journal article·2023-12-04

Electronic Structure Modulation of Unconventional Phase Metal Nanomaterials for Highly Selective Carbon Dioxide Electroreduction

Juan Wang, Haoyi Tan, Hongming Xu, Shibo Xi, Qingbo Wa, Yunhao Wang, Wei Xi, Jingwen Zhou, Jinli Yu, Fengkun Hao, Yuecheng Xiong, Yangbo Ma, Guozhi Wang, Qi Liu, Guangcun Shan, Minhua Shao, Zhanxi Fan

ACS Materials Letters· Volume 5· Issue 12
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Abstract

The electrochemical carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) has been considered as a promising approach to convert atmospheric CO 2 to value-added chemicals to promote carbon neutrality. However, developing electrocatalysts with superior activity and high selectivity toward individual products remains a great challenge. Herein we report the electronic structure modulation of unconventional phase metal nanomaterials to achieve highly efficient CO 2 electroreduction. It has been found that growing cerium oxide (CeO x ) nanostructures on 4H/face-centered cubic (fcc) gold (Au) nanorods can significantly enhance their catalytic activity and selectivity toward the electrochemical conversion of CO 2 to carbon monoxide. X-ray analysis indicates the electronic structure change of 4H/fcc Au nanorods after CeO x overgrowth. In-situ attenuated total reflection infrared spectroscopy measurements reveal that the HCO 3 – concentration near the surface of Au-CeO x heteronanostructures is much higher than that of Au nanorods, facilitating the CO 2 reduction process. Density functional theory calculations suggest the activation effect of CeO x on the 4H/fcc Au nanorod surface for the electrocatalytic CO 2 RR. The synergy between 4H/fcc Au and CeO x promotes the formation of carboxyl (*COOH) species and thus boosts the electrocatalytic CO 2 RR performance. This work highlights the importance of rational electronic structure regulation of unusual phase nanomaterials toward the electrocatalytic conversion of small molecules.
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Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Advanced Thermoelectric Materials and Devices · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, City University of Hong Kong, Hong Kong 999077, China

School of Instrumentation Science and Opto-electronics Engineering, Beihang University, Beijing 100083, China

Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong 999077, China

Institute of Sustainability for Chemicals, Energy and Environment, A*STAR (Agency for Science, Technology and Research), 1 Pesek Road, Jurong Island, Singapore 627833, Singapore

Center for Electron Microscopy, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China

Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Hong Kong 999077, China

Department of Physics, City University of Hong Kong, Hong Kong 999077, China

Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China

City University of Hong Kong Shenzhen Research Institute, Shenzhen 518057, China

Funding

Research Grants Council, University Grants Committee · Science, Technology and Innovation Commission of Shenzhen Municipality · Innovation and Technology Commission · City University of Hong Kong · National Natural Science Foundation of China

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