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在从水性二氧化碳进行甲酸盐电合成中具有高催化性能的改性锡金属有机框架材料。

In-modified Sn-MOFs with high catalytic performance in formate electrosynthesis from aqueous carbon dioxide.

作者信息

Yan Jiaying, Wang Xuanyu, Ning Fanghua, Yi Jin, Liu Yuyu, Wu Kai

机构信息

Institute for Sustainable Energy, College of Sciences, Shanghai University, Baoshan District, Shanghai 200444, China.

Nanotechnology Research Institute, College of Materials and Textile Engineering, Jiaxing University, Jiaxing 314001, China.

出版信息

Dalton Trans. 2023 Aug 29;52(34):11904-11912. doi: 10.1039/d3dt01610b.

DOI:10.1039/d3dt01610b
PMID:37564013
Abstract

Electrochemical reduction of carbon dioxide (COER) has become an effective solution to relieve the energy crisis and tackle climate change. In this study, a series of tin-based organic frameworks modified by In (Sn-MOF/In) were successfully synthesized a simple hydrothermal method and explored for high formate-selective COER. The pure Sn-MOF exhibits maximum formate selectivity with a faradaic efficiency (FE) of approximately 85.0% and a current density of 15 mA cm at -1.16 V, while the In (6%)-modified Sn-MOF (Sn-MOF/In) delivers a much higher maximum FE (around 97.5%) and a current density of 16 mA cm at -0.96 V. Remarkably, the Sn-MOF/In exhibits a significantly larger specific surface area (183.3 m g) compared to the Sn-MOF (65.2 m g). These findings indicate that introducing In, an alien element with a slightly different outer orbital electron number from that of Sn, can significantly boost the selectivity and activity for COER to formate. This study presents an efficient way to modify MOF catalysts through a well-designed introducing process.

摘要

二氧化碳的电化学还原(COER)已成为缓解能源危机和应对气候变化的有效解决方案。在本研究中,通过简单的水热法成功合成了一系列铟改性的锡基有机框架材料(Sn-MOF/In),并对其进行了高甲酸盐选择性COER的探索。纯Sn-MOF在-1.16 V时表现出最大甲酸盐选择性,法拉第效率(FE)约为85.0%,电流密度为15 mA cm²,而铟(6%)改性的Sn-MOF(Sn-MOF/In)在-0.96 V时具有更高的最大FE(约97.5%)和16 mA cm²的电流密度。值得注意的是,与Sn-MOF(65.2 m² g⁻¹)相比,Sn-MOF/In的比表面积显著更大(183.3 m² g⁻¹)。这些发现表明,引入铟(一种外层轨道电子数与锡略有不同的异类元素)可以显著提高COER生成甲酸盐的选择性和活性。本研究提出了一种通过精心设计的引入过程来改性MOF催化剂的有效方法。

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