Citation: Sanmei Wang, Dengxin Yan, Wenhua Zhang, Liangbing Wang. Graphene-supported isolated platinum atoms and platinum dimers for CO₂ hydrogenation: Catalytic activity and selectivity variations[J]. Chinese Chemical Letters, ;2025, 36(4): 110611. doi: 10.1016/j.cclet.2024.110611 shu

Graphene-supported isolated platinum atoms and platinum dimers for CO₂ hydrogenation: Catalytic activity and selectivity variations

Sanmei Wang ^{a, b, c, 1} ,
Dengxin Yan ^{d, 1} ,
Wenhua Zhang ^{c, d, *,} ,
Liangbing Wang ^{b, *,}

a.
Research Institute of Interdisciplinary Sciences (RISE) and School of Materials Science & Engineering, Dongguan University of Technology, Dongguan 523808, China
b.
State Key Laboratory for Powder Metallurgy, School of Materials Science and Engineering, Central South University, Changsha 410083, China
c.
Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Centre of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei 230026, China
d.
Laboratory for Chemical Technology, Ghent University, Ghent 9052, Belgium

whhzhang@ustc.edu.cn

wanglb@csu.edu.cn

Received Date: 11 September 2024
Revised Date: 31 October 2024
Accepted Date: 4 November 2024
Available Online: 5 November 2024

Figures(6)

Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO₂ hydrogenation. Combining density functional theory calculations and microkinetic analysis, we proposed that graphene-supported isolated Pt atoms (Pt₁/graphene) and Pt₂ dimers (Pt₂/graphene) exhibited distinct selectivity in CO₂ hydrogenation. Pt₁/graphene facilitated the conversion of CO₂ into formic acid, whereas Pt₂/graphene favored methanol generation. The variation in product selectivity arose from the synergistic interaction of Pt₂ dimers, which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from ^*COOH intermediates to ^*C(OH)₂ intermediates, altering the reaction pathways compared to isolated Pt atoms. Additionally, an analysis of the catalytic activities of three Pt₁/graphene and three Pt₂/graphene structures revealed that the turnover frequencies for formic acid generation on Pt_1ⅱ/graphene and methanol generation on Pt_2ⅰ/graphene were as high as 744.48 h^-1 and 789.48 h^-1, respectively. These values rivaled or even surpassed those previously reported in the literature under identical conditions. This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO₂ hydrogenation
- CO₂ hydrogenation,
- Graphene,
- Pt single-atom,
- Pt₂ dimers,
- DFT
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Graphene-supported isolated platinum atoms and platinum dimers for CO2 hydrogenation: Catalytic activity and selectivity variations

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通讯作者: 陈斌, bchen63@163.com

Graphene-supported isolated platinum atoms and platinum dimers for CO₂ hydrogenation: Catalytic activity and selectivity variations