Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via lo...Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.展开更多
Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted ...Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted significant attention due to their strong structural flexibility and easy accessibility.Nevertheless,understanding the connection between their electronic,structural properties,and catalytic performance must remain a top priority.Synchrotron radiation(SR)X-ray absorption spectroscopy(XAS)techniques,including hard XAS and soft XAS,are recognized as efficient and comprehensive platforms for probing the surface,interface,and bulk electronic structure of elements of interest in the materials community.In the past decade,the flourishing development of materials science and advanced characterization technologies have led to a deeper understanding at different temporal,longitudinal,and spatial scales.In this review,we briefly describe the concept of XAS techniques and summarize their recent progress in addressing scientific questions on carbon-supported electrocatalysts through the development of advanced instruments and experimental methods.We then discuss the remaining challenges and potential research directions in nextgeneration materials frontiers,and suggest challenges and perspectives for shedding light on the structure–activity relationship.展开更多
Rational synthesis of a new class of electrocatalysts with high-performance and low-cost is of great significance for future fuel cell devices. Herein, we demonstrate a general one-step simultaneous reduction method t...Rational synthesis of a new class of electrocatalysts with high-performance and low-cost is of great significance for future fuel cell devices. Herein, we demonstrate a general one-step simultaneous reduction method to prepare carbon-supported Pd M（M = Co, Fe, Ni） alloyed nanodendrites with the assistance of oleylamine and octadecylene. The morphology, structure and composition of the obtained Pd M nanodendrites/C catalysts have been fully characterized. The combination of the dendritic structural feature and alloyed synergy offer higher atomic utilization efficiency, excellent catalytic activity and enhanced stability for the formic acid oxidation reaction（FAOR）. Strikingly, the as-synthesized Pd Co nanodendrites/C catalyst could afford a mass current density of 2467.7 A g, which is almost 3.53 and 10.4 times higher than those of lab-made Pd/C sample(698.3 A g) and commercial Pd/C catalyst(237.6 A g), respectively. Furthermore, the PdC o nanodendrites/C catalyst also exhibit superior stability relative to the Pd/C catalysts, make it a promising anodic electrocatalyst in practical fuel cells in the future. Additionally, the present feasible synthetic approach is anticipated to provide a versatile strategy toward the preparation of other metal alloy nanodendrites/carbon nanohybrids.展开更多
This study explores a novel strategy to enhance the hydrogen evolution reaction(HER)activity of carbon-supported rock salt-type NiCo_(2)(O,F)_(3) nanorods through lattice modifications induced by fluorine and excess a...This study explores a novel strategy to enhance the hydrogen evolution reaction(HER)activity of carbon-supported rock salt-type NiCo_(2)(O,F)_(3) nanorods through lattice modifications induced by fluorine and excess amorphous carbon.X-ray absorption near-edge structure(XANES)analysis confirmed that Co and Ni predominantly exist in the+2 oxidation state,whereas extended X-ray absorption fine structure(EXAFS)analysis revealed shortened Co-O and Co-Co bond lengths,indicating lattice distortions.Rietveld refinement and electron microscopy confirmed the formation of a homogeneous solid solution(NixCo_(2-x)(O,F)_(3))rather than a simple CoO/NiO composite.The optimized material(AH-2)exhibited the lowest overpotential(145 mV at 10 mA cm^(-1))and the smallest Tafel slope(98 mV dec^(-1)),attributed to its balanced phase composition,enhanced electronic conductivity,and synergistic effects of carbon and fluorine incorporation.Electrochemical impedance spectroscopy(EIS)confirmed improved charge transfer efficiency,correlating with enhanced catalytic activity.These findings provide critical insights into the tunability of transition metal oxide catalysts via controlled lattice modifications,offering a promising avenue for developing cost-effective and efficient electrocatalysts for sustainable hydrogen production.展开更多
Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements hav...Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.展开更多
The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-ass...The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.展开更多
Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt...Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt-based electrocatalysts,emphasizing their structural engineering for enhanced the performance of electrocatalytic nitrate reduction reaction(NO3RR)through dimensional control,compositional tuning,and coordination microenvironment modulation.Notably,by critically analyzing metallic cobalt,cobalt alloys,cobalt compounds,cobalt single atom and molecular catalyst configurations,we firstly establish correlations between atomic-scale structural features and catalytic performance in a coordination environment perspective for NO3RR,including the dynamic reconstruction during operation and its impact on active site.Synergizing experimental breakthroughs with computational modeling,we decode mechanisms underlying competitive hydrogen evolution suppression,intermediate adsorption-energy optimization,and durability enhancement in complex aqueous environments.The development of cobalt-based catalysts was summarized and prospected,and the emerging opportunities of machine learning in accelerating the research and development of high-performance catalysts and the configuration of series reactors for scalable nitrate-to-ammonia systems were also introduced.Bridging surface science and applications,it outlines a framework for designing multifunctional electrocatalysts to restore nitrogen cycle balance sustainably.展开更多
Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparti...Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.展开更多
Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that...Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.展开更多
Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is design...Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is designed by using Co-compounds as the core and PO_(4)^(3-)decorated Fe-compounds as the shell.The inner Co-core and outer Fe-shell are connected through Co-O-Fe and Fe-O-P linkage.The Co@Fe-P electrocatalyst exhibits an enhanced performance for OER with a low overpotential(280 mV),low Tafel slope(41.9 mV dec^(-1))at 10 mA cm^(-2),and a 60-h durability.The electron transfer from the CoOOH-core to the FeOOH-shell is greatly facilitated,which improves the OER activity of Co@Fe-P kinetically.Theoretical calculations indicate that the interaction of Co-O-Fe and Fe-O-P in Co@Fe-P reduces the overlap between the O 2p and Fe 3d orbitals,which greatly facilitates the transformation from*OH to*O during the OER process via the adsorbate evolution mechanism(AEM)pathway.This finding provides insight for the design of efficient electrocatalysts for OER.展开更多
Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen ba...Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.展开更多
The activated carbon-supported TiO2 nanoparticles(TiO2/AC)were prepared by a properly controlled sol-gel method.The effects of activated carbons(AC)support on inactivated properties of TiO2 nanoparticles were evaluate...The activated carbon-supported TiO2 nanoparticles(TiO2/AC)were prepared by a properly controlled sol-gel method.The effects of activated carbons(AC)support on inactivated properties of TiO2 nanoparticles were evaluated by photocatalytic inactivation experiments of Escherichia coli.The key factors affecting the inactivation effciency were investigated,including electric power of lamp, temperature,and pH values.The results show that the TiO2/AC composites have high inactivation properties of E.coli in compari...展开更多
As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants....As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.展开更多
Carbon-supported copper catalyst was prepared for the first time in one-step with copper nitrate and corn stalk through calcination under different temperatures. Uniformly dispersed nanoparticles were obtained and wer...Carbon-supported copper catalyst was prepared for the first time in one-step with copper nitrate and corn stalk through calcination under different temperatures. Uniformly dispersed nanoparticles were obtained and were identified to be Cu（0） and Cu（Ⅰ） in XRD patterns. Excellent catalytic activity and selectivity were achieved in the N-arylation of pyrazole under ligand and protection gas free conditions. About90.4% of product yield was achieved with only 0.5 mol% of copper catalyst（Cu-C-300）, which was considerably more efficient than previous reports. XPS results suggested that the N-arylation of pyrazole activity was closely related to the surface Cu（Ⅰ） species.展开更多
Electrocatalysts play a crucial role in the development of renewable energy conversion and storage nanotechnologies.The unique advantages of heteroatom-doped porous carbon-supported single-atom electrocatalysts(SAC-HD...Electrocatalysts play a crucial role in the development of renewable energy conversion and storage nanotechnologies.The unique advantages of heteroatom-doped porous carbon-supported single-atom electrocatalysts(SAC-HDPCs)are clear.These SAC-HDPCs exhibit outstanding activity,selectivity and stability due to their distinct electronic structure,satisfactory conductivity,controllable porosity and heteroatomdoping effect.Rapid and significant developments involving the synthesis,characterization,and structure-property-function relationship of SAC-HDPCs have been made in recent years.In this review,we describe recent research efforts involving advanced(in situ)characterization techniques,innovative synthetic strategies,and electrochemical energy conversion examples of SAC-HDPCs.The electrocatalytic performance of SAC-HDPCs is further considered at an atomic level,and the mechanisms underlying this performance are also discussed in detail.We expect that these analyses and deductions will be useful for the design of new materials and may help to establish a foundation for the design of future SAC-HDPCs.展开更多
By evaluating the SEM images,specific surface area,and the catalytic synthesis reaction conditions of an activated carbon-supported p-toluenesulfonic acid catalyst,and comparing the physical and chemical properties,in...By evaluating the SEM images,specific surface area,and the catalytic synthesis reaction conditions of an activated carbon-supported p-toluenesulfonic acid catalyst,and comparing the physical and chemical properties,infrared spectra,nuclear magnetic resonance spectra,oxidation stability,thermal stability,hydrolytic stability,and extreme pressure anti-wear performance of the synthesized trihydroxymethylpropyl trioleate with imported reference esters,the feasibility of its application as a substitute was investigated.The results indicated that the activated carbon-supported p-toluenesulfonic acid catalyst exhibited loose porosity,high specific surface area,and high esterification efficiency.When synthesized under optimal conditions,the yield rate of trihydroxymethylpropyl trioleate reached 99.3%,with a simple separation process that did not require additional steps such as neutralization and washing and generated minimal wastewater.The physical and chemical properties of the synthesized trihydroxymethylpropyl trioleate were comparable to those of the reference ester in terms of color,viscosity,viscosity index,flash point,and pour point.Moreover,the peak position and peak height in the infrared and nuclear magnetic carbon spectra were essentially the same.Through comprehensive evaluations and comparisons of various properties,it was determined that the performance of trihydroxymethylpropyl trioleate was comparable to that of the imported reference esters.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
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
Advanced OER/HER electrocatalytic alternatives are crucial for the wide adaptation of green hydrogen energy.Herein,Ru/NiMnB spherical cluster pillar(SCP),denoted as Ru/NiMnB,is synthesized using a combination of elect...Advanced OER/HER electrocatalytic alternatives are crucial for the wide adaptation of green hydrogen energy.Herein,Ru/NiMnB spherical cluster pillar(SCP),denoted as Ru/NiMnB,is synthesized using a combination of electro-deposition and hydrothermal reaction.Systematic investigation of Ru doping in the NiMnB matrix revealed significant improvements in electrocatalytic performance.The Ru/NiMnB SCPs demonstrate superior OER/HER activity with low overpotentials of 150 and 103 mV at 50mA/cm^(2)in 1 M KOH,making them highly competitive with state-of-the-art electrocatalysts.Remarkably,the Ru/NiMnB SCPs exhibit a low 2-E cell voltage of 2.80 V at ultra-high current density of 2,000 m A/cm^(2)in 1 M KOH,outperforming the standard benchmark electrodes of RuO_(2)||Pt/C,thereby positioning Ru/NiMnB as one of the best bifunctional electrocatalysts.These SCPs exhibit exceptional high-current characteristics,stability and corrosion resistance,as evidenced by continuous operation at 1,000 mA/cm^(2)high-current density for over 150 h in 6 M KOH at elevated temperatures under harsh industrial conditions.Only a small amount of Ru incorporation significantly enhances the electrocatalytic performances of NiMnB,attributed to increased active sites and improved intrinsic properties such as conductivity,adsorption/desorption capability and reaction rates.Consequently,Ru/NiMnB SCPs present a promising bi-functional electrode concept for efficient green H_(2)production.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
基金the National Nature Science Foundation of China for Excellent Young Scientists Fund(32222058)Fundamental Research Foundation of CAF(CAFYBB2022QB001).
文摘Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.
基金supported in part by the National Key R&D Program of China(Nos.2020YFA0405800,2022YFA1504104,and 2022YFA1605400)the National Natural Science Foundation of China(Nos.12225508,12322515,U1932201,U2032113,and 22075264)+5 种基金the Youth Innovation Promotion Association of CAS(No.2022457)the Institute of Energy,Hefei Comprehensive National Science Center,University Synergy Innovation Program of Anhui Province(No.GXXT-2020-002)and the CAS Iterdisciplinary Innovation Team.We thank the Shanghai Synchrotron Radiation Facility(BL14W1,BL14B1,and SSRF)the Beijing Synchrotron Radiation Facility(1W1B,4B7A,and BSRF)the Hefei Synchrotron Radiation Facility(Infrared Spectroscopy and Microspectroscopy,MCD-A and MCD-B Soochow Beamline for Energy Materials at NSRL)and the USTC Center for Micro and Nanoscale Research and Fabrication for helps in characterizations.
文摘Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted significant attention due to their strong structural flexibility and easy accessibility.Nevertheless,understanding the connection between their electronic,structural properties,and catalytic performance must remain a top priority.Synchrotron radiation(SR)X-ray absorption spectroscopy(XAS)techniques,including hard XAS and soft XAS,are recognized as efficient and comprehensive platforms for probing the surface,interface,and bulk electronic structure of elements of interest in the materials community.In the past decade,the flourishing development of materials science and advanced characterization technologies have led to a deeper understanding at different temporal,longitudinal,and spatial scales.In this review,we briefly describe the concept of XAS techniques and summarize their recent progress in addressing scientific questions on carbon-supported electrocatalysts through the development of advanced instruments and experimental methods.We then discuss the remaining challenges and potential research directions in nextgeneration materials frontiers,and suggest challenges and perspectives for shedding light on the structure–activity relationship.
基金financial supports from NSFC(no.21576139,21503111 and 21376122)Natural Science Foundation of Jiangsu Province(BK20171473)+2 种基金Natural Science Foundation of Jiangsu Higher Education Institutions of China(16KJB150020)National and Local Joint Engineering Research Center of Biomedical Functional Materialsa project sponsored by the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Rational synthesis of a new class of electrocatalysts with high-performance and low-cost is of great significance for future fuel cell devices. Herein, we demonstrate a general one-step simultaneous reduction method to prepare carbon-supported Pd M（M = Co, Fe, Ni） alloyed nanodendrites with the assistance of oleylamine and octadecylene. The morphology, structure and composition of the obtained Pd M nanodendrites/C catalysts have been fully characterized. The combination of the dendritic structural feature and alloyed synergy offer higher atomic utilization efficiency, excellent catalytic activity and enhanced stability for the formic acid oxidation reaction（FAOR）. Strikingly, the as-synthesized Pd Co nanodendrites/C catalyst could afford a mass current density of 2467.7 A g, which is almost 3.53 and 10.4 times higher than those of lab-made Pd/C sample(698.3 A g) and commercial Pd/C catalyst(237.6 A g), respectively. Furthermore, the PdC o nanodendrites/C catalyst also exhibit superior stability relative to the Pd/C catalysts, make it a promising anodic electrocatalyst in practical fuel cells in the future. Additionally, the present feasible synthetic approach is anticipated to provide a versatile strategy toward the preparation of other metal alloy nanodendrites/carbon nanohybrids.
基金supported by the Russian Science Foundation(project No.24-43-00215,http://rscf.ru/project/24-43-00215/).
文摘This study explores a novel strategy to enhance the hydrogen evolution reaction(HER)activity of carbon-supported rock salt-type NiCo_(2)(O,F)_(3) nanorods through lattice modifications induced by fluorine and excess amorphous carbon.X-ray absorption near-edge structure(XANES)analysis confirmed that Co and Ni predominantly exist in the+2 oxidation state,whereas extended X-ray absorption fine structure(EXAFS)analysis revealed shortened Co-O and Co-Co bond lengths,indicating lattice distortions.Rietveld refinement and electron microscopy confirmed the formation of a homogeneous solid solution(NixCo_(2-x)(O,F)_(3))rather than a simple CoO/NiO composite.The optimized material(AH-2)exhibited the lowest overpotential(145 mV at 10 mA cm^(-1))and the smallest Tafel slope(98 mV dec^(-1)),attributed to its balanced phase composition,enhanced electronic conductivity,and synergistic effects of carbon and fluorine incorporation.Electrochemical impedance spectroscopy(EIS)confirmed improved charge transfer efficiency,correlating with enhanced catalytic activity.These findings provide critical insights into the tunability of transition metal oxide catalysts via controlled lattice modifications,offering a promising avenue for developing cost-effective and efficient electrocatalysts for sustainable hydrogen production.
基金financially supported by the National Natural Science Foundation of China (22350410386,W2412116,22375200,U22A202175,21961142006)。
文摘Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.
基金financial support of the National Natural Science Foundation of China (21875247,21072221, 21172252)the Project of Talent Cultivation for Carbon Peak and Carbon Neutrality of the University of Chinese of Academy of Science
文摘The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.
基金supported by the National Natural Science Foundation of China(Grant Nos.:21825201,52401244 and 52201227)Henan Province Key Research and Development and Promotion Program(Scientific and Technological Breakthrough Project:232102240088 and 252102230078)+3 种基金the Key Research&Development and Promotion of Special Project(Scientific Problem Tackling)of Henan Province(252102230078)Doctoral Research Startup Fund Project of Henan Open University(BSJH-2025-04)Zhejiang Provincial Natural Science Foundation of China(LQ24B020005,LQ23B030001)China Postdoctoral Science Foundation(2024M762442).
文摘Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt-based electrocatalysts,emphasizing their structural engineering for enhanced the performance of electrocatalytic nitrate reduction reaction(NO3RR)through dimensional control,compositional tuning,and coordination microenvironment modulation.Notably,by critically analyzing metallic cobalt,cobalt alloys,cobalt compounds,cobalt single atom and molecular catalyst configurations,we firstly establish correlations between atomic-scale structural features and catalytic performance in a coordination environment perspective for NO3RR,including the dynamic reconstruction during operation and its impact on active site.Synergizing experimental breakthroughs with computational modeling,we decode mechanisms underlying competitive hydrogen evolution suppression,intermediate adsorption-energy optimization,and durability enhancement in complex aqueous environments.The development of cobalt-based catalysts was summarized and prospected,and the emerging opportunities of machine learning in accelerating the research and development of high-performance catalysts and the configuration of series reactors for scalable nitrate-to-ammonia systems were also introduced.Bridging surface science and applications,it outlines a framework for designing multifunctional electrocatalysts to restore nitrogen cycle balance sustainably.
基金the staff of beamline BL13SSW at Shanghai Synchrotron Radiation Facility for experiments supports. This study was financially supported by the National Natural Science Foundation of China (No. 12205165)Hebei Province Innovation Ability Improvement Plan Project (No. 225676111H).
文摘Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.
基金Funded by the National Natural Science Foundation of China Guangdong(No.22279096)。
文摘Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.
基金financially supported by the National Natural Science Foundation of China(Nos.22372143 and 22208281)the Hebei Natural Science Foundation(Nos.B2023203001 and B2025203050)the Science Research Project of Hebei Education Department(BJK2024122)。
文摘Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is designed by using Co-compounds as the core and PO_(4)^(3-)decorated Fe-compounds as the shell.The inner Co-core and outer Fe-shell are connected through Co-O-Fe and Fe-O-P linkage.The Co@Fe-P electrocatalyst exhibits an enhanced performance for OER with a low overpotential(280 mV),low Tafel slope(41.9 mV dec^(-1))at 10 mA cm^(-2),and a 60-h durability.The electron transfer from the CoOOH-core to the FeOOH-shell is greatly facilitated,which improves the OER activity of Co@Fe-P kinetically.Theoretical calculations indicate that the interaction of Co-O-Fe and Fe-O-P in Co@Fe-P reduces the overlap between the O 2p and Fe 3d orbitals,which greatly facilitates the transformation from*OH to*O during the OER process via the adsorbate evolution mechanism(AEM)pathway.This finding provides insight for the design of efficient electrocatalysts for OER.
基金financially supported by the National Natural Science Foundation of China(U21A20311,U24A2040,52171141,52272117)the Natural Science Foundation of Shandong Province(ZR2022JQ19)+3 种基金the Key Technology Research Project of Shandong Province(2023CXGC010202)the Taishan Industrial Experts Program(TSCX202306142)the Core Facility Sharing Platform of Shandong Universitythe Foundation of Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University。
文摘Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.
基金supported by the Educational and Tech-nological Department of Hunan Province(No.08B063)the Natural Science Foundation of Science and Technology Department of Hunan Government(No.2007GK3060)the Doctor Foundation of Jishou University(No.JSDXKYZZ200648).
文摘The activated carbon-supported TiO2 nanoparticles(TiO2/AC)were prepared by a properly controlled sol-gel method.The effects of activated carbons(AC)support on inactivated properties of TiO2 nanoparticles were evaluated by photocatalytic inactivation experiments of Escherichia coli.The key factors affecting the inactivation effciency were investigated,including electric power of lamp, temperature,and pH values.The results show that the TiO2/AC composites have high inactivation properties of E.coli in compari...
基金This work was financially supported by the Science and Technology project of Jiangsu province(BN2015021,XZ-SZ201819).
文摘As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.
基金supported by the Natural Science Foundation of China(91645115 and 21473003)High-level talents funding project of Hebei(CL201601,E2016100015)science technology research and development guidance program project of Baoding City(No.16ZF027)
文摘Carbon-supported copper catalyst was prepared for the first time in one-step with copper nitrate and corn stalk through calcination under different temperatures. Uniformly dispersed nanoparticles were obtained and were identified to be Cu（0） and Cu（Ⅰ） in XRD patterns. Excellent catalytic activity and selectivity were achieved in the N-arylation of pyrazole under ligand and protection gas free conditions. About90.4% of product yield was achieved with only 0.5 mol% of copper catalyst（Cu-C-300）, which was considerably more efficient than previous reports. XPS results suggested that the N-arylation of pyrazole activity was closely related to the surface Cu（Ⅰ） species.
基金financial support from the Nankai UniversityNational Science Foundation of China(No.21875119)+1 种基金Natural Science Foundation of Tianjin(19JCYBJC17500)the open fund of the key laboratory of advanced functional polymer materials,the ministry of education(Nankai University,KLFPM202001)。
文摘Electrocatalysts play a crucial role in the development of renewable energy conversion and storage nanotechnologies.The unique advantages of heteroatom-doped porous carbon-supported single-atom electrocatalysts(SAC-HDPCs)are clear.These SAC-HDPCs exhibit outstanding activity,selectivity and stability due to their distinct electronic structure,satisfactory conductivity,controllable porosity and heteroatomdoping effect.Rapid and significant developments involving the synthesis,characterization,and structure-property-function relationship of SAC-HDPCs have been made in recent years.In this review,we describe recent research efforts involving advanced(in situ)characterization techniques,innovative synthetic strategies,and electrochemical energy conversion examples of SAC-HDPCs.The electrocatalytic performance of SAC-HDPCs is further considered at an atomic level,and the mechanisms underlying this performance are also discussed in detail.We expect that these analyses and deductions will be useful for the design of new materials and may help to establish a foundation for the design of future SAC-HDPCs.
文摘By evaluating the SEM images,specific surface area,and the catalytic synthesis reaction conditions of an activated carbon-supported p-toluenesulfonic acid catalyst,and comparing the physical and chemical properties,infrared spectra,nuclear magnetic resonance spectra,oxidation stability,thermal stability,hydrolytic stability,and extreme pressure anti-wear performance of the synthesized trihydroxymethylpropyl trioleate with imported reference esters,the feasibility of its application as a substitute was investigated.The results indicated that the activated carbon-supported p-toluenesulfonic acid catalyst exhibited loose porosity,high specific surface area,and high esterification efficiency.When synthesized under optimal conditions,the yield rate of trihydroxymethylpropyl trioleate reached 99.3%,with a simple separation process that did not require additional steps such as neutralization and washing and generated minimal wastewater.The physical and chemical properties of the synthesized trihydroxymethylpropyl trioleate were comparable to those of the reference ester in terms of color,viscosity,viscosity index,flash point,and pour point.Moreover,the peak position and peak height in the infrared and nuclear magnetic carbon spectra were essentially the same.Through comprehensive evaluations and comparisons of various properties,it was determined that the performance of trihydroxymethylpropyl trioleate was comparable to that of the imported reference esters.
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Core Research Institute Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.2018R1A6A1A03025242)in part by the research grant of Kwangwoon University in 2024。
文摘Advanced OER/HER electrocatalytic alternatives are crucial for the wide adaptation of green hydrogen energy.Herein,Ru/NiMnB spherical cluster pillar(SCP),denoted as Ru/NiMnB,is synthesized using a combination of electro-deposition and hydrothermal reaction.Systematic investigation of Ru doping in the NiMnB matrix revealed significant improvements in electrocatalytic performance.The Ru/NiMnB SCPs demonstrate superior OER/HER activity with low overpotentials of 150 and 103 mV at 50mA/cm^(2)in 1 M KOH,making them highly competitive with state-of-the-art electrocatalysts.Remarkably,the Ru/NiMnB SCPs exhibit a low 2-E cell voltage of 2.80 V at ultra-high current density of 2,000 m A/cm^(2)in 1 M KOH,outperforming the standard benchmark electrodes of RuO_(2)||Pt/C,thereby positioning Ru/NiMnB as one of the best bifunctional electrocatalysts.These SCPs exhibit exceptional high-current characteristics,stability and corrosion resistance,as evidenced by continuous operation at 1,000 mA/cm^(2)high-current density for over 150 h in 6 M KOH at elevated temperatures under harsh industrial conditions.Only a small amount of Ru incorporation significantly enhances the electrocatalytic performances of NiMnB,attributed to increased active sites and improved intrinsic properties such as conductivity,adsorption/desorption capability and reaction rates.Consequently,Ru/NiMnB SCPs present a promising bi-functional electrode concept for efficient green H_(2)production.
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.
