Regulated reaction pathway of CO2 photoreduction into CH4 by metal atom pair 
sites

He, Dong-Po; Huang, Guang-Bing; Hu, Jun; Wu, Yang; Li, Xiao-Dong; Chen, Qing-Xia; Zhu, Shan; Yan, Wen-Sheng; Zhu, Jun-Fa; Pan, Yang; Jiao, Xing-Chen

doi:10.1007/s12598-024-02757-y

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Regulated reaction pathway of CO₂ photoreduction into CH₄ by metal atom pair sites

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Li, Xiao-Dong
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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https://doi.org/10.1007/s12598-024-02757-y
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引用

He, D.-P., Huang, G.-B., Hu, J., Wu, Y., Li, X.-D., Chen, Q.-X., Zhu, S., Yan, W.-S., Zhu, J.-F., Pan, Y., & Jiao, X.-C. (2024). Regulated reaction pathway of CO₂ photoreduction into CH₄ by metal atom pair sites. Rare Metals. doi:10.1007/s12598-024-02757-y.

引用: https://hdl.handle.net/21.11116/0000-000F-6458-E

要旨

The carbon dioxide (CO₂) reduction process involves complex protonation, making the resulting product often unpredictable. To achieve the desired product, it is crucial to manipulate the reaction steps. Herein, we build the metal atom pair sites for selective CO₂ photoreduction into methane. As a prototype, Ni atom pair sites loaded on the MoS₂ nanosheets were synthesized and verified by high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure spectra (XANES). In-situ Fourier transform infrared spectroscopy (FTIR) monitors the *CHO group, a crucial intermediate in CH₄ production, during CO₂ photoreduction on the Ni-MoS₂ nanosheets, whereas this monitoring is not observed for the MoS₂ nanosheets. Also, theoretical calculations disclose that over the Ni-MoS₂ nanosheet slab, the formation energy of *CHO intermediates is determined to be lower (0.585 eV) than the desorption energy of *CO intermediates for CO production (0.64 eV), implying the higher selectivity of CH4 production. Accordingly, the Ni-MoS₂ nanosheets demonstrate a methane formation rate of 27.21 μmol·g⁻¹·h⁻¹, coupled with an impressive electron selectivity of 94.2%.