{"title":"提高CO2还原活性的原位氧空位工程","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":"{\"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}","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
摘要
具有丰富表面氧空位的大块金属氧化物在电催化二氧化碳还原反应（CO2RR）中具有广阔的应用前景。然而，氧释放行为的模糊量化阻碍了高活性和鲁棒性电催化剂的发展。本文在理论指导下，制备了具有原位生成反应诱导氧空位能力的石墨烯约束SnOx纳米点（rGO@SnOx ND），并将其作为模型催化剂。Operando x射线吸收精细结构（XAFS）定量分析了可逆的氧释放行为，促进了SnOx晶格调制对*OCHO中间体的吸附。这些结构的变化进一步促进了优异的性能，产生567 mA cm-2的峰构型，92.5%的选择性和50 h的rGO@SnOx ND长期稳定性。这些发现极大地促进了对可控氧空位与反应活性之间定量关系的全面理解，突出了operando光谱在更广泛的金属氧化物基电化学体系中的能力。
In Situ Oxygen-Vacancy Engineering for Enhancing CO2 Reduction Activity
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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