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Recent progress on mechanisms,principles,and strategies for high-activity and high-stability non-PGM fuel cell catalyst design

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Carbon Energy 2024年第5期6卷 25-52页

作者： Yuping Yuan Yun Zheng Dan Luo Weibin Qiu Jiantao Wang Xin Wang Zhongwei Chen GRINM(Guangdong)Institute of New Materials Technology FoshanChina Department of Chemical Engineering Waterloo Institute for NanotechnologyWaterloo Institute for Sustainable EnergyUniversity of WaterlooWaterlooOntarioCanada Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and Devices School of Information and Optoelectronic Science and EngineeringSouth China Normal UniversityGuangdongChina National Power Battery Innovation Center GRINM Group Co.Ltd.BeijingChina

The commercialization of a polymer membrane H2-O2 fuel cell and its widespread use call for the development of cost-effective oxygen reduction reaction(ORR)nonplatinum group metal(NPGM)catalysts.Nevertheless,to meet the requests for the real-world fuel cell application and replacing platinum catalysts,it still needs to address some challenges for NPGM catalysts regarding the sluggish ORR kinetics in the cathode and their poor durability in acidic environment.In response to these issues,numerous efforts have been made to study NPGM catalysts both theoretically and experimentally,developed these into the atomically dispersed coordinated metal-nitrogen-carbon(M-N-C)form over the past decades.In this review,we present a comprehensive summary of recent advancements on NPGM catalysts with high activity and durability.Catalyst design strategies in terms of optimizing active-site density and enhancing catalyst stability against demetalization and carbon corrosion are highlighted.It is also emphasized the importance of understanding the mechanisms and principles behind those strategies through a combination of theoretical modeling and experimental work.Especially,further understanding the mechanisms related to the active-site structure and the formation process of the single-atom active site under pyrolysis conditions is critical for active-site engineering.Optimizing the active-site distance is the basic principle for improving catalyst activity through increasing the catalyst active-site density.Theoretical studies for the catalyst deactivation mechanism and modeling stable active-site structures provide both mechanisms and principles to improve the NPGM catalyst durability.Finally,currently remained challenges and perspectives in the future on designing high-performance atomically dispersed NPGM catalysts toward fuel cell application are discussed.

关键词： batteries electrocatalysis energy storage and conversion fuel cells

Recent advances in electrocatalytic generation of indole-derived radical cations and their applications in organic synthesis

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Chinese Chemical Letters 2024年第4期35卷 106-123页

作者： Wei Zhou Xi Chen Lin Lu Xian-Rong Song Mu-Jia Luo Qiang Xiao Key Laboratory of Organic Chemistry of Jiangxi Province Jiangxi Science&Technology Normal UniversityNanchang 330013China

Indole-derived radical cations, open-shell reactive species, display distinctive dual reactivity due to the carbon-centered radical and more electrophilic carbocation, which frequently appear in a variety of single electron oxidation reactions for synthesizing structurally diverse functionalized indoles and indolines. electrocatalysis is considered as a synthetically attractive and environmentally friendly alternative for driving the single electron oxidation of indoles. Remarkable achievements in electrocatalytic indolederived radical cation-mediated indole functionalization have been realized so far. This review comprehensively summarizes the recent progresses in the applications of electrocatalytic indole radical cations,including C(sp~2)–H functionalization, dearomative 2,3-difunctionalization, and ring-opening reaction, emphasizing the vital single electron oxidation steps of indoles, the substrates scope and limitations, and the reaction mechanisms.

关键词： electrocatalysis Indole radical cation C-H functionalizatin Dearomative 2 3-difunctionalization

Designing Membrane Electrode Assembly for Electrochemical CO_(2)Reduction:a Review

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Transactions of Tianjin University 2024年第2期30卷 117-129页

作者： Xuerong Wang Shulin Zhao Tao Guo Luyao Yang Qianqian Zhao Yuping Wu Yuhui Chen State Key Laboratory of Materials-Oriented Chemical Engineering and School of Energy Science and EngineeringNanjing Tech UniversityNanjing 211816China Jiangsu Academy of Environmental Industry and Technology Corp Nanjing 210036China

Currently, the electrochemical CO_(2) reduction reaction (CO_(2) RR) can realize the resource conversion of CO_(2) , which is a promising approach to carbon resource use. Important advancements have been made in exploring the CO_(2) RR performance and mechanism because of the rational design of electrolyzer systems, such as H-cells, flow cells, and catalysts. Considering the future development direction of this technology and large-scale application needs, membrane electrode assembly (MEA) systems can improve energy use efficiency and achieve large-scale CO_(2) conversion, which is considered the most promising technology for industrial applications. This review will concentrate on the research progress and present situation of the MEA component structure. This paper begins with the composition and construction of a gas diff usion electrode. Then, the application of ion-exchange membranes in MEA is introduced. Furthermore, the eff ects of pH and the anion and cation of the anolyte on MEA performance are explored. Additionally, we present the anode reaction type in MEA. Finally, the challenges in this field are summarized, and upcoming trends are projected. This review should offer researchers a clearer picture of MEA systems and provide important, timely, and valuable insights into rational electrolyzer design to facilitate further development of CO_(2) electrochemical reduction.

关键词： CO_(2)reduction electrocatalysis Membrane electrode assembly

Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO_(2)reduction

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Nano Research 2024年第6期17卷 4850-4855页

作者： Wenxuan Zhang Mengran Zhang Hongjuan Wang Wen Zhang Min Zhang MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion School of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China

Double-site catalysts have attracted widespread attention in the field of electrocatalysis due to their high metal loading,adjustable active centres,and electronic valence states.However,the development of bimetallic sites catalysts that coordinate with definite atoms is still in the exploratory stage.Here,we designed and synthesized a bimetallic palladium complex(BPB-Pd_(2))with conjugated backbone.The supported BPB-Pd_(2)was applied to electrochemical CO_(2)reduction reaction(CO_(2)RR)for the first time.The as-obtained BPB-Pd_(2)gives an exceptional Faradaic efficiency of CO(FECO)of 94.4%at−0.80 V vs.reversible hydrogen electrode(RHE),which is significantly superior to monoatomic palladium catalyst(BPB-Pd1).The density functional theory(DFT)calculations revealed that the essential reason for the outstanding activity of BPB-Pd_(2)toward CO_(2)RR was that the electronic effect between diatomic palladium reduces the free energy change for CO_(2)RR process.Thus,BPB-Pd_(2)exhibits moderate free energy change to form COOH*intermediate,which was beneficial for the generation of CO in CO_(2)RR.

关键词： synthesis electrocatalysis CO_(2)reduction bimetallic palladium complex synergistic catalysis

Coupling Co-Ni phosphides for energy-saving alkaline seawater splitting

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Nano Research 2024年第6期17卷 4797-4806页

作者： Weijia Liu Wenxian Liu Tong Hou Junyang Ding Zhigui Wang Ruilian Yin Xingyuan San Ligang Feng Jun Luo Xijun Liu State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Nonferrous Metals and Featured MaterialsMOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Hebei Key Laboratory of Optic-electronic Information and Materials the College of Physics Science and TechnologyHebei UniversityBaoding 071002China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion issues.However,the fabrication of efficient multifunctional catalysts for this promising technology is of great challenge.Herein,a heterostructured catalyst comprising CoP and Ni_(2)P on nickel foam(CoP/Ni_(2)P@NF)is reported for hydrazine oxidation(HzOR)-assisted alkaline seawater splitting.The coupling of CoP and Ni_(2)P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and HER.Impressively,the two-electrode HzOR-assisted alkaline seawater splitting(OHzS)cell based on the CoP/Ni_(2)P@NF required only 0.108 V to deliver 100 mA·cm^(−2),much lower than 1.695 V for alkaline seawater electrolysis cells.Moreover,the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm^(−2).Furthermore,the CoP/Ni_(2)P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation,methanol oxidation,and urea oxidation in alkaline seawater electrolytes.This work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H_(2) production.

关键词： seawater splitting heterostructure electrocatalysis hydrazine oxidation reaction hydrogen evolution reaction

Electrospinning-derived functional carbon-based materials for energy conversion and storage

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Chinese Chemical Letters 2024年第6期35卷 3-13页

作者： Xinyu Ren Hong Liu Jingang Wang Jiayuan Yu Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringUniversity of JinanJi’nan 250022China State Key Laboratory of Crystal Materials Shandong UniversityJi’nan 250100China

The over-exploitation of fossil fuel energy has brought about serious environmental problems.It would be of great significance to construct efficient energy conversion and storage system to maximize utilize renewable energy,which contributes to reducing environmental hazards.For the past few years,in terms of electrocatalysis and energy storage,carbon fiber materials show great advantages due to its outstanding electrical conductivity,good flexibility and mechanical property.As a simple and low-cost technique,electrospinning can be employed to prepare various nanofibers.It is noted that the functional fiber materials with different special structure and composition can be obtained for energy conversion and storage by combining electrospinning with other post-processing.In this paper,the structural design,controllable synthesis and multifunctional applications of electrospinning-derived functional carbon-based materials(EFCMs)is reviewed.Firstly,we briefly introduce the history,basic principle and typical equipment of electrospinning.Then we discuss the strategies for preparing EFCMs with different structures and composition in detail.In addition,we show recently the application of advanced EFCMs in energy conversion and storage,such as nitrogen species reduction reaction,CO_(2) reduction reaction,oxygen reduction reaction,water-splitting,supercapacitors and ion batteries.In the end,we propose some perspectives on the future development direction of EFCMs.

关键词： Electrospinning Carbon materials Functional fiber Energy conversion Energy storage electrocatalysis

Boosted Electrocatalytic Glucose Oxidation Reaction on Noble-Metal-Free MoO_(3)-Decorated Carbon Nanotubes

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Transactions of Tianjin University 2024年第1期30卷 63-73页

作者： Yu-Long Men Ning Dou Yiyi Zhao Yan Huang Lei Zhang Peng Liu Department of Chemical Engineering School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Thyroid Breast and Vascular Surgery Shanghai Fourth People’s Hospital Affi liated to Tongji University School of MedicineShanghai 200081China Department of Vascular Surgery Changhai HospitalNaval Medical UniversityShanghai 200433China

Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells.

关键词： Interface eff ect electrocatalysis Molybdenum oxide Glucose Oxidation reaction

Unveiling the intrinsic properties of single NiZnFeO_x entity for promoting electrocatalytic oxygen evolution

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Chinese Chemical Letters 2024年第4期35卷 181-186页

作者： Zhihao Gu Jiabo Le Hehe Wei Zehui Sun Mahmoud Elsayed Hafez Wei Ma Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201China Department of Chemistry Faculty of ScienceBeni-Suef UniversityBeni-Suef 62511Egypt

Although considerable research efforts have been devoted to the design and development of non-noble electrocatalysts for oxygen evolution reaction(OER), substantial enhancement of OER performance with commercial-scale water electrolysis remains a big challenge. This could result from the difficulties in detecting the intrinsic properties and overlooking the assembly process for electrochemical OER process. Here, we employ a microjet collision method to investigate the intrinsic OER activities of individual NiZnFeO_x entities with and without a moderate magnetic field. Our results demonstrate that single NiZnFeO_x nanoparticles(NPs) show the excellent OER performance with a lowest onset potential(~1.35 V vs. RHE) and a greatest magnetic enhancement(~118%) among bulk materials, single agglomerations and NPs. Furthermore, we explore the utility of theoretical investigation by density functional theory(DFT)calculations for studying OER process on NiZnFeO_x surfaces without and with spin alignment, indicating monodispersed NiZnFeO_xNPs with totally spin alignment facilitates the OER process under the external magnetic field. It is found that the well-dispersion of NiZnFeO_x NPs would increase the electrical conductivity and the surface spin state, resulting in promoting their OER activities. This work provides a test for uncovering the essential roles of NPs assembly to a significant promotion of their magnet-assisted OER.

关键词： Single entity OER Magnetic enhancement electrocatalysis Well-dispersion

Charge-asymmetry Fe_(1)Cu single-atom alloy catalyst for efficient oxygen reduction reaction

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Nano Research 2024年第6期17卷 4702-4710页

作者： Xudong Niu Jian Wei Dongyao Xu Jiajing Pei Rui Sui School of Chemical&Environmental Engineering China University of Mining and TechnologyBeijing 100083China Institute of Water Ecology and Environment Chinese Research Academy of Environmental SciencesBeijing 100083China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084China

The development of high-efficient and low-cost oxygen reduction reaction(ORR)electrocatalysts is crucial for the practical applications of metal-air batteries.One promising way is to develop Fe single-atom catalysts.However,the single active center and inherent electronic structure of Fe single-atom catalysts lead to the undesirable adsorption of multiple ORR intermediates.Herein,a charge-asymmetry single-atom alloy(SAA)catalyst with Fe-Cu dual sites supported on nitrogen-doped carbon nanosheet(Fe_(1)Cu SAA/NC)was constructed.Various characterizations manifest the existence of electron interaction between Fe and Cu in Fe_(1)Cu SAA/NC,which facilitates the adsorption of ORR intermediate for fast kinetics.Consequently,the charge-asymmetry Fe_(1)Cu SAA/NC exhibits much faster ORR kinetics with a half-wave potential of 0.917 V vs.reversible hydrogen electrode(RHE),outperforming its counterparts in the references.Furthermore,Fe_(1)Cu SAA/NC still maintains a high half-wave potential with only a drop of 5 mV after 5000 cycles,indicating excellent stability.This work provides a new strategy to design highly active and non-noble metal ORR electrocatalysts,which hold great potential for various catalytic applications.

关键词： Fe_(1)Cu single-atom alloy(SAA) electrocatalysis oxygen reduction reaction charge-asymmetry