Ultrathin LayCoOx Nanosheets with High Porosity Featuring Boosted Catalytic Oxidation of Benzene: Mechanism Elucidation via an Experiment–Theory Combined Paradigm

Ultrathin LayCoOx Nanosheets with High Porosity Featuring Boosted Catalytic Oxidation of Benzene: Mechanism Elucidation via an Experiment–Theory Combined Paradigm

Inorganic Chemistry

10.1021/acs.inorgchem.3c04621

http://dx.doi.org/10.1021/acs.inorgchem.3c04621

Qun Li, Chunyan Deng, Wenyu Zhou, Peng Huang, Chenyang Lu, Haisong Feng, Lichun Dong, Luxi Tan, Yong-Wei Zhang, Cailong Zhou, Yi Qin, Dong Xia

13 February 2024

Li, Q., Deng, C., Zhou, W., Huang, P., Lu, C., Feng, H., Dong, L., Tan, L., Zhang, Y.-W., Zhou, C., Qin, Y., & Xia, D. (2024). Ultrathin LayCoOx Nanosheets with High Porosity Featuring Boosted Catalytic Oxidation of Benzene: Mechanism Elucidation via an Experiment–Theory Combined Paradigm. Inorganic Chemistry, 63(8), 3974–3985. https://doi.org/10.1021/acs.inorgchem.3c04621

Designing transition-metal oxides for catalytically removing the highly-toxic benzene holds significance in addressing indoor/outdoor environmental pollution issues. Herein, we successfully synthesized ultrathin LayCoOx nanosheets (thickness of 1.8 nm) with high porosity, using a straightforward co-precipitation method. Comprehensive characterization techniques were employed to analyze the synthesized LayCoOx catalysts, revealing their low crystallinity, high surface area, and abundant porosity. Catalytic benzene oxidation tests demonstrated that the La0.029CoOx-300 nanosheet exhibited the most optimal performance. This catalyst enabled complete benzene degradation at a relatively-low temperature of 220 oC, even under a high space velocity (SV) of 20,000 h-1, and displayed remarkable durability throughout various catalytic assessments, including SV variations, exposure to water vapor, recycling, and long time-on-stream tests. Characterization analyses confirmed the enhanced interactions between Co and doped-La, the presence of abundant adsorbed oxygen, and extensive exposure of Co3+ species in La0.029CoOx-300 nanosheets. Theoretical calculations further revealed that La doping was beneficial for the formation of oxygen vacancies and the adsorption of more hydroxyl groups. These features strongly promoted the adsorption and activation of oxygen, thereby accelerating the benzene oxidation processes. This work underscores the advantages of doping rare-earth elements into transition-metal oxides as a cost-effective yet efficient strategy for purifying industrial exhausts.

Publisher Copyright

This research / project is supported by the National Research Foundation - Competitive Research Programme
Grant Reference no. : NRF-CRP24-2020-0002

This research / project is supported by the A*STAR - Central Research Fund
Grant Reference no. : NA

This work was supported by the National Natural Science Foundation of China (No. 22202024); the Chongqing Science and Technology Foundation (CSTB2022NSCQBHX0021); the China Scholarship Council (No. 202206050117).

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Inorganic Chemistry, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see doi.org/10.1021/acs.inorgchem.3c04621

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