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Boosting CO2 Hydrogenation to Formate over Edge‐Sulfur Vacancies of Molybdenum Disulfide

Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but is confronted with challenges in developing high‐performance non‐precious metal catalysts for application of the process. Herein, we report a highly durable edge‐rich molybdenum disulfide (MoS2) catalyst...

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Published in:Angewandte Chemie International Edition 2023-11, Vol.62 (45), p.e202307086-e202307086
Main Authors: Wang, Zifeng, Kang, Yiran, Hu, Jingting, Ji, Qinqin, Lu, Zhixuan, Xu, Guilan, Qi, Yutai, Zhang, Mo, Zhang, Wangwang, Huang, Rui, Yu, Liang, Zhong‐qun Tian, Deng, Dehui
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container_issue 45
container_start_page e202307086
container_title Angewandte Chemie International Edition
container_volume 62
creator Wang, Zifeng
Kang, Yiran
Hu, Jingting
Ji, Qinqin
Lu, Zhixuan
Xu, Guilan
Qi, Yutai
Zhang, Mo
Zhang, Wangwang
Huang, Rui
Yu, Liang
Zhong‐qun Tian
Deng, Dehui
description Synthesis of formate from hydrogenation of carbon dioxide (CO2) is an atom‐economic reaction but is confronted with challenges in developing high‐performance non‐precious metal catalysts for application of the process. Herein, we report a highly durable edge‐rich molybdenum disulfide (MoS2) catalyst for CO2 hydrogenation to formate at 200 °C, which delivers a high selectivity of over 99 % with a superior turnover frequency of 780.7 h−1 surpassing those of previously reported non‐precious metal catalysts. Multiple experimental characterization techniques combined with theoretical calculations reveal that sulfur vacancies at MoS2 edges are the active sites and the selective production of formate is enabled via a completely new water‐mediated hydrogenation mechanism, in which surface OH* and H* species in dynamic equilibrium with water serve as moderate hydrogenating agents for CO2 with residual O* reduced by hydrogen. This study provides a new route for developing low‐cost high‐performance catalysts for CO2 hydrogenation to formate.
doi_str_mv 10.1002/anie.202307086
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subjects Atom economy
Carbon dioxide
Catalysts
Hydrogenation
Molybdenum
Molybdenum disulfide
Noble metals
Sulfur
title Boosting CO2 Hydrogenation to Formate over Edge‐Sulfur Vacancies of Molybdenum Disulfide
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