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用于CO电还原的间隙合金的原位拓扑转变

In Situ Topotactic Transformation of an Interstitial Alloy for CO Electroreduction.

作者信息

Zhao Changming, Luo Gan, Liu Xiaokang, Zhang Wei, Li Zhijun, Xu Qian, Zhang Qinghua, Wang Huijuan, Li Deming, Zhou Fangyao, Qu Yunteng, Han Xiao, Zhu Zezhou, Wu Geng, Wang Jing, Zhu Junfa, Yao Tao, Li Yafei, Bouwmeester Henny J M, Wu Yuen

机构信息

Department of Chemistry, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, 230026, China.

Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.

出版信息

Adv Mater. 2020 Oct;32(39):e2002382. doi: 10.1002/adma.202002382. Epub 2020 Aug 23.

Abstract

Electrochemical reduction of CO to value-added products holds promise for storage of energy from renewable sources. Copper can convert CO into multi-carbon (C ) products during CO electroreduction. However, developing a Cu electrocatalyst with a high selectivity for CO reduction and desirable production rates for C products remains challenging. Herein, highly lattice-disordered Cu N with abundant twin structures as a precursor electrocatalyst is examined for CO reduction. Through in situ activation during the CO reduction reaction (CORR) and concomitant release of nitrogen, the obtained metallic Cu° catalyst particles inherit the lattice dislocations present in the parent Cu N lattice. The de-nitrified catalyst delivers an unprecedented C Faradaic efficiency of over 90% at a current density of 727 mA cm in a flow cell system. Using a membrane electrode assembly (MEA) electrolyzer with a solid-state electrolyte (SSE), a 17.4 vol% ethylene stream and liquid streams with concentration of 1.45 m and 230 × 10 m C products at the outlet of the cathode and SSE-containment layer are obtained.

摘要

将CO电化学还原为增值产品有望实现可再生能源的能量存储。在CO电还原过程中,铜可以将CO转化为多碳(C)产品。然而,开发一种对CO还原具有高选择性且对C产品具有理想产率的铜电催化剂仍然具有挑战性。在此,研究了具有丰富孪晶结构的高度晶格无序的CuN作为前驱体电催化剂用于CO还原。通过在CO还原反应(CORR)过程中的原位活化以及伴随的氮释放,所获得的金属Cu°催化剂颗粒继承了母体CuN晶格中存在的晶格位错。在流动池系统中,脱氮催化剂在电流密度为727 mA cm时实现了超过90%的前所未有的C法拉第效率。使用具有固态电解质(SSE)的膜电极组件(MEA)电解槽,在阴极和SSE包容层的出口处获得了17.4 vol%的乙烯流以及浓度分别为1.45 m和230×10 m C产品的液流。

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