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author:

Ma, Zongyu (Ma, Zongyu.) [1] | Zhang, Zhen (Zhang, Zhen.) [2] | Chen, Yinye (Chen, Yinye.) [3] | Su, Jianghua (Su, Jianghua.) [4] | Zuo, Jiachang (Zuo, Jiachang.) [5] | Yang, Mengqing (Yang, Mengqing.) [6] | Wang, Xiuyun (Wang, Xiuyun.) [7] | Qian, Qingrong (Qian, Qingrong.) [8] | Chen, Qinghua (Chen, Qinghua.) [9] | Luo, Yongjin (Luo, Yongjin.) [10]

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Abstract:

In-plane sulfur vacancies in the MoS2 catalyst exhibit great potential for low-temperature CO2 hydrogenation to methanol. However, both CO2 and H2 adsorb and activate at sulfur vacancies, leading to competition between them. Anchoring atomically dispersed Co atoms over MoS2 may facilitate H2 adsorption and activation. Here, a thiourea-assisted strategy was employed to construct a Co-thiourea complex, which transformed into atomically dispersed Co species after heat treatment. Under reaction conditions of 5 MPa and 220 °C, the 0.5Co/MoS2 catalyst achieved a methanol space-time yield of 323 mgMeOH gcat-1 h-1 after induction, with stability maintained for at least 500 h, compared to 177 mgMeOH gcat-1 h-1 for pristine MoS2. Mechanistic study revealed that the hydrogenation of CO2 to methanol follows the COOH* pathway, where CO2 is first hydrogenated to COOH* intermediate and then gradually hydrogenated CH3O* species. This work presents a viable strategy for developing atomically dispersed metal-MoS2 catalysts for CO2 hydrogenation to methanol. © 2025 American Chemical Society.

Keyword:

Carbon dioxide Catalysis Catalysts Cobalt compounds Hydrogenation Layered semiconductors Methanol Molybdenum compounds Sulfur Temperature Thioureas

Community:

  • [ 1 ] [Ma, Zongyu]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 2 ] [Zhang, Zhen]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 3 ] [Chen, Yinye]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 4 ] [Su, Jianghua]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 5 ] [Zuo, Jiachang]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 6 ] [Yang, Mengqing]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 7 ] [Wang, Xiuyun]Qingyuan Innovation Laboratory, Quanzhou; 362100, China
  • [ 8 ] [Wang, Xiuyun]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou; 350002, China
  • [ 9 ] [Qian, Qingrong]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 10 ] [Chen, Qinghua]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China
  • [ 11 ] [Luo, Yongjin]Fujian Key Laboratory of Pollution Control and Resource Reuse, College of Environmental and Resource Sciences, Fujian Normal University, Fuzhou; 350007, China

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Source :

ACS Sustainable Chemistry and Engineering

Year: 2025

Issue: 27

Volume: 13

Page: 10690-10700

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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