Citation: Junwen Lu, Shunan Zhang, Haozhi Zhou, Chaojie Huang, Lin Xia, Xiaofang Liu, Hu Luo, Hui Wang. Ir Single Atoms and Clusters Supported on α-MoC as Catalysts for Efficient Hydrogenation of CO₂ to CO[J]. Acta Physico-Chimica Sinica, ;2023, 39(11): 230202. doi: 10.3866/PKU.WHXB202302021 shu

Ir Single Atoms and Clusters Supported on α-MoC as Catalysts for Efficient Hydrogenation of CO₂ to CO

Junwen Lu ^{1, 2} ,
Shunan Zhang ^3,, ,
Haozhi Zhou ³ ,
Chaojie Huang ^{1, 2} ,
Lin Xia ¹ ,
Xiaofang Liu ¹ ,
Hu Luo ¹ ,
Hui Wang ^{1, 3,,}

1.
CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Institute of Carbon Neutrality, ShanghaiTech University, Shanghai 201203, China

Corresponding author: Shunan Zhang, zhangshn2@shanghaitech.edu.cn Hui Wang, wanghh@sari.ac.cn
Received Date: 14 February 2023
Revised Date: 20 March 2023
Accepted Date: 21 March 2023
Available Online: 24 March 2023
Fund Project: the National Key Research and Development Program of China 2022YFA1504800the National Key Research and Development Program of China 2022YFA1504702the National Key Research and Development Program of China 2022YFB4101900the National Natural Science Foundation of China 22108289the National Natural Science Foundation of China 22279158the National Natural Science Foundation of China 21905291CNOOC Institute of Chemicals & Advanced Materials YJSCZX07956YJShanghai Institute of Cleantech Innovation E244831E01

The conversion of CO₂ into CO via the reverse water gas shift (RWGS) reaction has recently attracted considerable attention owing to the increase in atmospheric CO₂ emissions. However, metal-supported catalysts easily undergo sintering and become inactive at high temperatures. To fabricate highly active and stable catalysts, molybdenum carbide (Mo_xC), with properties similar to those of precious metals, has been extensively investigated. In particular, it has been demonstrated that face-centered cubic α-MoC can strongly interact with support metals, rendering it an attractive candidate as a catalyst for the RWGS reaction. Furthermore, it has been previously demonstrated that metallic Ir, with unique electronic properties and a low CO desorption barrier, is active for the RWGS at low temperatures (250–300 ℃). Accordingly, in this study, a system of Ir species and α-MoC was constructed using a solvent evaporation self-assembly method. The catalytic performance of the Ir/MoC catalysts for the RWGS reaction was considerably superior to that of pure α-MoC over a wide temperature range (200–500 ℃) owing to the synergistic effect of Ir and α-MoC. The optimal 0.5%Ir/MoC catalyst yielded a CO₂ conversion of 48.4% at 500 ℃, 0.1 MPa, and 300000 mL·g⁻¹·h⁻¹, which was comparable to the equilibrium conversion (49.9%). The CO selectivity and space-time yield of CO over 0.5%Ir/MoC reached 94.0% and 423.1 μmol·g⁻¹·s⁻¹, respectively, which were higher than most of the previously reported values. Moreover, 0.5%Ir/MoC retained its catalytic properties over 100 h and demonstrated excellent stability at high temperatures. Several characterization methods were used to demonstrate that the Ir species supported on α-MoC substrates were highly dispersed. The strong metal-support interaction between Ir and α-MoC, which occurred via electron transfer, considerably improved the stability of the Ir/MoC catalysts. For the Ir/MoC catalysts with Ir loadings > 0.2% (mass fraction), Ir single atoms (Ir₁) and clusters (Ir_n) coexisted to create Ir_n-Ir₁-C-Mo synergistic sites between Ir and α-MoC. The number of Ir₁ species and size of Ir_n species of 0.5%Ir/MoC were higher and smaller, respectively, than those of the other Ir/MoC catalysts. This conferred 0.5%Ir/MoC an optimal electron density, which contributed to the remarkable adsorption and activation of CO₂ and H₂ during the RWGS. In situ diffuse reflectance infrared Fourier transform spectroscopy experiments revealed that the RWGS reaction mechanism occurred via a formate pathway. Although the formation of Ir_n-Ir₁-C-Mo synergistic sites did not affect the reaction mechanism, the generation and decomposition of formate intermediates were distinctly promoted. Therefore, the catalytic performance of Ir/MoC was effectively improved by the synergistic effect. This study provides a guide for designing efficient and stable catalysts for CO₂ utilization.
- Reverse water gas shift reaction,
- Metal-support interaction,
- Synergistic effect,
- Molybdenum carbide,
- Iridium catalyst
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Ir Single Atoms and Clusters Supported on α-MoC as Catalysts for Efficient Hydrogenation of CO2 to CO

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Ir Single Atoms and Clusters Supported on α-MoC as Catalysts for Efficient Hydrogenation of CO₂ to CO