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罗马里奥

至尊木虫 (正式写手)

MN-EPI: 9
应助: 27 (小学生)
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在线: 763.2小时
虫号: 1110146
注册: 2010-09-28
性别: GG
专业: 无机纳米化学

[交流] 均相银空位通过增强轨道杂化实现高电流、高选择性合成超纯CO 已有2人参与

河南大学李杰教授/陈珂教授、中南大学刘敏教授，联手在Nano Letters发表了题为“Homogeneous Vacancies-Enhanced Orbital Hybridization for Selective and Efficient CO2-to-CO Electrocatalysis”研究论文。

在这项工作中，通过电化学重构卤化银，实现了空位在银纳米颗粒内的均匀分布。表面银空位提供结合CO2和中间体的活性位点，而内部银空位则有助于优化电子结构。表面空位和内部空位的协同催化作用增强了银和中间体的轨道杂化，大幅度降低电催化还原CO2合成CO（ECO2RR-to-CO）的反应势垒，使得大面积电极（9 cm2）在7.5A的电流下能够以几乎100%的法拉第效率合成超纯CO（CO/H2法拉第效率比值为6932）。

文章链接：
https://pubs.acs.org/doi/10.1021/acs.nanolett.3c01905

期刊：
Nano Letters

DOI：
https://doi.org/10.1021/acs.nanolett.3c01905

题目：
Homogeneous Vacancies-Enhanced Orbital Hybridization for Selective and Efficient CO2-to-CO Electrocatalysis

作者：
Yuntong Qin, Guangming Zhan, Cun Tang, Di Yang, Xibo Wang, Jianhua Yang, Chengliang Mao, Zhentian Hao, Shuangyu Wang, Yixin Qin, Hongmei Li, Ke Chen*, Min Liu*, and Jie Li*

摘要：
Crafting vacancies offers an efficient route to upgrade the selectivity and productivity of nanomaterials for CO2 electroreduction. However, defective nanoelectrocatalysts bear catalytically active vacancies mostly on their surface, with the rest of the interior atoms adiaphorous for CO2-to-product conversion. Herein, taking nanosilver as a prototype, we arouse the catalytic ability of internal atoms by creating homogeneous vacancies realized via electrochemical reconstruction of silver halides. The homogeneous vacancies-rich nanosilver, compared to the surface vacancies-dominated counterpart, features a more positive d-band center to trigger an intensified hybridization of the Ag_d orbital with the C_P orbital of the *COOH intermediate, leading to an accelerated CO2-to-CO transformation. These structural and electronic merits allow a large-area (9 cm–2) electrode to generate nearly pure CO with a CO/H2 Faradaic efficiency ratio of 6932 at an applied current of 7.5 A. These findings highlight the potential of designing new-type defects in realizing the industrialization of electrocatalytic CO2 reduction.

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