Prompting CO2 Electroreduction to Ethanol by Iron Group Metal Ion Dopants Induced Multi-sites at the Interface of SnSe/SnSe2 p-n Heterojunction.

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-10-17 DOI:10.1002/anie.202415273
Xinyue Zheng, Yan Hu, Xiangyu Wang, Jiahui Zhu, Xingyue Zhang, Tian Sheng, Zhengcui Wu
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Abstract

The development of non-copper-based materials for CO2 electroreduction to ethanol with high selectivity at large current density is highly desirable, but still a great challenge. Herein, we report iron group metal ions of M2+ (M=Fe, Co, or Ni)-doped amorphous/crystalline SnSe/SnSe2 nanorod/nanosheet hierarchical structures (a/c-SnSe/SnSe2) for selective CO2 electroreduction to ethanol. Iron group metal ions doping induces multiple active sites at the interface of M2+-doped SnSe/SnSe2 p-n heterojunction, which strengthens *CO intermediate binding for further C-C coupling to eventual ethanol generation. As a representative, Fe9.0%-a/c-SnSe/SnSe2 exhibits an ethanol Faradaic efficiency of 62.7 % and a partial current density of 239.0 mA cm-2 at -0.6 V in a flow cell. Moreover, it can output an ethanol Faradaic efficiency of 63.5 % and a partial current density of 201.2 mA cm-2 with a full-cell energy efficiency of 24.1 % at 3.0 V in a membrane electrode assembly (MEA) electrolyzer. This work provides insight into non-Cu based catalyst design for stabilizing the key intermediates for selective ethanol production from CO2 electroreduction.

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通过铁族金属离子掺杂剂诱导 SnSe/SnSe2 p-n 异质结界面上的多位点,促进二氧化碳电还原成乙醇。
开发在大电流密度下具有高选择性的二氧化碳电还原为乙醇的非铜基材料是非常理想的,但仍然是一个巨大的挑战。在此,我们报告了掺杂铁族金属离子的 M2+(M = Fe、Co 或 Ni)非晶/晶态 SnSe/SnSe2 纳米棒/纳米片分层结构(a/c-SnSe/SnSe2)用于选择性 CO2 电还原为乙醇的情况。铁族金属离子的掺杂在掺杂了 M2+ 的 SnSe/SnSe2 p-n 异质结的界面上诱导出多个活性位点,从而加强了 *CO 中间体的结合,使其能进一步通过 C-C 耦合最终生成乙醇。作为代表,Fe9.0%-a/c-SnSe/SnSe2 在流动池中的乙醇法拉第效率为 62.7%,-0.6 V 时的部分电流密度为 239.0 mA cm-2。此外,在膜电极组件(MEA)电解槽中,当电压为 3.0 V 时,乙醇法拉第效率为 63.5%,部分电流密度为 201.2 mA cm-2,全电池能量效率为 24.1%。这项研究为稳定二氧化碳电还原选择性乙醇生产的关键中间产物的非铜基催化剂设计提供了深入的见解。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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