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用于高效可见光驱动二氧化碳还原为一氧化碳的具有核壳结构的铁/镍有机框架的优化

Optimization of Fe/Ni organic frameworks with core-shell structures for efficient visible-light-driven reduction of carbon dioxide to carbon monoxide.

作者信息

Gu Lin, Deng Guozhi, Huang Ruting, Shi Xianyang

机构信息

Anhui Province Key Laboratory of Wetland Ecosystem Protection and Restoration, School of Resource and Environmental Engineering, Anhui University, Hefei 230601, China.

出版信息

Nanoscale. 2022 Nov 3;14(42):15821-15831. doi: 10.1039/d2nr04377g.

Abstract

To address CO emissions caused by the overuse of fossil fuels, photocatalytic CO reduction from metal-organic frameworks (MOFs) to valuable chemicals is critical for energy conversion and storage. Core-shell MOFs improve interfacial interactions, increasing the number of active sites in the catalyst, thereby improving the photocatalytic reduction. In this work, the catalytic performance of Fe/Ni-MOFs toward photocatalytic CO reduction was improved using a bimetallic strategy. We successfully synthesized a series of Fe/Ni-MOFs with a core-shell structure using a single-step approach combined with hydrothermal synthesis. By altering the synthesis conditions of the bimetallic organic skeleton and contrasting it with a single MOF, we successfully synthesized Fe/Ni-T120 through an efficient photocatalytic reduction of CO. The results of photocatalytic CO reduction experiments indicated that upon using [Ru(bpy)]Cl·6HO as a photosensitizer and triethanolamine (TEOA) and acetonitrile (MeCN) as sacrificial agents, the CO evolution rate of Fe/Ni-T120 reached 9.74 mmol g h and the CO to CO selectivity reached up to 92.1%. Additionally, Fe/Ni-T120 has a broad response range to visible light, a high photocurrent intensity, good chemical stability, and strong photocatalytic efficiency, even after repeated cycles. This study proposes a straightforward method for producing adaptable and stable MOFs for effective photocatalytic CO reduction that is driven by visible light.

摘要

为解决因过度使用化石燃料而产生的一氧化碳排放问题,通过金属有机框架(MOF)将光催化一氧化碳还原为有价值的化学品对于能量转换和存储至关重要。核壳型MOF改善了界面相互作用,增加了催化剂中活性位点的数量,从而提高了光催化还原性能。在这项工作中,采用双金属策略提高了Fe/Ni-MOF对光催化一氧化碳还原的催化性能。我们通过将一步法与水热合成相结合,成功合成了一系列具有核壳结构的Fe/Ni-MOF。通过改变双金属有机骨架的合成条件并将其与单一MOF进行对比,我们通过高效的光催化一氧化碳还原成功合成了Fe/Ni-T120。光催化一氧化碳还原实验结果表明,以[Ru(bpy)]Cl·6H₂O作为光敏剂,三乙醇胺(TEOA)和乙腈(MeCN)作为牺牲剂时,Fe/Ni-T120的一氧化碳析出速率达到9.74 mmol g⁻¹ h⁻¹,一氧化碳到二氧化碳的选择性高达92.1%。此外,Fe/Ni-T120对可见光具有较宽的响应范围、高光电流强度、良好的化学稳定性和较强的光催化效率,即使经过多次循环也是如此。本研究提出了一种直接的方法,用于制备适用于可见光驱动的有效光催化一氧化碳还原的适应性强且稳定的MOF。

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