Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR cataly...Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.展开更多
Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electro...Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electrocatalysts,hampering their large-scale commercial application.Hence,considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use,and consequently,the cost.Therefore,this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts,which significantly affect the nanoparticle size,shape,and dispersion on supports and thus the activity and durability of the prepared electrocatalysts.The reviewed processes include(i)the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects,(ii)the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts,(iii)the preparation of spheri-cal and nonspherical Pt-based electrocatalysts(polyhedrons,nanocages,nanoframes,one-and two-dimensional nanostruc-tures),and(iv)the postsynthesis treatments of supported electrocatalysts.The influences of the supports,key experimental parameters,and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail.Future research directions are outlined,including(i)the full exploitation of the potential functionalization of commercial carbon supports,(ii)scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts,and(iii)simplification of postsynthesis treatments.One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts.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
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
Proton-exchange membrane fuel cells(PEMFCs)have been widely used commercially to solve the energy crisis and environmental pollution.The oxygen reduction reaction(ORR)at the cathode is the rate-determining step in PEM...Proton-exchange membrane fuel cells(PEMFCs)have been widely used commercially to solve the energy crisis and environmental pollution.The oxygen reduction reaction(ORR)at the cathode is the rate-determining step in PEMFCs.Platinum(Pt)catalysts are used to accelerate the ORR kinetics.Pt’s scarcity,high cost,and instability in an acidic environment at high potentials seriously hinder the commercialization of PEMFCs.Therefore,studies should explore electrocatalysts with high catalytic activity,enhanced stability,and low-Pt loading.This review briefly introduces the research progress on Pt and Pt-based ORR electrocatalysts for PEMFCs,including anticorrosion catalyst supports,Pt,and Pt-based alloy electrocatalysts.Advanced preparation technology and material characterization of Pt-based ORR electrocatalysts are necessary to improve the performance and corresponding reaction mechanisms.展开更多
Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactio...Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research focus.In this review,the catalytic mechanism of Pt-based electrocatalysts is firstly introduced.Subsequently,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural reconfiguration.Finally,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy.展开更多
Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)...Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.展开更多
Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,e...Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,electronic structure,physiochemical property and function of Pt.This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts,with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports,including porous carbon,heteroatom doped carbon,carbon-based binary support,and their corresponding electrocatalytic applications.Finally,the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed.展开更多
Application of an oxygen-depolarized cathode will contribute to energy saving in chlor-alkali electrolysis. For this purpose, the development of high-performance cathode with the best electrocatalyst is essential. Usi...Application of an oxygen-depolarized cathode will contribute to energy saving in chlor-alkali electrolysis. For this purpose, the development of high-performance cathode with the best electrocatalyst is essential. Using bimetallic Pt-based alloy electrocatalysts including PtPd and PtAg carbon-supported in oxygen-depolarized cathode chlor-alkali cell has been shown to have the high cell performance. This study presents application of PtRu carbon supported electrocatalyst oxygen-depolarized cathode and performance comparison of cells with carbon-supported PtRu, PtPd and PtAg electrocatalysts cathodes using the same DSA-Cl2 anode. Results show that there are quite similarity between the effects of various factors on the caustic current efficiency (CCE) in a zero-gap oxygen-depolarized chlor-alkali cells employing carbon-supported PtPd, PtRu and PtAg electrocatalysts. Besides, it seems that the PtPd/C electrocatalyst cathode has relatively higher performance than the other cathodes with PtAg/C and PtRu/C electrocatalysts in zero-gap chlor-alkali cells.展开更多
Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for ox...Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of PEMFCs.Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior.In this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail.First,recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed.Then,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively discussed.Finally,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.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
The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplore...The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplored challenge of substantial electrochemical overpotential,surface reconstruction has emerged as a necessary strategy.Focusing on key aspects such as Janus structures,overflow effects,the d-band center displacement hypothesis,and interface coupling related to electrochemical reactions is essential for water electrolysis.Emerging as frontrunners among next-generation electrocatalysts,Mott-Schottky(M-S)catalysts feature a heterojunction formed between a metal and a semiconductor,offering customizable and predictable interfacial synergy.This review offers an in-depth examination of the processes driving the hydrogen and oxygen evolution reactions(HER and OER),highlighting the benefits of employing nanoscale transition metal nitrides,carbides,oxides,and phosphides in M-S heterointerface catalysts.Furthermore,the challenges,limitations,and future prospects of employing M-S heterostructured catalysts for water splitting are thoroughly discussed.展开更多
Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as...Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.展开更多
Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These cata...Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction(ORR)due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be achieved.This agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these catalysts.However,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ORR.Therefore,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin states.Additionally,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR activity.We have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.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
The realization of practical solar hydrogen production relies on the development of efficient devices with nontoxic and low-cost materials.Since the predominant contributors for the performance and cost are the cataly...The realization of practical solar hydrogen production relies on the development of efficient devices with nontoxic and low-cost materials.Since the predominant contributors for the performance and cost are the catalyst and the light absorber,it is imperative to develop cost-effective catalysts and absorbers that are compatible with each other for achieving high performance.In this study,a 10%efficient solar-to-hydrogen conversion device was developed through the meticulous integration of low-cost Ni Heazlewoodite-based catalysts for the hydrogen evolution reaction(HER)and ternary bulk heterojunction organic semiconductor(OS)-based light absorbers.Se-incorporated Ni_(3)S_(2)was synthesized using a simple one-step hydrothermal method,which demonstrated a low overpotential and Tafel slope,indicating superior HER activity compared to Ni_(3)S_(2).The theoretical calculation results validate the enhanced HER performance of the Se-incorporated Ni_(3)S_(2)catalyst in alkaline electrolytes.The ternary phase organic light absorber is designed to generate tailored photovoltage and maximized photocurrent,resulting in a photocurrent density of 8.24 mA cm^(-2)under unbiased conditions,which corresponds to 10%solar to hydrogen conversion.Low-temperature photoluminescence spectroscopy results revealed that the enhanced photocurrent density originates from a reduction in both phonon-and vibration-induced inter-and intramolecular non-radiative decay.Our results establish a new benchmark for the emerging OS-based efficient solar hydrogen production based on nontoxic and cost-effective materials.展开更多
Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic perfo...Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.展开更多
The oxygen evolution reaction(OER),a critical half-reaction in water electrolysis,has garnered significant attention.However,sluggish OER kinetics has emerged as a major impediment to efficient electrochemical energy c...The oxygen evolution reaction(OER),a critical half-reaction in water electrolysis,has garnered significant attention.However,sluggish OER kinetics has emerged as a major impediment to efficient electrochemical energy conversion.There is an urgent need to design novel electrocatalysts with optimized OER kinetics and enhanced intrinsic activity to improve overall OER performance.Herein,one-dimensional(1D)nanocomposites with high electrocatalytic activity were developed through the deposition of CoFePBA nanocubes onto the surface of MnO_(2) nanowires.The electronic structure of the nanocomposite surface was modified,and the synergistic effects between transition metals were leveraged to enhance catalytic activity through the deposition of Prussian blue analog(PBA)nanocubes on manganese dioxide nanowires.Specifically,CoFePBA featured an open crystal structure that offiered numerous electrochemical active sites and efficient charge transfer pathways.Additionally,the synergistic interactions between Co and Fe significantly reduced the OER overpotential.Additionally,the 1D rigid MnO_(2) acted as protective armor,ensuring the stability of active sites within CoFePBA during the OER.The synthesized MnO_(2)@CoFePBA achieved an overpotential of 1.614 V at 10 mA/cm^(2) and a small Tafel slope of 94 mV/dec and demonstrated stable performance for over 200 h.This work offers new insights into the rational design of various PBA-based nanocomposites with high activity and stability.展开更多
基金supported by the National Natural Science Foundation of China(92061125,21978294)Beijing Natural Science Foundation(Z200012)+3 种基金Jiangxi Natural Science Foundation(20212ACB213009)DNL Cooperation Fund,CAS(DNL201921)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E055B003)Hebei Natural Science Foundation(B2020103043)。
文摘Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.
基金the Natural Sciences and Engineering Research Council of Canada(NSERC)via CRD Grant No.CRDPJ 522410-17a Discovery Grant from the Canadian Urban Transit Research&Innovation Consortium(CUTRIC)via Project No.160028Ballard Power Systems Inc.via Project No.SRA#077701.
文摘Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electrocatalysts,hampering their large-scale commercial application.Hence,considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use,and consequently,the cost.Therefore,this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts,which significantly affect the nanoparticle size,shape,and dispersion on supports and thus the activity and durability of the prepared electrocatalysts.The reviewed processes include(i)the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects,(ii)the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts,(iii)the preparation of spheri-cal and nonspherical Pt-based electrocatalysts(polyhedrons,nanocages,nanoframes,one-and two-dimensional nanostruc-tures),and(iv)the postsynthesis treatments of supported electrocatalysts.The influences of the supports,key experimental parameters,and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail.Future research directions are outlined,including(i)the full exploitation of the potential functionalization of commercial carbon supports,(ii)scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts,and(iii)simplification of postsynthesis treatments.One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts.
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Project supported by the National Key Research and Development Program of China(Grant No.2018YFB1502503)Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21090101)
文摘Proton-exchange membrane fuel cells(PEMFCs)have been widely used commercially to solve the energy crisis and environmental pollution.The oxygen reduction reaction(ORR)at the cathode is the rate-determining step in PEMFCs.Platinum(Pt)catalysts are used to accelerate the ORR kinetics.Pt’s scarcity,high cost,and instability in an acidic environment at high potentials seriously hinder the commercialization of PEMFCs.Therefore,studies should explore electrocatalysts with high catalytic activity,enhanced stability,and low-Pt loading.This review briefly introduces the research progress on Pt and Pt-based ORR electrocatalysts for PEMFCs,including anticorrosion catalyst supports,Pt,and Pt-based alloy electrocatalysts.Advanced preparation technology and material characterization of Pt-based ORR electrocatalysts are necessary to improve the performance and corresponding reaction mechanisms.
基金supported by the National Natural Science Foundation of China (22122202,22072051,21972051)the Guangdong Basic and Applied Basic Research Foundation (2021A1515012343)。
文摘Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research focus.In this review,the catalytic mechanism of Pt-based electrocatalysts is firstly introduced.Subsequently,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural reconfiguration.Finally,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy.
基金supported by the National Natural Science Foundation of China(21571038,22035004)the Education Department of Guizhou Province(2021312)+2 种基金the Foundation of Guizhou Province(2019-5666)the National Key R&D Program of China(2017YFA0700101)the State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University,202009)。
文摘Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.
基金National Key Research and Development Program of China(Grant Nos.2022YFB3805600 and 2022YFB3805604)National Natural Science Foundation of China(Grant No.52201286)+5 种基金Sino-German Center COVID19 Related Bilateral Collaborative Project(C-0046),FRFCU(2021qntd13)National 111 Project(B20002)Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2019A1515110436,2021A1515111131,2022A1515011905,and 2022A1515010137)Guangzhou Science and Technology Project(Grant No.202102020463)Guangdong Province International Scientific and Technological Cooperation Projects(Grant No.2020A0505100036)Shenzhen Science and Technology Program(Grant Nos.GJHZ20210705143204014,JCYJ20210324142010029,and KCXFZ20211020170006010).
文摘Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,electronic structure,physiochemical property and function of Pt.This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts,with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports,including porous carbon,heteroatom doped carbon,carbon-based binary support,and their corresponding electrocatalytic applications.Finally,the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed.
文摘Application of an oxygen-depolarized cathode will contribute to energy saving in chlor-alkali electrolysis. For this purpose, the development of high-performance cathode with the best electrocatalyst is essential. Using bimetallic Pt-based alloy electrocatalysts including PtPd and PtAg carbon-supported in oxygen-depolarized cathode chlor-alkali cell has been shown to have the high cell performance. This study presents application of PtRu carbon supported electrocatalyst oxygen-depolarized cathode and performance comparison of cells with carbon-supported PtRu, PtPd and PtAg electrocatalysts cathodes using the same DSA-Cl2 anode. Results show that there are quite similarity between the effects of various factors on the caustic current efficiency (CCE) in a zero-gap oxygen-depolarized chlor-alkali cells employing carbon-supported PtPd, PtRu and PtAg electrocatalysts. Besides, it seems that the PtPd/C electrocatalyst cathode has relatively higher performance than the other cathodes with PtAg/C and PtRu/C electrocatalysts in zero-gap chlor-alkali cells.
基金supported by the Natural Science Foundation of Shaanxi Province,China(Nos.2023-JC-YB-122,2024JCYBQN-0072)the High-level Innovation and Entrepreneurship Talent Project from Qinchuangyuan of Shaanxi Province,China(No.QCYRCXM-2022-226)+3 种基金the Fundamental Research Funds for the Central Universities,China(No.D5000210987)the Joint Fund Project-Enterprise-Shaanxi Coal Joint Fund Project,China(No.2021JLM-38)the National Natural Science Foundation of China(Grant No.22379123,No.22250710676)the Fujian Province Minjiang Scholar Program,China.
文摘Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of PEMFCs.Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior.In this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail.First,recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed.Then,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively discussed.Finally,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.
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supported by the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2021L574)the Guizhou Provincial Science and Technology Foundation([2024]ZK General 425 and 438)+1 种基金the National Natural Science Foundation of China(22309033)the Academic Young Talent Foundation of Guizhou Normal University([2022]B05 and B06)。
文摘The electron configuration of the active sites can be effectively modulated by regulating the inherent nanostructure of the electrocatalysts,thereby enhancing their electrocatalytic performance.To tackle the unexplored challenge of substantial electrochemical overpotential,surface reconstruction has emerged as a necessary strategy.Focusing on key aspects such as Janus structures,overflow effects,the d-band center displacement hypothesis,and interface coupling related to electrochemical reactions is essential for water electrolysis.Emerging as frontrunners among next-generation electrocatalysts,Mott-Schottky(M-S)catalysts feature a heterojunction formed between a metal and a semiconductor,offering customizable and predictable interfacial synergy.This review offers an in-depth examination of the processes driving the hydrogen and oxygen evolution reactions(HER and OER),highlighting the benefits of employing nanoscale transition metal nitrides,carbides,oxides,and phosphides in M-S heterointerface catalysts.Furthermore,the challenges,limitations,and future prospects of employing M-S heterostructured catalysts for water splitting are thoroughly discussed.
基金supported by the National Natural Science Foundation of China(No.52401284)the Natural Science Foundation of Jiangsu Province(No.BK20240957)+1 种基金the Key Research and Development Program of Nantong(No.GZ2024005)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_3677)。
文摘Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.
基金supported by the Research Fund for International Scientists(RFIS-Grant numbers:52150410410)National Natural Science Foundation of Chinathe Deanship of Scientific Research and Graduate Studies at King Khalid University for funding this research work through Large Research Project under the grant number RGP2/121/1445.
文摘Inspired by molecular catalysts,researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon(M-N-C)to fully utilize metallic sites for 02activation.These catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction(ORR)due to their distinct coordination and electrical structures,Nonetheless,their maximum efficacy in practical applications has yet to be achieved.This agenda identifies tailoring the coordination environment,spin states,intersite distance,and metal-metal interaction as innovative approaches to regulate the ORR performance of these catalysts.However,it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ORR.Therefore,this review aims to analyze recent progress in M-N-C ORR catalysts,emphasizing their innovative engineering with aspects such as alteration in intersite distance,metal-metal interaction,coordination environment,and spin states.Additionally,we critically discuss how to logically monitor the atomic structure,local coordination,spin,and electronic states of M-N-C catalysts to modulate their ORR activity.We have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.
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supported by the National R&D Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(Grant No.RS-2023-0025177 and 2021R1A2B5B01002879)The technology Innovation Program funded by the Ministry of Trade Industry and Energy(MOTIE,Korea)(Grant No.RS-2024-00435432)。
文摘The realization of practical solar hydrogen production relies on the development of efficient devices with nontoxic and low-cost materials.Since the predominant contributors for the performance and cost are the catalyst and the light absorber,it is imperative to develop cost-effective catalysts and absorbers that are compatible with each other for achieving high performance.In this study,a 10%efficient solar-to-hydrogen conversion device was developed through the meticulous integration of low-cost Ni Heazlewoodite-based catalysts for the hydrogen evolution reaction(HER)and ternary bulk heterojunction organic semiconductor(OS)-based light absorbers.Se-incorporated Ni_(3)S_(2)was synthesized using a simple one-step hydrothermal method,which demonstrated a low overpotential and Tafel slope,indicating superior HER activity compared to Ni_(3)S_(2).The theoretical calculation results validate the enhanced HER performance of the Se-incorporated Ni_(3)S_(2)catalyst in alkaline electrolytes.The ternary phase organic light absorber is designed to generate tailored photovoltage and maximized photocurrent,resulting in a photocurrent density of 8.24 mA cm^(-2)under unbiased conditions,which corresponds to 10%solar to hydrogen conversion.Low-temperature photoluminescence spectroscopy results revealed that the enhanced photocurrent density originates from a reduction in both phonon-and vibration-induced inter-and intramolecular non-radiative decay.Our results establish a new benchmark for the emerging OS-based efficient solar hydrogen production based on nontoxic and cost-effective materials.
基金financially supported by the Yancheng Polytechnic College School-Level Scientific Research, China (No. ygy1903)the National Natural Science Foundation of China (Nos. 52001163, 52075237, and 52371157)+2 种基金the Open Project of Taihu Laboratory of Deep-Sea Technology Science, Key Research and Development Plan of Jiangsu Province, China (No. BE2019119)supported by the Priority Academic Program Development of Jiangsu Higher Education Institution (PAPD), Chinathe research funding for the Jiangsu Specially-Appointed Professor Program, China。
文摘Recent advancements in electrocatalysis have highlighted the exceptional application value of amorphous electrocatalysts. Withtheir unique atomic configurations, these electrocatalysts exhibit superior catalytic performance compared to that of their crystalline coun-terparts. Transition metal(TM) amorphous ribbon-shaped electrocatalysts have recently emerged as a new frontier in the catalysis field.Dealloying is widely considered a fascinating method for enhancing the electrocatalyst performance. In this review, we comprehensivelyexamine the principles of water electrolysis, discuss the prevalent methods for fabricating ribbon-configured electrocatalysts, and providean overview of amorphous alloys. Furthermore, we discuss binary, ternary, and high-entropy amorphous TM-based electrocatalysts,which satisfy the requirements necessary for effective water electrolysis. We also propose strategies to enhance the activity of amorphousTM-based ribbons, including morphology control, defect engineering, composition optimization, and heterostructure creation in differentelectrolytes. Our focus extends to the latest developments in the design of heterogeneous micro/nanostructures, management of prepara-tion techniques, and synthesis of different compositions. Finally, we address the ongoing challenges and provide a perspective on the fu-ture development of broadly applicable, self-supporting TM ribbon-shaped electrocatalysts.
基金supported by the National Natural Science Foundation of China(No.52371240)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘The oxygen evolution reaction(OER),a critical half-reaction in water electrolysis,has garnered significant attention.However,sluggish OER kinetics has emerged as a major impediment to efficient electrochemical energy conversion.There is an urgent need to design novel electrocatalysts with optimized OER kinetics and enhanced intrinsic activity to improve overall OER performance.Herein,one-dimensional(1D)nanocomposites with high electrocatalytic activity were developed through the deposition of CoFePBA nanocubes onto the surface of MnO_(2) nanowires.The electronic structure of the nanocomposite surface was modified,and the synergistic effects between transition metals were leveraged to enhance catalytic activity through the deposition of Prussian blue analog(PBA)nanocubes on manganese dioxide nanowires.Specifically,CoFePBA featured an open crystal structure that offiered numerous electrochemical active sites and efficient charge transfer pathways.Additionally,the synergistic interactions between Co and Fe significantly reduced the OER overpotential.Additionally,the 1D rigid MnO_(2) acted as protective armor,ensuring the stability of active sites within CoFePBA during the OER.The synthesized MnO_(2)@CoFePBA achieved an overpotential of 1.614 V at 10 mA/cm^(2) and a small Tafel slope of 94 mV/dec and demonstrated stable performance for over 200 h.This work offers new insights into the rational design of various PBA-based nanocomposites with high activity and stability.
