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Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells

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Frontiers in energy 2024年第2期18卷 206-222页

作者： Cheng YUAN Shiming ZHANG Jiujun ZHANG institute for Sustainable energy/College of Sciences Shanghai UniversityShanghai 200444China

Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading *** on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this *** design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are *** single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the *** advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions

Crystallization management of CsPbI_(2)Br perovskites by PbAc_(2)-incorporated twice spin-coating process for efficient and stable CsPbI_(2)Br perovskite solar cells

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Journal of energy Chemistry 2024年第10期97卷 419-428,I0008页

作者： Yu Liu Kun Lang Huifang Han Huijing Liu Yao Fu Pengchen Zou Yinhui Lyu Jia Xu Jianxi Yao State Key Laboratory of Alternate Electrical Power System with Renewable energy Sources Beijing Key Laboratory of Energy Safety and Clean UtilizationNorth China Electric Power UniversityBeijing 102206China

CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase ***,the presence of bromine leads to a rapid crystallization rate of CsPbI_(2)Br films,resulting in small grain size and high defect ***,CsPbI_(2)Br demonstrates poor light absorption due to its wide ***,it is crucial to control the crystallization rate and increase the film thickness to reduce defect density,enhance light absorption,and improve photovoltaic *** this study,we utilized a PbAc_(2)-incorporated twice spincoating(PTS) process to address these ***,PbAc_(2) was added to the CsPbI_(2)Br precursor solution to form a CsPbI_(2)Br film,which was then coated with the CsPbI_(2)Br precursor solution to produce the PTS film,Ac^(-)can delay the perovskite crystallization,leading to the formation of thicker and denser CsPbI_(2)Br ***,lone-pair electrons of the oxygen atom provided by Ac^(-)formed coordination bonds with under-coordinated Pb~(2+) ions to fill halogen ion vacancies,thereby reducing the defect ***,the PTS CsPbI_(2)Br device achieved a peak power conversion efficiency(PCE) of 16.19% and maintained 96.7% of its initial PCE over 1500 h at room temperature under 25% relative humidity without any encapsulation.

关键词： CsPbI_(2)Br Twice spin-coating process PbAc_(2) Crystallization management Perovskite solar cells

Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic CO_(2) reduction

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Nano Research 2024年第4期17卷 2410-2419页

作者： Weiyi Pan Zhihe Wei Yanhui Su Yuebin Lian Zhangyi Zheng Huihong Yuan Yongze Qin Xulan Xie Qianqian Bai Zhenyang Jiao Wei Hua Jinzhou Chen Wenjun Yang Zhao Deng Yang Peng Soochow institute for energy and Materials Innovations College of EnergySoochow UniversitySuzhou 215006China Key Laboratory of Advanced Carbon Materials and Wearable energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China School of Photoelectric Engineering Changzhou institute of technologyChangzhou 213032China Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China

Assembly of two-dimensional(2D)metal–organic layers(MOLs)based on the hard and soft acid–base theorem represents an exquisite strategy for the construction of photocatalytic platforms in virtue of the highly exposed active sites,much improved mass transport,and greatly elevated ***,nanocages composed of MOLs are produced for the first time through a cosolvent approach utilizing zirconium-based UiO-66-(OH)2 as the structural *** endow the catalytic activity for CO_(2) conversion,single atomic Co^(2+)sites are appended to the Zr-oxo nodes of the MOL cages,demonstrating a remarkable CO yield of 7.74 mmol·g^(-1)·h^(-1) and operational stability of 97.1%product retention after five repeated *** an outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology comprising enormous 2D nanosheets for augmented Co^(2+)exposure and the abundant surface hydroxyl groups for local CO_(2) *** work underlines the tailoring of both metal–organic framework(MOF)morphology and functionality to boost the turnover rate of photocatalytic CO_(2) reduction reaction(CO_(2)RR).

关键词： photocatalytic CO_(2) reduction metal–organic layer nanocage single-atom catalyst co-catalyst

Promoted hydrogenation of CO2 to methanol over single-atom Cu sites with Na+-decorated microenvironment

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National Science Review 2024年第6期11卷 264-272页

作者： Li-Li Ling Xinyu Guan Xiaoshuo Liu Xiao-Mei Lei Zhongyuan Lin Hai-Long Jiang Hefei National Research Center for Physical Sciences at the Microscale Department of Chemistry University of Science and Technology of China School of energy and Power Engineering North China Electric Power University School of energy and Environment Southeast University

Although single-atom Cu sites exhibit high efficiency in CO2hydrogenation to methanol,they are prone to forming Cu nanoparticles due to reduction and aggregation under reaction conditions,especially at high ***,single-atom Cu sites stabilized by adjacent Na+ions have been successfully constructed within a metal-organic framework（MOF）-based catalyst,namely *** is found that the electrostatic interaction between the Na+and Hδ-species plays a pivotal role in upholding the atomic dispersion of Cu in MOF-808-NaCu during CO2hydrogenation,even at temperatures of up to 275℃.This exceptional stabilization effect endows the catalyst with excellent activity(306 g·kgcat-1·h-1),high selectivity to methanol（93%） and long-term stability at elevated reaction temperatures,far surpassing the counterpart in the absence of Na+（denoted as MOF-808-Cu）.This work develops an effective strategy for the fabrication of stable single-atom sites for advanced catalysis by creating an alkali-decorated microenvironment in close proximity.

关键词： single-atom sites metal–organic framework CO2 hydrogenation heterogeneous catalysis alkali-metal decoration

Unraveling the atomic interdiffusion mechanism of NiFe_(2_)O_(4)oxygen carriers during chemical looping CO_(2)conversion

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Carbon energy 2024年第8期6卷 105-121页

作者： Da Song Yan Lin Shiwen Fang Yang Li Kun Zhao Xinfei Chen Zhen Huang Fang He Zengli Zhao Hongyu Huang Fanxing Li Guangzhou institute of energy Conversion Chinese Academy of SciencesGuangzhouChina School of energy Science and Engineering University of Science and Technology of ChinaHefeiChina College of Mechanical and Electrical Engineering Zhongkai University of Agriculture and EngineeringGuangzhouChina College of Chemistry and Bioengineering Guilin University of TechnologyGuilinChina North Carolina State University RaleighNorth CarolinaUSA

By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2)into ***,NiFe_(2_)O_(4)oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2)***,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains ***,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen ***,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4)oxygen carriers during H2 reduction and CO_(2)/lab air oxidation *** discovered that during the H2 reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the *** the CO_(2)splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni *** the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice *** metal atom migration paths depend on the oxygen transfer *** discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen *** work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers.

关键词： chemical looping CO_(2)splitting density functional theory in situ characterization ionic migration

Nanocavity enriched CuPd alloy with high selectivity for CO_(2) electroreduction toward C_(2)H_(4)

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Rare Metals 2024年第4期43卷 1513-1523页

作者： Ze-Yu Zhang Hai-Bin Wang Fei-Fei Zhang Jing-Wei Li Xin-Zhuo Hu Si-Wei Yan Yi-Ming Bai Xun Zhang Gu-Rong Shen Peng-Fei Yin Jing Yang Cun-Ku Dong Jing Mao Hui Liu Xi-Wen Du institute of New-energy Materials School of Materials Science and EngineeringTianjin UniversityTianjin300350China

Electrocatalysis of CO_(2)reduction reaction is an effective way to convert CO_(2)into high value-added products,but the selectivity of Cu-based catalysts for C2+products needs to be improved due to the high energy barrier of C-C ***,a viable catalyst design strategy to decrease energy barrier of C-C coupling should be put ***,a nanocavity-enriched CuPd single atom alloy(CuPd SAA)catalyst is designed to promote CC coupling *** faradaic efficiency of CuPd SAA for ethylene and C_(2+)reaches 75.6%and 85.7%at-0.7 V versus reversible hydrogen electrode(RHE),*** on the results given by in situ characterization,the porous hollow structure dramatically increases the ratio of the linear-bond*CO,thus enhancing the faradaic efficiency for *** functional theory(DFT)calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C-C coupling,further improving the faradaic *** work provides a new idea for designing catalyst with high selectivity for ethylene.

关键词： Adsorption configuration C-C coupling CO_(2) electrocatalysis Ethylene Single atom alloy

Metal-based cathode catalysts for electrocatalytic ORR in microbial fuel cells:A review

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Chinese Chemical Letters 2024年第5期35卷 85-96页

作者： Yaxin Sun Huiyu Li Shiquan Guo Congju Li School of energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China

Microbial fuel cells(MFCs)have a simple structure and excellent pollutant treatment and power generation ***,the slow kinetics of the oxygen reduction reaction(ORR)at the MFC cathode limit power *** electrochemical performance of MFCs can be improved through *** far,metal-based catalysts have shown astonishing results in the field of electrocatalysis,enabling MFC devices to demonstrate power generation capabilities comparable to those of Pt,thus showing enormous *** article reviews the research progress of meta-based MFC cathode ORR catalysts,including the ORR reaction mechanism of MFC,different types of catalysts,and preparation *** catalytic effects of different catalysts in MFC are compared and *** discussing the practical application and expanded manufacturing of catalysts,we summarize the key challenges that must be addressed when using metal-based catalysts in MFC,with the aim of providing a scientific direction for the future development of advanced materials.

关键词： Microbial fuel cells Metal-based cathode catalysts Oxygen reduction reaction Noble metal catalysts MOFs M-N-C Single-atom Transition metal oxides

Single-atom-mediated electron islands boost photocatalytic CO_(2)chemical fixation

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Science china Chemistry 2024年第7期67卷 2292-2299页

作者： Shu Shang Lei Li Xin He Hui Wang Lirong Zheng Wei Shao Xiaodong Zhang Yi Xie Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China institute of energy Hefei Comprehensive National Science CenterHefei 230031China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering Hefei Normal UniversityHefei 230031China

Photocatalytic cycloadditions of CO_(2)with epoxides are emerging as a significant platform for the green synthesis of valuable carbonates,where efficient catalytic systems with spatially separated charge carriers are ***,a single p-block metal atom is proposed to be a candidate for photogenerated electron localization on a metal oxide *** taking the Bi single-atom supported on ZnO nanosheet(Bi1/ZnO)as an example,we show that the Bi atom plays the role of an electron island in the sea of delocalized holes within ***,the as-formed electron island could readily promote the rate-determining ring-opening process of cycloaddition *** from the unique spatially separated electrons and holes,the Bi1/ZnO achieves a high yield of cyclic carbonates with almost 100%*** study provides a pioneering strategy for enhancing the performances of photocatalytic CO_(2)chemical fixation.

关键词： electron islands CO_(2)photofixation photogenerated charge carriers

Electrochemical Oxygen Evolution Performance of Nitrogen-Doped Ultra-Thin Carbon Nanosheets Composite Ru1Co Single atom Alloy Catalysts

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Chinese Journal of Chemistry 2024年第9期42卷 973-979页

作者： Ziwei Deng Zhiyi Sun Yaqiong Li Jiajing Pei Wenxing Chen energy&Catalysis Center Schoolof Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 00049China

energy transformation is imminent,and hydrogen energy is one of the important new energy *** of the keys to increasing the rate of hydrogen evolution during electrolysis is the use of high-performance catalysts for oxygen evolution reactions(OER).Single-atom alloys(SAAs)have garnered significant attention because they partially reduce costs and combine the advantages of both single-atom catalysts(SACs)and alloy ***,an efficient pyrolysis strategy based on a mixing and drying process is designed to anchor ultra-small Co cluster particles,combined with Ru single atoms dispersed on nitrogen-doped ultra-thin carbon nanosheets(Ru_(1)Co SAA/NC).The prepared electrocatalyst exhibits superior OER activity and superb stability,demonstrating an overpotential of 238 mV for OER with a current density of 10 mA·cm^(-2) in 0.5 mol/L H_(2)SO_(4).And we also utilized in-situ XAS to detect the oxidation state of Ru sites during *** in all,this method achieves cost reductions and efficiency improvements through the design of SAAs,offering new prospects for the structural transformation of clean energy.

关键词： Oxygen evolution reaction Single alloy catalyst Ultra-thin carbon nanosheets Electrocatalyst Pyrolysis RuiCo SAA/NC