Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/163720
Title: A two-dimensional van der Waals heterostructure with isolated electron-deficient cobalt sites toward high-efficiency co2 electroreduction
Authors: Gu, Huoliang
Shi, Guoshuai
Zhong, Lixiang
Liu, Lingmei
Zhang, Honghao
Yang, Chunlei
Yu, Ke
Zhu, Chenyuan
Li, Jiong
Zhang, Shuo
Chen, Chen
Han, Yu
Li, Shuzhou
Zhang, Liming
Keywords: Engineering::Materials
Issue Date: 2022
Source: Gu, H., Shi, G., Zhong, L., Liu, L., Zhang, H., Yang, C., Yu, K., Zhu, C., Li, J., Zhang, S., Chen, C., Han, Y., Li, S. & Zhang, L. (2022). A two-dimensional van der Waals heterostructure with isolated electron-deficient cobalt sites toward high-efficiency co2 electroreduction. Journal of the American Chemical Society, 144(47), 21502-21511. https://dx.doi.org/10.1021/jacs.2c07601
Journal: Journal of the American Chemical Society 
Abstract: Electrochemical CO2 conversion is a promising way for sustainable chemical fuel production, yet the conversion efficiency is strongly limited by the sluggish kinetics and complex reaction pathways. Here we report the ultrathin conjugated metalloporphyrin covalent organic framework epitaxially grown on graphene as a two-dimensional van der Waals heterostructure to catalyze CO2 reduction. Operando X-ray absorption and density functional theory calculations reveal the strong interlayer coupling leads to electron-deficient metal centers and speeds up electrocatalysis. The Co(III)-N4 centers exhibit a CO Faradaic efficiency of 97% at a partial current density of 8.2 mA cm-2 in an H-cell, along with a stable running over 30 h. The selectivity of CO approached 99% with a partial current density of 191 mA cm-2 in a liquid flow cell, and the turnover frequency achieved 50 400 h-1 at -1.15 V vs RHE, outperforming most reported organometallic frameworks. This work highlights the key role of strong electronic coupling between van der Waals layers for accelerating the dynamics of CO2 conversion.
URI: https://hdl.handle.net/10356/163720
ISSN: 0002-7863
DOI: 10.1021/jacs.2c07601
Rights: © 2022 American Chemical Society. All rights reserved.
Fulltext Permission: none
Fulltext Availability: No Fulltext
Appears in Collections:MSE Journal Articles

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