Search

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. [ABSTRACT FROM AUTHOR]

Keywords: Carbon Dioxide Conversion; Heterogeneous Catalysis; Materials Science; Reaction Mechanisms; Reduction EN Carbon Dioxide Conversion Heterogeneous Catalysis Materials Science Reaction Mechanisms Reduction 1 1 1 10/31/23 20231106 NES 231106 B CO SB 2 sb hydrogenation to formate b is an attractive route for the utilization of this greenhouse gas. Comprehensive mechanism studies reveal that selective production of formate is enabled at MoS SB 2 sb edge sulfur vacancies via a new water-mediated hydrogenation mechanism. Carbon Dioxide Conversion, Heterogeneous Catalysis, Materials Science, Reaction Mechanisms, Reduction. [Extracted from the article]

Moreover, the water-anion interactions can repel the contact of water with the active centers, thus inhibiting the occurrence of HER. The halogen anions can form hydrogen bonds with intermediates (*COOH) and thus lower the energy barrier to the formation of CO. Keywords: CO; CO2 Electrocatalysis; Covalent Organic Framework; Hydrogen Bond; Imidazolium EN CO CO2 Electrocatalysis Covalent Organic Framework Hydrogen Bond Imidazolium 1 1 1 02/07/23 20230206 NES 230206 B A hydrogen bonding strategy b for achieving an excellent electrocatalytic CO SB 2 sb reduction reaction performance over an imidazolium-functionalized covalent organic framework (Co-iBFBim-COF-X) is reported by Yuan-Biao Huang and co-workers in their Research Article (e202215687). [Extracted from the article]