{"title":"In Situ Oxygen-Vacancy Engineering for Enhancing CO2 Reduction Activity","authors":"Jianing Mao, Bingbao Mei*, Shuai Yang, Jianrong Zeng, Fanfei Sun, Wei Chen, Fei Song* and Zheng Jiang*, ","doi":"10.1021/acsmaterialslett.4c01776","DOIUrl":null,"url":null,"abstract":"<p >Bulk metallic oxides with abundant surface oxygen vacancies are promising for the electrocatalytic carbon dioxide reduction reaction (CO<sub>2</sub>RR). However, the obscure quantification of oxygen-release behavior has hindered the development of highly active and robust electrocatalysts. Herein, based on theoretical guidance, graphene confined SnO<sub><i>x</i></sub> nanodots (rGO@SnO<sub><i>x</i></sub> ND) holding the capacity for <i>in situ</i> formation of reaction-induced oxygen vacancies were prepared and taken as the model catalyst. <i>Operando</i> X-ray absorption fine structure (XAFS) quantitatively analyzed the reversible oxygen-released behavior, promoting the SnO<sub><i>x</i></sub> lattice modulation of the adsorption of *OCHO intermediate. These structure changes further facilitate the exceptional performance, yielding a peak <i>j</i><sub>formate</sub> of 567 mA cm<sup>–2</sup>, a selectivity of 92.5% and a 50 h long-term stability of rGO@SnO<sub><i>x</i></sub> ND. The findings significantly advance the comprehensive understanding of the quantitative relationship between controllable oxygen vacancies and reaction activity, highlighting the capabilities of <i>operando</i> spectroscopy toward much wider metallic oxide-based electrochemical systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"6 12","pages":"5375–5383 5375–5383"},"PeriodicalIF":8.7000,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Materials Letters","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsmaterialslett.4c01776","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Bulk metallic oxides with abundant surface oxygen vacancies are promising for the electrocatalytic carbon dioxide reduction reaction (CO2RR). However, the obscure quantification of oxygen-release behavior has hindered the development of highly active and robust electrocatalysts. Herein, based on theoretical guidance, graphene confined SnOx nanodots (rGO@SnOx ND) holding the capacity for in situ formation of reaction-induced oxygen vacancies were prepared and taken as the model catalyst. Operando X-ray absorption fine structure (XAFS) quantitatively analyzed the reversible oxygen-released behavior, promoting the SnOx lattice modulation of the adsorption of *OCHO intermediate. These structure changes further facilitate the exceptional performance, yielding a peak jformate of 567 mA cm–2, a selectivity of 92.5% and a 50 h long-term stability of rGO@SnOx ND. The findings significantly advance the comprehensive understanding of the quantitative relationship between controllable oxygen vacancies and reaction activity, highlighting the capabilities of operando spectroscopy toward much wider metallic oxide-based electrochemical systems.
期刊介绍：
ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.
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