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金属(铜/铟)氧化物的晶界和界面相互作用以促进将二氧化碳高效电催化还原为合成气。

Grain boundary and interface interaction of metal (copper/indium) oxides to boost efficient electrocatalytic carbon dioxide reduction into syngas.

作者信息

He Ruinan, Luo Xi, Li Lulu, Zhang Yang, Peng Luwei, Xu Nengneng, Qiao Jinli

机构信息

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Environmental Science and Engineering, Donghua University, 2999 Ren'min North Road, Shanghai 201620, China; Department of Applied Physics, The Hong Kong Polytechnic University, Kowloon 999077, Hong Kong, China.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Environmental Science and Engineering, Donghua University, 2999 Ren'min North Road, Shanghai 201620, China.

出版信息

J Colloid Interface Sci. 2024 Mar 15;658:1016-1024. doi: 10.1016/j.jcis.2023.12.127. Epub 2023 Dec 23.

Abstract

Electrochemical conversion of carbon dioxide (CO) into syngas is considered a promising approach to mitigate global warming and achieve the recycling of carbon resources. In this work, a series of core-shell metal (copper/indium) oxides with abundant grain boundaries (GBs) between the amorphous InO and cubic CuO have been prepared by template-assisted co-precipitation method and tested for the synthesis of syngas by electrochemical CO reduction reaction (CORR). The phases of CuO and InO are independent in bimetallic oxides and do not form any alloy oxidation phase, thus CuO and InO can maintain their crystal structure and chemical properties in bimetallic oxides. The CuO and InO would been completely reduced to metallic Cu and In during CORR. The derived copper/indium possesses the maximum FE of CO (80 %) at -0.77 V vs. reversible hydrogen electrode (RHE) and a good stability of 10 h in an H-type cell. Further applied the copper/indium oxide in the MEA reactor, the FE of CO is more than 80 % at 2.6 V and the total FE of syngas is near 100 % at all applied potentials. More importantly, the H/CO ratios can be tuned from 1/1 to 1/4 by changing the applied voltages in MEA. Therefore, this study provides a promising strategy to promote the electrocatalytic CORR conversion by creating abundant grain boundaries in bimetallic oxides to regulate the ratio of H/CO.

摘要

将二氧化碳(CO₂)电化学转化为合成气被认为是缓解全球变暖及实现碳资源循环利用的一种很有前景的方法。在本工作中,通过模板辅助共沉淀法制备了一系列在非晶态In₂O₃与立方CuO之间具有大量晶界(GBs)的核壳型金属(铜/铟)氧化物,并通过电化学CO₂还原反应(CORR)测试了其合成合成气的性能。在双金属氧化物中,CuO和In₂O₃的相是独立的,不会形成任何合金氧化相,因此CuO和In₂O₃在双金属氧化物中可以保持其晶体结构和化学性质。在CORR过程中,CuO和In₂O₃会完全还原为金属Cu和In。所制备的铜/铟在相对于可逆氢电极(RHE)为-0.77 V时具有最大的CO法拉第效率(FE)(80%),并且在H型电解池中具有10小时的良好稳定性。进一步将铜/铟氧化物应用于MEA反应器中,在2.6 V时CO的FE超过80%,并且在所有施加电位下合成气的总FE接近100%。更重要的是,通过改变MEA中的施加电压,H/CO比可以从1/1调节到1/4。因此,本研究提供了一种很有前景的策略,即通过在双金属氧化物中创造大量晶界来调节H/CO比,从而促进电催化CORR转化。

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