution reaction in order to maximize the utilization of metal atoms.Herein,ruthenium clusters wi...Exploring platinum single-atom electrocatalysts(SACs)is of great significance for effectively catalyzing the hydrogen evolution reaction in order to maximize the utilization of metal atoms.Herein,ruthenium clusters with several atoms(Rux)supported on nitrogen-doped,cost-efficient Black Pearls 2000(Ru_(x)NBP),were synthesized as initial materials via a simple hydrothermal method.Then,[PtCl_(4)]^(2–)ion was reductively deposited on RuxNBP to obtain a Pt SAC(Pt1/RuxNBP).Electrochemical measurements demonstrate the excellent HER performance of Pt_(1)/Ru_(x)NBP with a 5.7-fold increase in mass activity compared to the commercial Pt/C at 20 mV.Moreover,the cell voltage of the proton exchange membrane electrolyzer with Pt_(1)/Ru_(x)NBP is 20 mV lower compared to that with commercial Pt/C at 1.0 A cm^(−2).Physical characterization and density functional theory calculations revealed that the preserved Pt–Cl bond of[PtCl_(4)]^(2–)and the RuxNBP support co-regulate the 5d state of isolated Pt atoms and enhance the catalytic HER capacity of Pt1/RuxNBP.展开更多
Electrochemical water splitting is a highly promising approach for producing carbon-neutral hydrogen.The development of efficient electrocatalysts for the hydrogen evolution reaction(HER)is crucial to lowering the ene...Electrochemical water splitting is a highly promising approach for producing carbon-neutral hydrogen.The development of efficient electrocatalysts for the hydrogen evolution reaction(HER)is crucial to lowering the energy barriers and enhancing hydrogen production.This drives the search for HER electrocatalysts that are not only cost-effective and abundant but also exhibit high activity and long-term stability.In this review,we provide an in-depth analysis of recent progress in the application of ruthenium phosphides as HER electrocatalysts,offering key insights into their design and performance.Meanwhile,we explore various strategies to enhance their catalytic efficiency,such as increasing the availability of active sites and optimizing their electronic structure.Finally,we outline the key challenges and future directions for developing the next generation of ruthenium phosphide-based HER electrocatalysts.展开更多
High-performance catalyst is significant for the sustainable hydrogen(H_(2))production by electrocatalytic water splitting.Optimizing porous structure and active groups of substrate can promote the interaction of subs...High-performance catalyst is significant for the sustainable hydrogen(H_(2))production by electrocatalytic water splitting.Optimizing porous structure and active groups of substrate can promote the interaction of substrate and active metal particles,enabling excellent catalytic properties and stability.Herein,the optimization strategy of delignification and 2,2,6,6-tetramethylpyperidine-1-oxyl(TEMPO)oxidization was developed to modify the porous structure and active groups of wood substrate,and Ru doped Co/CO_(2)P(Ru-Co/CO_(2)P)nanoparticles were encapsulated into the optimized wood carbon substrate(Ru-Co/CO_(2)P@TDCW)for the efficient pH-universal hydrogen evolution reaction(HER).The nanopore and carboxyl groups were produced by delignification and TEMPO oxidation,which accelerated the dispersion and deposition of Ru-Co/CO_(2)P nanoparticles.The RuCo alloy and RuCoP nanoparticles were produced with the doping of Ru,and more Ru-Co/CO_(2)P nanoparticles were anchored by the delignified and TEMPO oxidized wood carbon(TDCW).As anticipated,the Ru-Co/CO_(2)P@TDCW catalyst exhibited excellent pH-universal HER activity,and only 16.6,93,and 43 mV of overpotentials were required to deliver the current density of 50 mA cm^(-2)in alkaline,neutral,and acidic electrolytes,outperforming the noble Pt/C/TDCW catalyst significantly.In addition,Ru-Co/CO_(2)P@TDCW catalyst presented excellent stability for more than 600 h working at 100 mA cm^(-2)in alkaline solution(1.0 M KOH).Density function theory(DFT)results revealed that energy barriers for the dissociation of H_(2)O and the formation of H_(2)were decreased by the doping of Ru,and the conductivity and efficiency of electron migration were also enhanced.This work demonstrated a strategy to optimize the structure and properties of wood carbon substrate,providing a promising strategy to synthesize high-efficiency catalyst for H_(2)production.展开更多
Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the stron...Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the strong adsorption of Ru-OH intermediates(Ru-OHad)blocks the active site,leading to unsatisfactory HER performance.In this study,we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP-CoP heterostructure-anchored Ru single-atom site catalyst(Ru-FeP-CoP/NPC).The obtained catalyst shows a low overpotential(28 mV at 10 mA cm^(-2))and a high mass activity(9.29 A mg^(-1) at 100 mV),surpassing the performance of commercial Pt/C by a factor of 46.Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH-blockages,accelerating water dissociation and facilitating hydrogen adsorption/desorption,thus enhancing HER activity.This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.展开更多
Correction to:Nano-Micro Letters(2025)17:123 https://doi.org/10.1007/s40820-025-01654-y Following publication of the original article[1],the authors reported that Dr.Mohamed Bououdina’s affiliation needed to be corre...Correction to:Nano-Micro Letters(2025)17:123 https://doi.org/10.1007/s40820-025-01654-y Following publication of the original article[1],the authors reported that Dr.Mohamed Bououdina’s affiliation needed to be corrected from 1 to 2.The correct author affiliation has been provided in this Correction and the original article[1]has been corrected.展开更多
Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-prot...Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-proton transfers more complex when determining kinetics and mass transfer information.Understanding how HER competes with other electrochemical reduction reactions is crucial for both fundamental studies and system performance improvements.In this study,we employed the oxygen reduction reaction(ORR)as a model reaction to investigate HER competition on a polycrystalline-Au surface,using a rotating ring and disk electrode.It’s proved that water molecules serve as the proton source for ORR in alkaline,neutral,and even acidic electrolytes,and a 4-electron process can be achieved when the overpotential is sufficiently high.The competition from H⁺reduction becomes noticeable at the H⁺concentration higher than 2 mmol L^(–1)and intensi-fies as the H^(+)concentration increases.Based on the electrochemical results,we obtained an equivalent circuit diagram for the ORR system with competition from the H+reduction reaction,showing that these reactions occur in parallel and compete with each other.Electrochemical impedance spectroscopy measurements further confirm this argument.Additionally,we discover that the contribution of H+mass transfer to the total H^(+)reduction current is significant and comparable to the kinetic current.We believe this work will deepen our understanding of HER and its competition in electrochemical reduction systems.展开更多
基金Funded by the Breeding Project of Anhui Polytechnic University(No.2019YQQ027)the Scientific Research Foundation of Anhui Polytechnic University(No.xjky2022016)+1 种基金the Open Research Found of Anhui Key Laboratory of High-performance Non-ferrous Metal Materials(No.YSJS-2023-07)the Innovative Entrepreneurship Training Program for College Students in Anhui Province(No.S202210363391)。
文摘A series of CoS_(2-x)Se_(x)(x=0.05,0.1,0.2,0.3,and 2)composite catalysts were synthesized on carbon fiber paper via the hydrothermal method with Se doping.By precisely controlling the reaction temperature and Se doping level,a hollow spherical catalyst structure composed of CoSSe was successfully synthesized,which exhibited exceptional activity for hydrogen evolution in acidic solutions.The influences of Se doping on the microstructure and catalytic mechanism of hydrogen evolution reaction(HER)of these composites were systematically investigated.The experimental results reveal that the hollow spherical sample displays an overpotential value of 143 mV along with a Tafel slope value of 69.8 mV·dec^(-1)at a current density of 10 mA·cm^(-2)in an acid aqueous solution.Furthermore,it demonstrates remarkable cycling stability after undergoing 3000 cycles.The comprehensive analysis indicates that Se doping optimizes the electronic structure and enhances conductivity,meanwhile the unique hollow spherical architecture increases active sites for HER and significantly improves overall electrocatalytic performance.
基金financial support by the National Natural Science Foundation of China(No.52102241)Doctor of Suzhou University Scientific Research Foundation(Nos.2022BSK019,2020BS015)+2 种基金the Primary Research and Development Program of Anhui Province(No.201904a05020087)the Natural Science Research Project in Universities of Anhui Province in China(Nos.2022AH051386,KJ2021A1114)the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking Qilu University of Technology。
文摘Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
基金the German Research Foundation (DFG) under Germany's excellence strategy–EXC 2089/1–390776260, Germany's excellence cluster “e-conversion”the DFG project BA 5795/6-1+2 种基金funding from the European Union's Horizon 2020 research and innovation program under grant agreement HERMES No 952184the National Science Foundation (NSF) support through the NSF CAREER award (Grant No. CBET1941204)financial support from TUM Innovation Network for Artificial Intelligence powered Multifunctional Material Design (ARTEMIS).
文摘The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts in recent years.The hydrogen and oxygen evolution reactions during alkaline water electrolysis and the oxygen electro-reduction taking place in fuel cells are of particular importance.There is no universal theory explaining all the details of the AM cation effect in electrocatalysis.For example,it remains unclear how“spectator”AM-cations can change the kinetics of electrocatalytic reactions often more significantly than the modifications of the elec-trode structure and composition.This situation originates partly from a lack of systematic experimental and theoretical studies of this phenomenon.The present work exploits impedance spectroscopy to investigate the influence of the AM cations on the mechanism of the hydrogen evolution reaction at Pt microelectrodes.The activity follows the trend:Li^(+)≥Na^(+)≥K^(+)≥Cs^(+),where the highest activity corresponds to 0.1 M LiOH electrolytes at low overpotentials.We demonstrate that the nature of the AM cations also changes the relative contribution of the Volmer–Heyrovsky and Volmer–Tafel mechanisms to the overall reaction,with the former being more important for LiOH electrolytes.Our density functional theory-based thermodynamics and molecular dynamics calculations support these findings.
基金supported by Research Grants of the NRF(2023R1A2C2003823,RS-2024-00405818)funded by the National Research Foundation under the Ministry of Science,ICT&Future,Korea。
文摘Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a series of Schreibersite-type intermetallic compounds,particularly Mo_(2)Fe_(0.8)Ru_(0.2)P,are synthesized through high-temperature solid-phase synthesis.Experimental results demonstrate that the integration of Ru significantly improves the kinetics of proton adsorption and desorption during the hydrogen evolution reaction(HER).Additionally,density functional theory(DFT)calculations and X-ray absorption near edge structure(XANES)analyses effectively corroborate the pronounced d-orbital hybridization of Fe within the structure,which facilitates the transfer of hydroxide ions and the maintenance of material durability during alkaline HER processes.Remarkably,Mo_(2)Fe_(0.8)Ru_(0.2)P exhibits superior alkaline HER activity,characterized by an overpotential of merely 48 mV at a current density of 10 mA cm^(-2).After prolonged operation of 1000 h at high current densities(1.1 A cm^(-2)),the activity decline remains minimal,under 4%(with overpotential increasing from 258 mV to 268 mV).These results demonstrate the potential of strategically combining metallic elements to design high-performance industrial-grade electrocatalysts.
基金the final support of ARC DP220103045the startup support of KFUPMPrince Sultan University for their support。
文摘Transition metal carbides,known as MXenes,particularly Ti_(3)C_(2)T_(x),have been extensively explored as promising materials for electrochemical reactions.However,transition metal carbonitride MXenes with high nitrogen content for electrochemical reactions are rarely reported.In this work,transition metal carbonitride MXenes incorporated with Pt-based electrocatalysts,ranging from single atoms to sub-nanometer dimensions,are explored for hydrogen evolution reaction(HER).The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared to the single-atom-incorporated MXene and commercial Pt/C catalyst in both acidic and alkaline electrolytes.The optimized sample shows low overpotentials of 28,65,and 154 mV at a current densities of 10,100,and 500 m A cm^(-2),a small Tafel slope of 29 m V dec^(-1),a high mass activity of 1203 mA mgPt^(-1)and an excellent turnover frequency of 6.1 s^(-1)in the acidic electrolyte.Density functional theory calculations indicate that this high performance can be attributed to the enhanced active sites,increased surface functional groups,faster charge transfer dynamics,and stronger electronic interaction between Pt and MXene,resulting in optimized hydrogen absorption/desorption toward better HER.This work demonstrates that MXenes with a high content of nitrogen may be promising candidates for various catalytic reactions by incorporating single atoms or clusters.
基金supported by the National Natural Science Foundation of China(Nos.22103045 and 52273077)the State Key Laboratory of Bio-Fibers and Eco-Textiles,Qingdao University(Nos.ZDKT202108,RZ2000003334 and G2RC202022)support from the Australian National Fabrication Facility’s Queensland Node(No.ANFF-Q),the UQ-Yonsei International Research Project,and the JST-ERATO Yamauchi Materials Space-Tectonics Project(No.JPMJER2003).
文摘High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of phosphides.Herein,electrospinning and in situ phosphating were employed to prepare three-dimensional(3D)networks of self-supporting HEMP nanofibers with varying degrees of phosphate content.Comprehensive characterizations via X-ray diffraction and X-ray photoelectron spectroscopy,as well as density functional theory calculations,demonstrate that the introduction of phosphorus(P)atoms to HEMP carbon nanofibers mediates their electronic structure,leads to lattice expansion,which in turn enhances their catalytic performance in the hydrogen evolution reaction(HER).Moreover,the formation of metal-P bonds weakens metal-metal interaction and decreases the free energy of hydrogen adsorption,contributing to the exceptional activity observed in the HEMP catalyst.Electrochemical measurements demonstrate that the HEMP-0.75 catalyst with an ultralow loading of 1.22 wt%ruthenium(Ru)exhibits the highest HER catalytic activity and stability in a 1 M KOH electrolyte,achieving a minimal overpotential of 26 mV at a current density of 10 mA·cm^(-2)and Tafel slope of 50.9 mV·dec^(-1).
基金financially supported by the National Natural Science Foundation of China(No.5217042069)the Young Elite Scientist Sponsorship Program by China Association for Science and Technology(CAST)(No.YESS20200103)the Fundamental Research Funds for the Central Universities(No.265QZ2022004)。
文摘Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.
基金supported by the National Natural Science Foundation of China(22179138).
文摘The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications.However,the unsatisfied cyclic stability and electrochemical activity limit their further application.In this work,nickel-molybdenum(Ni-Mo)alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition,thermal annealing,and electrochemical activation.Owing to the synergistic interaction of molybdenum trinickelide(Ni_(3)Mo)and molybdenum dioxide(MoO_(2))in Ni-Mo alloy,the catalyst display superior overall electrochemical properties.A low overpotential of 86 mV at 10 mA/cm^(2)and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H_(2)SO_(4)solution can be achieved.Notably,remarkable stability with negligible performance degradation even after 100 h could be maintained.This work presents a novel and effective strategy for the design and fabrication of high-performance,non-precious metal electrocatalysts for acidic water electrolysis.
基金supported by the National Natural Science Foundation of China(Nos.22102167 and U21A20317)。
文摘Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.
基金supported by the National Natural Science Foundation of China(62404063)the Natural Science Foundation of Heilongjiang Province(YQ2022B008,LH2023A011)+1 种基金the Basic research support plan project for outstanding young teachers in undergraduate universities of Heilongjiang Province(YQJH2023160)the Basic scientific research business expense project of Heilongjiang Provincial Department of Education(2022-KYYWF-0170).
文摘An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-doped CoP electrocatalysts in the alkaline hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The introduction of Br modulates the electronic structure of the Co site,endowing Br-CoP with a more metallic character.In addition,P ion leaching promotes the in situ reconstruction of Br-CoOOH,which is the real active site for the OER reaction.Meanwhile,the HER situation is different.On the basis of P ion leaching,the leaching of Br ions promotes the formation of CoP-Co(OH)_(2) active species.In addition,Br doping enhances the adsorption of^(*)H,showing excellent H adsorption free energy,thereby greatly improving the HER activity.Simultaneously,it also enhances the adsorption of OOH^(*),effectively facilitating the occurrence of OER reactions.Br-CoP only needs 261 and 76 mV overpotential to drive the current density of 20 mA cm^(-2) and 10 mA^(-2),which can be maintained unchanged for 100 h.This study provides new insights into anion doping strategies and catalyst reconstruction mechanisms.
基金supported by the Development Project of Youth Innovation Team in Shandong Colleges and Universities(No.2019KJC031)the Natural Science Foundation of Shandong Province(Nos.ZR2019MB064,ZR2021MB122 and ZR2022MB137)the Doctoral Program of Liaocheng University(No.318051608).
文摘Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.
基金supported by the National Natural Science Foundation of China(Nos.22171287 and 52303274)Taishan Scholar Project of Shandong Province(No.tsqn202103046)+2 种基金Natural Science Foundation of Shandong Province(No.ZR2022QE175)Young Innovative Science and Technology Support Program for Universities of Shandong Province,P.R.China(Nos.2023KJ280 and 2021KJ014)Fundamental Research Funds for the Central Universities(Nos.24CX07007A and 22CX01002A-1)
文摘Constructing clus ter heterostructures with strongly coupled interfaces is of great importance to accelerating the catalytic reactions that involve multiple intermediates.Herein,a strongly coupled cluster heterostructure composed of platinum and molybdenum carbide(Pt@Mo_(2)C)derived from polyoxometalate clusters is designed to achieve excellent alkaline hydrogen evolution reaction.The Pt@Mo_(2)C cluster exhibits strong electronic interactions between Pt and Mo_(2)C,working together to facilitate the H_(2)O dissociation by concurrently binding intermediates(Pt-H*and Mo-OH*),thus accelerating the kinetics of the rate-determining Volmer step.Theoptimized Pt@Mo_(2)C exhibits a high mass activity of12.1 A·mgpt^(-1),19.2 times higher than that of 20%Pt/C in alkaline media.Moreover,it can be stabilized at a current density of 100 mA·cm^(-2)for more than 200 h.This work demonstrated the superiority of the cluster heterostructures and co-catalytic effect towards the development of highly efficient electrocatalysts.
基金financial support from the National Natural Science Foundation of China(No.52471219)the Fundamental Research Funds for the Central Universities(No.00007838)+5 种基金financial support from the National Natural Science Foundation of China(No.52471220 and U2441264)the Guangdong Basic and Applied Basic Research Foundation(No.2022A1515140051)financial support from the National Natural Science Foundation of China(No.92163209)Beijing Natural Science Foundation(No.JQ22004)financial support from the National Natural Science Foundation of China(No.52476146)Guangdong Basic and Applied Basic Research Foundation(2023A1515140059,2025A1515011255).
文摘The structural modulation of metal-based heterostructure plays a vital role in achieving enhanced performances for highly efficient electrocatalysis.Here we design submonolayered Ru-modified Pd mesoporous nanosheets(Pd-Ru MNSs)with the exposure of both Pd and Ru active sites as well as the high atomic utilization of two-dimensional structure.The obtained Pd-Ru MNSs can act as a highly efficient multifunctional catalyst for hydrogen evolution reaction(HER)and alcohol oxidation reactions including ethylene glycol oxidation(EGOR)and ethanol oxidation(EOR),offering new opportunities towards the alcohol oxidation assisted hydrogen production.Specifically,Pd-Ru MNSs demonstrate excellent HER performance in alkaline electrolyte,requiring an overpotential of only 16mV to reach 10mAcm^(−2),significantly outperforming Pd mesoporous nanosheets and commercial catalysts.Density functional theory calculations reveal that the Ru sites in Pd-Ru MNSs could facilitate the water adsorption,accelerate the water dissociation,and optimize the hydrogen desorption,leading to the superior HER activity.Pd-Ru MNSs also exhibit high mass activities of 11.19 A mg^(−1)Pd for EGOR and 8.84 A mg^(−1)Pd for EOR,which is 7.8 and 9.6 times than that of commercial Pd/C,respectively.The EGOR reaction pathway over Pd-Ru MNSs was further investigated by using in situ Fourier-transform infrared spectroscopy.
基金supported by the National Natural Science Foundation of China(No.52102470)。
文摘As a clean energy source,hydrogen plays a critical role in the global mission to achieve carbon neutrality.Among varied hydrogen production techniques,water electrolysis driven by clean energy,such as solar or wind energy,is the most promising and viable option,with the advantages of celerity,high efficiency,cleanliness,and sustainability.However,this process necessitates a highly active and durable hydrogen evolution reaction(HER)catalyst to enhance the overall reaction efficiency.This article thoroughly reviews the recent development of electrocatalysts exhibiting high-performance HER.In particular,a comprehensive look at noble metals platinum(Pt),ruthenium(Ru),iridium(Ir),and non-noble metals,including sulfides,carbides,nitrides and phosphides is taken.Synthesis strategies,methods for enhancing performance,and the correlation between structure,composition,and catalytic performance are discussed.We also pay particular attention to density functional theory(DFT)calculations to reveal the mechanisms behind the improvement of HER performance.Finally,the critical challenges associated with electrochemical water splitting and propose coping strategies are presented.
文摘Exploring platinum single-atom electrocatalysts(SACs)is of great significance for effectively catalyzing the hydrogen evolution reaction in order to maximize the utilization of metal atoms.Herein,ruthenium clusters with several atoms(Rux)supported on nitrogen-doped,cost-efficient Black Pearls 2000(Ru_(x)NBP),were synthesized as initial materials via a simple hydrothermal method.Then,[PtCl_(4)]^(2–)ion was reductively deposited on RuxNBP to obtain a Pt SAC(Pt1/RuxNBP).Electrochemical measurements demonstrate the excellent HER performance of Pt_(1)/Ru_(x)NBP with a 5.7-fold increase in mass activity compared to the commercial Pt/C at 20 mV.Moreover,the cell voltage of the proton exchange membrane electrolyzer with Pt_(1)/Ru_(x)NBP is 20 mV lower compared to that with commercial Pt/C at 1.0 A cm^(−2).Physical characterization and density functional theory calculations revealed that the preserved Pt–Cl bond of[PtCl_(4)]^(2–)and the RuxNBP support co-regulate the 5d state of isolated Pt atoms and enhance the catalytic HER capacity of Pt1/RuxNBP.
基金supported by the Frontier Exploration Projects of Longmen Laboratory(No.LMQYTSKT008)the Program for Science and Technology Innovation Talents in Universities of Henan Province(Nos.22HASTIT008 and 24HASTIT006)+2 种基金the Natural Science Foundations of Henan Province(Nos.222300420502 and 242300420045)the Programs for Science and Technology Development of Henan Province(No.242102240066)the Key Scientific Research Projects of University in Henan Province(No.23B430002)。
文摘Electrochemical water splitting is a highly promising approach for producing carbon-neutral hydrogen.The development of efficient electrocatalysts for the hydrogen evolution reaction(HER)is crucial to lowering the energy barriers and enhancing hydrogen production.This drives the search for HER electrocatalysts that are not only cost-effective and abundant but also exhibit high activity and long-term stability.In this review,we provide an in-depth analysis of recent progress in the application of ruthenium phosphides as HER electrocatalysts,offering key insights into their design and performance.Meanwhile,we explore various strategies to enhance their catalytic efficiency,such as increasing the availability of active sites and optimizing their electronic structure.Finally,we outline the key challenges and future directions for developing the next generation of ruthenium phosphide-based HER electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(32101452)the Research Foundation of Education Bureau of Hunan Province(22B0283)+2 种基金the Hunan Provincial Natural Science Foundation(2022JJ40865)the Talents Research Funding of Central South University of Forestry and Technology(2021YJ007)the Scientific Innovation Fund for Graduate of Central South University of Forestry and Technology(2024CX02005)。
文摘High-performance catalyst is significant for the sustainable hydrogen(H_(2))production by electrocatalytic water splitting.Optimizing porous structure and active groups of substrate can promote the interaction of substrate and active metal particles,enabling excellent catalytic properties and stability.Herein,the optimization strategy of delignification and 2,2,6,6-tetramethylpyperidine-1-oxyl(TEMPO)oxidization was developed to modify the porous structure and active groups of wood substrate,and Ru doped Co/CO_(2)P(Ru-Co/CO_(2)P)nanoparticles were encapsulated into the optimized wood carbon substrate(Ru-Co/CO_(2)P@TDCW)for the efficient pH-universal hydrogen evolution reaction(HER).The nanopore and carboxyl groups were produced by delignification and TEMPO oxidation,which accelerated the dispersion and deposition of Ru-Co/CO_(2)P nanoparticles.The RuCo alloy and RuCoP nanoparticles were produced with the doping of Ru,and more Ru-Co/CO_(2)P nanoparticles were anchored by the delignified and TEMPO oxidized wood carbon(TDCW).As anticipated,the Ru-Co/CO_(2)P@TDCW catalyst exhibited excellent pH-universal HER activity,and only 16.6,93,and 43 mV of overpotentials were required to deliver the current density of 50 mA cm^(-2)in alkaline,neutral,and acidic electrolytes,outperforming the noble Pt/C/TDCW catalyst significantly.In addition,Ru-Co/CO_(2)P@TDCW catalyst presented excellent stability for more than 600 h working at 100 mA cm^(-2)in alkaline solution(1.0 M KOH).Density function theory(DFT)results revealed that energy barriers for the dissociation of H_(2)O and the formation of H_(2)were decreased by the doping of Ru,and the conductivity and efficiency of electron migration were also enhanced.This work demonstrated a strategy to optimize the structure and properties of wood carbon substrate,providing a promising strategy to synthesize high-efficiency catalyst for H_(2)production.
基金supported by the National Natural Science Foundation of China(22369025)Yunnan Applied Basic Research Projects(202201AT070095,202301AT070098,202301AT070107,202401AT070438,202401AT070433)+2 种基金the 3rd Professional Degree Graduate Practice Innovation Project of Yunnan University(ZC-23235291,ZC-23234269,KC-23236398,KC-23234063)the Education Reform Research Project of Yunnan University(No.2021Z06)the Xingdian Talent Program of Yunnan Province,and the Yunnan Revitalization Talent Support Program.
文摘Ruthenium(Ru)-based electrocatalysts show great promise as substitutes for platinum(Pt)for the alkaline hydrogen evolution reaction(HER)because of their efficient water dissociation capabilities.Nevertheless,the strong adsorption of Ru-OH intermediates(Ru-OHad)blocks the active site,leading to unsatisfactory HER performance.In this study,we report a universal ligand-exchange strategy for synthesizing a MOF-on-MOF-derived FeP-CoP heterostructure-anchored Ru single-atom site catalyst(Ru-FeP-CoP/NPC).The obtained catalyst shows a low overpotential(28 mV at 10 mA cm^(-2))and a high mass activity(9.29 A mg^(-1) at 100 mV),surpassing the performance of commercial Pt/C by a factor of 46.Theoretical studies show that regulating the local charge distribution of Ru single-atom sites could alleviate surrounding OH-blockages,accelerating water dissociation and facilitating hydrogen adsorption/desorption,thus enhancing HER activity.This work aims to inspire further design of highly active and durable electrocatalysts with tailored electronic properties for high-purity hydrogen production.
文摘Correction to:Nano-Micro Letters(2025)17:123 https://doi.org/10.1007/s40820-025-01654-y Following publication of the original article[1],the authors reported that Dr.Mohamed Bououdina’s affiliation needed to be corrected from 1 to 2.The correct author affiliation has been provided in this Correction and the original article[1]has been corrected.
文摘Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-proton transfers more complex when determining kinetics and mass transfer information.Understanding how HER competes with other electrochemical reduction reactions is crucial for both fundamental studies and system performance improvements.In this study,we employed the oxygen reduction reaction(ORR)as a model reaction to investigate HER competition on a polycrystalline-Au surface,using a rotating ring and disk electrode.It’s proved that water molecules serve as the proton source for ORR in alkaline,neutral,and even acidic electrolytes,and a 4-electron process can be achieved when the overpotential is sufficiently high.The competition from H⁺reduction becomes noticeable at the H⁺concentration higher than 2 mmol L^(–1)and intensi-fies as the H^(+)concentration increases.Based on the electrochemical results,we obtained an equivalent circuit diagram for the ORR system with competition from the H+reduction reaction,showing that these reactions occur in parallel and compete with each other.Electrochemical impedance spectroscopy measurements further confirm this argument.Additionally,we discover that the contribution of H+mass transfer to the total H^(+)reduction current is significant and comparable to the kinetic current.We believe this work will deepen our understanding of HER and its competition in electrochemical reduction systems.
