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
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
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
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
Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts...Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts has been ruled out,the impact of trace metal contamination during electrochemical activation remains unexplored.This study demonstrates that anodic pretreatment in alkaline electrolytes enhances the catalytic performance of carbon cloth.Specifically,carbon cloth activated in 8 mol/L Na OH achieves a current density of 10 m A/cm^(2)with an overpotential of only 338 m V,comparable to metalbased OER catalysts.Electrochemical and spectroscopic analyses show the deposition of Fe Ni O_(x)H_(y)oxyhydroxides(0.19±0.06μg/cm^(2))on specific sites of the carbon substrate during activation.These nanoparticles contribute significantly to the catalytic activity,with a synergistic effect between Fe Ni O_(x)H_(y)and the carbon substrate.The turnover frequency(TOF)for Fe correlates with the amount of C=O groups on the carbon substrate,providing evidence for an interfacial synergistic effect.This work emphasizes the importance of considering trace metal effects in metal-free catalyst evaluation and offers insights for the design of more efficient carbon-based hybrid OER catalysts.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
Hydrogen is widely regarded as a crucial energy carrier for achieving carbon neutrality and a sustainable future.Direct seawater electrolysis using renewable energy presents a promising approach for large-scale hydrog...Hydrogen is widely regarded as a crucial energy carrier for achieving carbon neutrality and a sustainable future.Direct seawater electrolysis using renewable energy presents a promising approach for large-scale hydrogen production.Reactions of this nature at high current density and Faradaic efficiency are hampered by two challenges.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
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
Proton exchange membrane water electrolyzer(PEMWE)is crucial for the storage and conversion of renewable energy.However,the harsh anode environment and the oxygen evolution reaction(OER),which involves a four-electron...Proton exchange membrane water electrolyzer(PEMWE)is crucial for the storage and conversion of renewable energy.However,the harsh anode environment and the oxygen evolution reaction(OER),which involves a four-electron transfer,result in a significant overpotential that limits the overall efficiency of hydrogen production.Identifying active sites in the OER is crucial for understanding the reaction mechanism and guiding the development of novel electrocatalysts with high activity,cost-effectiveness,and durability.Herein,we summarize the widely accepted OER mechanism in acidic media,in situ characterization and monitoring of active sites during the reaction,and provide a general understanding of the active sites on various catalysts in the OER,including Ir-based metals,Ir-based oxides,carbon/oxide-supported Ir,Ir-based perovskite oxides,and Ir-based pyrochlore oxides.For each type of electrocatalysts,reaction pathways and actual active sites are proposed based on in situ characterization techniques and theoretical calculations.Finally,the challenges and strategic research directions associated with the design of highly efficient Ir-based electrocatalysts are discussed,offering new insights for the further scientific advancement and practical application of acidic OER.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
Water electrolysis using renewable electricity is a promising strategy for high-purity hydrogen production.To realize the practical application of water electrolysis,an electrocatalyst with high redox properties and l...Water electrolysis using renewable electricity is a promising strategy for high-purity hydrogen production.To realize the practical application of water electrolysis,an electrocatalyst with high redox properties and low cost is essential for enhancing the sluggish oxygen evolution reaction.Herein,we fabricated Fe-doped nickel oxalate(Fe-NiC_(2)O_(4))directly grown on nickel(Ni)foam as an efficient electrocatalyst for the alkaline oxygen evolution reaction using a facile one-step hydrothermal method.Fe-NiC_(2)O_(4) served as a precursor for obtaining highly active Fe-doped Ni oxyhydroxide(Fe-NiOOH)via in situ electrochemical oxidation.Consequently,0.75Fe-NiOOH was demonstrated to be the optimal electrocatalyst,exhibiting outstanding oxygen evolution reaction activity with a low overpotential of 220 mV at a current density of 100 mA cm^(-2) and a Tafel slope of 20.5 mV dec^(-1).Furthermore,Fe-NiOOH maintained its oxygen evolution reaction activity without performance decay during long-term electrochemical measurements,owing to the phase transformation from nickel oxyhydroxide(NiOOH)toγ-NiOOH(gamma nickel oxyhydroxide).These performances significantly surpass those of recently reported transition-metal-based electrocatalysts.展开更多
High entropy materials(HEMs)show great potential as electrocatalysts for oxygen evolution reaction(OER)thanks to their interesting four-core effect.This paper presents the first systematic summary of the key factors i...High entropy materials(HEMs)show great potential as electrocatalysts for oxygen evolution reaction(OER)thanks to their interesting four-core effect.This paper presents the first systematic summary of the key factors in the synthetic methods and their influence on the structure and OER properties of HEMs(including complexing agent,synthetic temperature,and calcination atmosphere).Optimizing the components of high entropy alloys and compounds by introducing heteroatoms(such as O,S,P,N,C,and B)can enhance the chemical configurations of active sites and thus enhance the intrinsic OER kinetics.In addition,this paper emphasizes the importance of the electrocatalytic influence mechanism of the four-core effects(including the high entropy effect,lattice distortion effect,cocktail effect and sluggish diffusion effect)on catalyst structure and their OER performance.Finally,we outline the current challenges and future development directions,aiming to offer crucial insights for creating economical and efficient HEM-based electrocatalysts in the OER field.展开更多
Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)...Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)presents an encouraging alternative marked by mild reaction conditions,rapid reaction rates,and minimal byproduct pollution,successfully overcoming the challenges of the energy-intensive Haber-Bosch process.Recent innovations in two-dimensional(2D)electrocatalysts have emerged as a promising approach to enhance the efficiency and selectivity of this transformation.This review systematically examines the latest advancements in2D materials,including metals,metal compounds,nonmetallic elements,and organic frameworks,highlighting their unique electronic properties and high surface area that facilitate the electrocatalytic reactions.We explore strategies to optimize these catalysts,such as doping,heterostructure,and surface functionalization,which have shown significant improvements in catalytic performance.Furthermore,the role of in situ/operando characterization techniques in understanding the reaction mechanisms is highlighted,aiming to provide both theoretical and practical insights for the research and development of 2D nanoelectrocatalysts during eNRA.Additionally,future perspectives and ongoing challenges are discussed to offer insights for transitioning from experimental investigations to real-world applications.展开更多
The selective reduction of carbon dioxide(CO_(2))into high-value-added chemicals is one of the most effective means to solve the current energy and environmental problems,which could realize the utilization of CO_(2) ...The selective reduction of carbon dioxide(CO_(2))into high-value-added chemicals is one of the most effective means to solve the current energy and environmental problems,which could realize the utilization of CO_(2) and promote the balance of the carbon cycle.Formate is one of the most economical and practical products of all the electrochemical CO_(2) reduction products.Among the many metal-based electrocatalysts that can convert CO_(2) into formate,Sn-based catalysts have received a lot of attention because of their low-cost,non-toxic characteristics and high selectivity for formate.In this article,the most recent development of Sn-based electrocatalysts is comprehensively summarized by giving examples,which are mainly divided into monometallic Sn,alloyed Sn,Sn-based compounds and Sn composite catalysts.Finally,the current performance enhancement strategies and future directions of the field are summarized.展开更多
Electrochemical reduction reactions,including the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CRR),and nitrate reduction reaction(NRR),hold promise for energy conv...Electrochemical reduction reactions,including the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CRR),and nitrate reduction reaction(NRR),hold promise for energy conversion and storage.However,electrocatalysts exhibit slow kinetics and inactivation effects,resulting in inadequate energy efficiency and poor stability.To address these challenges,the groupⅧelement-based single-atom electrocatalysts(GVSAEs)were endowed with tunable electronic structures and porous carbon substrates to reduce intermediate adsorption and desorption energy barriers,which can accelerate electrochemical kinetics.This mini review summarises the recent achievements in GVSAEs with electronic structure and porous substrate engineering discussions.Furthermore,these GVSAEs are divided into non-noble iron series element(Fe,Co,and Ni)single-atom electrocatalysts and noble platinum series elements(Ru,Rh,Pd,Os,Ir,and Pt)based single-atom electrocatalysts for the ORR,HER,CRR,and NRR,where the porous substrate structure,electronic structure,and catalytic activity are discussed.Finally,conclusions and perspectives relating to future challenges and potential opportunities are provided for electrocatalysis with better performance.展开更多
Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains...Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains a great challenge to avoid the inhomogeneous distribution and aggregation of metal single-atomic active centers in the construction of bifunctional electrocatalysts with atomically dispersed multimetallic sites because of the common calcination method.Herein,we report a novel catalyst with phthalocyanine-assembled Fe-Co-Ni single-atomic triple sites dispersed on sulfur-doped graphene using a simple ultrasonic procedure without calcination,and X-ray absorption fine structure(XAFS),aberration-corrected scanning transmission electron microscopy(AC-STEM),and other detailed characterizations are performed to demonstrate the successful synthesis.The novel catalyst shows extraordinary bifunctional ORR/OER activities with a fairly low potential difference(ΔE=0.621 V)between the OER overpotential(Ej10=315 mV at 10 m A cm^(-2))and the ORR half-wave potential(Ehalf-wave=0.924 V).Moreover,the above catalyst shows excellent ZAB performance,with an outstanding specific capacity(786 mAh g^(-1)),noteworthy maximum power density(139 mW cm^(-2)),and extraordinary rechargeability(discharged and charged at 5 mA cm^(-2) for more than 1000 h).Theoretical calculations reveal the vital importance of the preferable synergetic coupling effect between adjacent active sites in the Fe-Co-Ni trimetallic single-atomic sites during the ORR/OER processes.This study provides a new avenue for the investigation of bifunctional electrocatalysts with atomically dispersed trimetallic sites,which is intended for enhancing the ORR/OER performance in ZABs.展开更多
Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses...Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.展开更多
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 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financially supported by the National Natural Science Foundation of China(No.22479097)the Shanghai Science and Technology Committee(Nos.23ZR1433000 and 22511100400)+1 种基金the National High-Level Talent Program for Young Scholarsthe Start-up Fund(F.Song)from Shanghai Jiao Tong University。
文摘Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts has been ruled out,the impact of trace metal contamination during electrochemical activation remains unexplored.This study demonstrates that anodic pretreatment in alkaline electrolytes enhances the catalytic performance of carbon cloth.Specifically,carbon cloth activated in 8 mol/L Na OH achieves a current density of 10 m A/cm^(2)with an overpotential of only 338 m V,comparable to metalbased OER catalysts.Electrochemical and spectroscopic analyses show the deposition of Fe Ni O_(x)H_(y)oxyhydroxides(0.19±0.06μg/cm^(2))on specific sites of the carbon substrate during activation.These nanoparticles contribute significantly to the catalytic activity,with a synergistic effect between Fe Ni O_(x)H_(y)and the carbon substrate.The turnover frequency(TOF)for Fe correlates with the amount of C=O groups on the carbon substrate,providing evidence for an interfacial synergistic effect.This work emphasizes the importance of considering trace metal effects in metal-free catalyst evaluation and offers insights for the design of more efficient carbon-based hybrid OER catalysts.
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.
文摘Hydrogen is widely regarded as a crucial energy carrier for achieving carbon neutrality and a sustainable future.Direct seawater electrolysis using renewable energy presents a promising approach for large-scale hydrogen production.Reactions of this nature at high current density and Faradaic efficiency are hampered by two challenges.
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.
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 Henan Province Science and Technology Research Project(Grant No.242103810058)Natural Science Foundation of Henan(Grant No.252300421104)+3 种基金National Natural Science Foundation of China(Grant No.52102346)Henan Key Research and Development Project(Grant No.231111230100)Heluo Youth Talent Project(Grant No.2024HLTJ14)Henan Postdoctoral Research Initiation Project(Grant No.HN2022040 and HN2022048).
文摘Proton exchange membrane water electrolyzer(PEMWE)is crucial for the storage and conversion of renewable energy.However,the harsh anode environment and the oxygen evolution reaction(OER),which involves a four-electron transfer,result in a significant overpotential that limits the overall efficiency of hydrogen production.Identifying active sites in the OER is crucial for understanding the reaction mechanism and guiding the development of novel electrocatalysts with high activity,cost-effectiveness,and durability.Herein,we summarize the widely accepted OER mechanism in acidic media,in situ characterization and monitoring of active sites during the reaction,and provide a general understanding of the active sites on various catalysts in the OER,including Ir-based metals,Ir-based oxides,carbon/oxide-supported Ir,Ir-based perovskite oxides,and Ir-based pyrochlore oxides.For each type of electrocatalysts,reaction pathways and actual active sites are proposed based on in situ characterization techniques and theoretical calculations.Finally,the challenges and strategic research directions associated with the design of highly efficient Ir-based electrocatalysts are discussed,offering new insights for the further scientific advancement and practical application of acidic OER.
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.
基金supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)(No.20213030040590)the Korea Institute for Advancement of Technology(KIAT)and the Ministry of Trade,Industry&Energy(MOTIE),Republic of Korea(No.P0022130)Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2021R1A6C101A404)。
文摘Water electrolysis using renewable electricity is a promising strategy for high-purity hydrogen production.To realize the practical application of water electrolysis,an electrocatalyst with high redox properties and low cost is essential for enhancing the sluggish oxygen evolution reaction.Herein,we fabricated Fe-doped nickel oxalate(Fe-NiC_(2)O_(4))directly grown on nickel(Ni)foam as an efficient electrocatalyst for the alkaline oxygen evolution reaction using a facile one-step hydrothermal method.Fe-NiC_(2)O_(4) served as a precursor for obtaining highly active Fe-doped Ni oxyhydroxide(Fe-NiOOH)via in situ electrochemical oxidation.Consequently,0.75Fe-NiOOH was demonstrated to be the optimal electrocatalyst,exhibiting outstanding oxygen evolution reaction activity with a low overpotential of 220 mV at a current density of 100 mA cm^(-2) and a Tafel slope of 20.5 mV dec^(-1).Furthermore,Fe-NiOOH maintained its oxygen evolution reaction activity without performance decay during long-term electrochemical measurements,owing to the phase transformation from nickel oxyhydroxide(NiOOH)toγ-NiOOH(gamma nickel oxyhydroxide).These performances significantly surpass those of recently reported transition-metal-based electrocatalysts.
基金supported by the National Natural Science Foundation of China(52103342 and 22209032)the Scientific Research Fund of Zhejiang Provincial Education Department(Y202456353)。
文摘High entropy materials(HEMs)show great potential as electrocatalysts for oxygen evolution reaction(OER)thanks to their interesting four-core effect.This paper presents the first systematic summary of the key factors in the synthetic methods and their influence on the structure and OER properties of HEMs(including complexing agent,synthetic temperature,and calcination atmosphere).Optimizing the components of high entropy alloys and compounds by introducing heteroatoms(such as O,S,P,N,C,and B)can enhance the chemical configurations of active sites and thus enhance the intrinsic OER kinetics.In addition,this paper emphasizes the importance of the electrocatalytic influence mechanism of the four-core effects(including the high entropy effect,lattice distortion effect,cocktail effect and sluggish diffusion effect)on catalyst structure and their OER performance.Finally,we outline the current challenges and future development directions,aiming to offer crucial insights for creating economical and efficient HEM-based electrocatalysts in the OER field.
基金supported by the National Natural Science Foundation of China(Nos.52172291,52122312,and 52473294)'Shuguang Program'supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.22SG31)the State Key Laboratory for Advanced Fiber Materials,Donghua University
文摘Excessive nitrogen emission caused by human activities has significantly disrupted the global nitrogen cycle,adversely affecting ecosystems and human health.Electrocatalytic nitrate reduction to valuable ammonia(eNRA)presents an encouraging alternative marked by mild reaction conditions,rapid reaction rates,and minimal byproduct pollution,successfully overcoming the challenges of the energy-intensive Haber-Bosch process.Recent innovations in two-dimensional(2D)electrocatalysts have emerged as a promising approach to enhance the efficiency and selectivity of this transformation.This review systematically examines the latest advancements in2D materials,including metals,metal compounds,nonmetallic elements,and organic frameworks,highlighting their unique electronic properties and high surface area that facilitate the electrocatalytic reactions.We explore strategies to optimize these catalysts,such as doping,heterostructure,and surface functionalization,which have shown significant improvements in catalytic performance.Furthermore,the role of in situ/operando characterization techniques in understanding the reaction mechanisms is highlighted,aiming to provide both theoretical and practical insights for the research and development of 2D nanoelectrocatalysts during eNRA.Additionally,future perspectives and ongoing challenges are discussed to offer insights for transitioning from experimental investigations to real-world applications.
基金Project(52204378)supported by the National Natural Science Foundation of China。
文摘The selective reduction of carbon dioxide(CO_(2))into high-value-added chemicals is one of the most effective means to solve the current energy and environmental problems,which could realize the utilization of CO_(2) and promote the balance of the carbon cycle.Formate is one of the most economical and practical products of all the electrochemical CO_(2) reduction products.Among the many metal-based electrocatalysts that can convert CO_(2) into formate,Sn-based catalysts have received a lot of attention because of their low-cost,non-toxic characteristics and high selectivity for formate.In this article,the most recent development of Sn-based electrocatalysts is comprehensively summarized by giving examples,which are mainly divided into monometallic Sn,alloyed Sn,Sn-based compounds and Sn composite catalysts.Finally,the current performance enhancement strategies and future directions of the field are summarized.
基金supported by the National Natural Science Foundation of China-Yunnan Joint Fund(No.U2002213)the Science and Technology Talent and Platform Program of Yunnan Provincial Science and Technology Department(No.202305AM070001)+1 种基金Open Foundation of Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials(No.2022GXYSOF10)Double First University Plan(No.C176220100042)
文摘Electrochemical reduction reactions,including the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CRR),and nitrate reduction reaction(NRR),hold promise for energy conversion and storage.However,electrocatalysts exhibit slow kinetics and inactivation effects,resulting in inadequate energy efficiency and poor stability.To address these challenges,the groupⅧelement-based single-atom electrocatalysts(GVSAEs)were endowed with tunable electronic structures and porous carbon substrates to reduce intermediate adsorption and desorption energy barriers,which can accelerate electrochemical kinetics.This mini review summarises the recent achievements in GVSAEs with electronic structure and porous substrate engineering discussions.Furthermore,these GVSAEs are divided into non-noble iron series element(Fe,Co,and Ni)single-atom electrocatalysts and noble platinum series elements(Ru,Rh,Pd,Os,Ir,and Pt)based single-atom electrocatalysts for the ORR,HER,CRR,and NRR,where the porous substrate structure,electronic structure,and catalytic activity are discussed.Finally,conclusions and perspectives relating to future challenges and potential opportunities are provided for electrocatalysis with better performance.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22305071,52472200,52271176,and52072114)the 111 Project(Grant No.D17007)+3 种基金Henan Center for Outstanding Overseas Scientists(Grant No.GZS2022017)the China Postdoctoral Science Foundation(Grant No.2022M721049)the Henan Province Key Research and Development Project(Grant No.231111520500)the Natural Science Foundation of Henan Province(Grant No.252300421556)。
文摘Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains a great challenge to avoid the inhomogeneous distribution and aggregation of metal single-atomic active centers in the construction of bifunctional electrocatalysts with atomically dispersed multimetallic sites because of the common calcination method.Herein,we report a novel catalyst with phthalocyanine-assembled Fe-Co-Ni single-atomic triple sites dispersed on sulfur-doped graphene using a simple ultrasonic procedure without calcination,and X-ray absorption fine structure(XAFS),aberration-corrected scanning transmission electron microscopy(AC-STEM),and other detailed characterizations are performed to demonstrate the successful synthesis.The novel catalyst shows extraordinary bifunctional ORR/OER activities with a fairly low potential difference(ΔE=0.621 V)between the OER overpotential(Ej10=315 mV at 10 m A cm^(-2))and the ORR half-wave potential(Ehalf-wave=0.924 V).Moreover,the above catalyst shows excellent ZAB performance,with an outstanding specific capacity(786 mAh g^(-1)),noteworthy maximum power density(139 mW cm^(-2)),and extraordinary rechargeability(discharged and charged at 5 mA cm^(-2) for more than 1000 h).Theoretical calculations reveal the vital importance of the preferable synergetic coupling effect between adjacent active sites in the Fe-Co-Ni trimetallic single-atomic sites during the ORR/OER processes.This study provides a new avenue for the investigation of bifunctional electrocatalysts with atomically dispersed trimetallic sites,which is intended for enhancing the ORR/OER performance in ZABs.
基金funding from the Hellenic Foundation for Research and Innovation(HFRI)under grant agreement No 3655.
文摘Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.
