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Zhendong Feng, Zhendong Feng, Chizhou Tang, Pengfei Zhang, Kun Li, Guanna Li, Jijie Wang, Zhaochi Feng, Zhaochi Feng, Can Li
The role of formate species for CO 2 hydrogenation is still under debate. Although formate has been frequently observed and commonly proposed as the possible intermediate, there is no definite evidence for the reaction of formate species for methanol production. Here, formate formation and conversion over the ZnZrO x solid solution catalyst are investigated by in situ/operando diffuse reflectance infrared Fourier transform spectroscopy-mass spectroscopy (DRIFTS-MS) coupled with density functional theory (DFT) calculations. Spectroscopic results show that bidentate carbonate formed from CO 2 adsorption is hydrogenated to formate on Zn–O–Zr sites (asymmetric sites), where the Zn site is responsible for H 2 activation and the Zr site is beneficial for the stabilization of reaction intermediates. The asymmetric Zn–O–Zr sites with adjacent and inequivalent features on the ZnZrO x catalyst promote not only formate formation but also its transformation. Both theoretical and experimental results demonstrate that the origin of the excellent performance of the ZnZrO x catalyst for methanol formation is associated with the H 2 heterolytic cleavage promoted by the asymmetric Zn and Zr sites.
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Feng, Z., Feng, Z., Tang, C., Zhang, P., Li, K., Li, G., Wang, J., Feng, Z., Feng, Z., & Li, C. (2023). Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation. Journal of the American Chemical Society, 145(23), 12663–12672. https://doi.org/10.1021/jacs.3c02248
Feng, Zhendong, et al. "Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation." Journal of the American Chemical Society, vol. 145, no. 23, 2023, pp. 12663–12672, https://doi.org/10.1021/jacs.3c02248.
Feng, Zhendong, Zhendong Feng, Chizhou Tang, Pengfei Zhang, Kun Li, Guanna Li, Jijie Wang, Zhaochi Feng, Zhaochi Feng, and Can Li. "Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation." Journal of the American Chemical Society 145, no. 23 (2023): 12663–12672. https://doi.org/10.1021/jacs.3c02248.
Feng Z., Feng Z., Tang C. [и др.] Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation // Journal of the American Chemical Society. — 2023. — Vol. 145, № 23. — P. 12663–12672. — URL: https://doi.org/10.1021/jacs.3c02248
@article{feng2023asymmetric,
title = {{Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation}},
author = {Zhendong Feng and Zhendong Feng and Chizhou Tang and Pengfei Zhang and Kun Li and Guanna Li and Jijie Wang and Zhaochi Feng and Zhaochi Feng and Can Li},
journal = {Journal of the American Chemical Society},
year = {2023},
volume = {145},
number = {23},
pages = {12663--12672},
doi = {10.1021/jacs.3c02248},
url = {https://doi.org/10.1021/jacs.3c02248}
}TY - JOUR AU - Feng, Zhendong AU - Feng, Zhendong AU - Tang, Chizhou AU - Zhang, Pengfei AU - Li, Kun AU - Li, Guanna AU - Wang, Jijie AU - Feng, Zhaochi AU - Feng, Zhaochi AU - Li, Can TI - Asymmetric Sites on the ZnZrO x Catalyst for Promoting Formate Formation and Transformation in CO 2 Hydrogenation JO - Journal of the American Chemical Society VL - 145 IS - 23 SP - 12663 EP - 12672 PY - 2023 DA - 2023/06/01 DO - 10.1021/jacs.3c02248 UR - https://doi.org/10.1021/jacs.3c02248 ER -
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