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Converting CO_(2)to ethanol on Ag nanowires with high selectivity investigated by operando Raman spectroscopy

Science China Chemistry 2023年第1期66卷 259-265页

作者： Qiong Liu Xia-Guang Zhang Zi-Yu Du Can-Jun Zou Huan-Yu Chen Yu Zhao Jin-Chao Dong Ping-Ping Fang Jian-Feng Li MOE Key Laboratory of Bioinorganic and Synthetic Chemistry The Key Lab of Low-carbon Chem&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China State Key Laboratory of Physical Chemistry of Solid Surfaces iChEMCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsState Key College of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Electrochemical conversion of CO_(2)into liquid fuels provides an efficient way to store the renewable energy in the production of fuels and chemicals.However,effectively converting CO_(2)to ethanol remains extremely challenging due to the low activity and selectivity.Herein,we achieve a high ethanol Faradaic efficiency(FE)as high as 85%on Ag nanowires(NWs)for CO_(2)electroreduction at-0.95 V.X-ray photoelectron spectroscopy and electrochemical experiments prove that such Ag NWs are partially oxidized.operando Raman spectroscopy finds the important CO intermediate adsorbed on partially oxidized Ag NWs,facilitating the ethanol formation.Density functional theory calculations prove that the reaction energy of CO coupling with the*CHO to*COCHO intermediate on the partially oxidized Ag NWs is smaller than that on the surface of Cu,which explains why the ethanol FE of such partially oxidized Ag NWs can exceed that of Cu,and therefore is the most favorable pathway for the formation of C_(2)products on partially oxidized Ag NWs.This study provides a new insight to design efficient catalysts and investigate the mechanisms to improve the selectivity.

关键词： surface-enhanced Raman spectroscopy CO_(2)electroreduction electrocatalysis Operando spectroscopy ethanol

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In situ and operando infrared spectroscopy of battery systems:Progress and opportunities

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能源化学:英文版 2023年第6期81卷 472-491,I0011页

作者： Murilo M.Amaral Carla G.Real Victor Y.Yukuhiro Gustavo Doubek Pablo S.Fernandez Gurpreet Singh Hudson Zanin Advanced Energy Storage Division Center for Innovation on New EnergiesSchool of Electrical and Computer EngineeringUniversity of CampinasCampinasSP 13083-852Brazil Alan Levin Department of Mechanical and Nuclear Engineering Kansas State UniversityManhattanKS 66506USA Chemistry Institute Center for Innovation on New EnergiesUniversity of CampinasCampinasSP 13083-970Brazil Advanced Energy Storage Division Center for Innovation on New EnergiesSchool of Chemical EngineeringUniversity of CampinasCampinasSP 13083-852Brazil

In situ and operando infrared spectroscopies are powerful techniques to support the design of novel materials for batteries and the development of new battery systems.These techniques can support the study of batteries by identifying the formation of new species and monitoring electrochemical energy stability.However,few works have employed these techniques,which can be used to investigate various materials,including systems beyond lithium-ion technology,in the research of batteries.Therefore,this review presents a comprehensive overview focusing on the main contributions of in situ and operando infrared spectroscopy for lithium-ion batteries(LIBs)and other battery systems.These techniques can successfully identify the formation of species during the electrolyte reduction,electrode degradation,and the formation of the solid-electrolyte interphase(SEI)layer.From these outcomes,it is possible to conclude that this characterization approach should be employed as a protocol to overcome remaining issues in batteries,consequently supporting battery research.This review aims to be a guide on how infrared spectroscopy can contribute to monitoring battery systems and to lead researchers interested in applying this technique.

关键词： In situ spectroscopy Operando spectroscopy FTIR Spectro-electrochemical cells Batteries

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Electrocatalytic water splitting:Mechanism and electrocatalyst design

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Nano Research 2023年第7期16卷 9142-9157页

作者： Han Wu Qiaoxian Huang Yuanyuan Shi Jiangwei Chang Siyu Lu Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China

Hydrogen energy,a new type of clean and efficient energy,has assumed precedence in decarbonizing and building a sustainable carbon-neutral economy.Recently,hydrogen production from water splitting has seen considerable advancements owing to its advantages such as zero carbon emissions,safety,and high product purity.To overcome the large energy barrier and high cost of water splitting,numerous efficient electrocatalysts have been designed and reported.However,various difficulties in promoting the industrialization of electrocatalytic water splitting remain.Further,as high-performance electrocatalysts that satisfy industrial requirements are urgently needed,a better understanding of water-splitting systems is required.In this paper,the latest progress in water electrolysis is reviewed,and experimental evidence from in situ/operando spectroscopic surveys and computational analyses is summarized to present a mechanistic understanding of hydrogen and oxygen evolution reactions.Furthermore,some promising strategies,including alloying,morphological engineering,interface construction,defect engineering,and strain engineering for designing and synthesizing electrocatalysts are highlighted.We believe that this review will provide a knowledge-guided design in fundamental science and further inspire technical engineering developments for constructing efficient electrocatalysts for water splitting.

关键词： water splitting mechanism Operando spectroscopy design strategy

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Investigating Why Sulfurization Can Greatly Improve Ethanol Selectivity for Carbon Dioxide Electroreduction

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CCS Chemistry 2022年第10期4卷 3319-3328页

作者： Qian-Yu Wang Yu-Hang Li Yu Zhao Yu-Yu Chen Bi-Jun Geng Rong-Kai Ye Qiong Liu Xiao-Qing Liu Ye-Xiang Tong Yue-Jiao Zhang Jun Cheng Ping-Ping Fang Jian-Qiang Hu Jian-Feng Li Zhong-Qun Tian MOE of the Key Laboratory of Bioinorganic and Synthetic Chemistry The Key Laboratory of Low-Carbon Chem&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275 Department Key Laboratory of Fuel Cell Technology of Guangdong Province Nanobiological Medicine CenterSchool of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640 State Key Laboratory of Physical Chemistry of Solid Surfaces iChEMCollege of Chemistry and Chemical EngineeringCollege of EnergyXiamen UniversityXiamen 361005

Carbon dioxide(CO_(2))electroreduction of products using renewable electricity sources is a promising avenue for chemical energy storage that is attracting increasing attention.Considerable effort has been focused on improving the activity and selectivity for CO_(2)electroreduction of C2+products,especially for ethanol.However,studies of this process’s underlying mechanism are still lacking.

关键词： surface-enhanced Raman spectroscopy CO_(2)electroreduction electrocatalysis Operando spectroscopy mechanisms

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