Tuning Cu/Cu2O Interfaces for the Reduction of Carbon Dioxide to Methanol in Aqueous Solutions

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2018-10-17 DOI:10.1002/anie.201805256
Dr. Xiaoxia Chang, Prof.?Dr. Tuo Wang, Dr. Zhi-Jian Zhao, Piaoping Yang, Prof.?Dr. Jeffrey Greeley, Dr. Rentao Mu, Gong Zhang, Zhongmiao Gong, Dr. Zhibin Luo, Dr. Jun Chen, Dr. Yi Cui, Prof.?Dr. Geoffrey A. Ozin, Prof.?Dr. Jinlong Gong
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引用次数: 143

Abstract

Artificial photosynthesis can be used to store solar energy and reduce CO2 into fuels to potentially alleviate global warming and the energy crisis. Compared to the generation of gaseous products, it remains a great challenge to tune the product distribution of artificial photosynthesis to liquid fuels, such as CH3OH, which are suitable for storage and transport. Herein, we describe the introduction of metallic Cu nanoparticles (NPs) on Cu2O films to change the product distribution from gaseous products on bare Cu2O to predominantly CH3OH by CO2 reduction in aqueous solutions. The specifically designed Cu/Cu2O interfaces balance the binding strengths of H* and CO* intermediates, which play critical roles in CH3OH production. With a TiO2 model photoanode to construct a photoelectrochemical cell, a Cu/Cu2O dark cathode exhibited a Faradaic efficiency of up to 53.6 % for CH3OH production. This work demonstrates the feasibility and mechanism of interface engineering to enhance the CH3OH production from CO2 reduction in aqueous electrolytes.

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调整Cu/Cu2O界面使二氧化碳在水溶液中还原为甲醇
人工光合作用可以用来储存太阳能,减少二氧化碳转化为燃料,从而有可能缓解全球变暖和能源危机。与产生气态产物相比,将人工光合作用的产物分布调整为适合储存和运输的液体燃料,如CH3OH,仍然是一个巨大的挑战。在此,我们描述了在Cu2O薄膜上引入金属Cu纳米颗粒(NPs),通过在水溶液中CO2还原,将产物分布从裸Cu2O上的气态产物转变为以CH3OH为主。特别设计的Cu/Cu2O界面平衡了H*和CO*中间体的结合强度,这在CH3OH的生成中起着关键作用。用TiO2模型光阳极构建电化学电池,Cu/Cu2O暗阴极制备CH3OH的法拉第效率高达53.6%。本研究证明了界面工程提高水溶液中CO2还原生成CH3OH的可行性和机理。
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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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