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Highly efficient catalyst for 1,1,2-trichloroethane dehydrochlorination via BN3 frustrated Lewis acid-base pairs

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Abstract

In this study, a novel non-metallic carbon-based catalyst co-doped with boron and nitrogen (B,N) was successfully synthesized. By precisely controlling the carbonization temperature of a binary mixed ionic liquid, we selectively modified the doping site structure, ultimately constructing a B,N co-doped frustrated Lewis acid-base pair catalyst. This catalyst exhibited remarkable catalytic activity, selectivity, and stability in the dehydrochlorination reaction of 1,1,2-trichloroethane (TCE). Detailed characterization and theoretical calculations revealed that the primary active center of this catalyst was the BN3 configuration. Compared to conventional graphitic N structures, the BN3 structure had a higher p-band center, ensuring superior adsorption and activation capabilities for TCE during the reaction. Within the BN3 site, three negatively charged nitrogen atoms acted as Lewis bases, while positively charged boron atoms acted as Lewis acids. This synergistic interaction facilitated the specific dissociation of chlorine and hydrogen atoms from TCE, significantly enhancing the 1,1-dichloroethene selectivity. Through this research, we not only explored the active site structure and catalytic mechanism of B,N co-doped catalysts in depth but also provided an efficient, selective, and stable catalyst for the dehydrochlorination of TCE, contributing significantly to the development of nonmetallic catalysts.

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Acknowledgements

The authors acknowledge the funding support from the National Natural Science Foundation of China (Nos. 22202036 and 22302001) and the Jilin Province Scientific, the Technological Planning Project of China (No. 20230101292JC).

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Authors and Affiliations

  1. School of Chemical Engineering, Northeast Electric Power University, Jilin, 132012, China

    Yuxue Yue, Fangmin Zuo, Bolin Wang, Haifeng Zhang & Zilong Zhang

  2. Industrial Catalysis Institute of Zhejiang University of Technology, Hangzhou, 310014, China

    Yuxue Yue

  3. Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, China

    Xiaoling Xian & Wei Chen

  4. College of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan, 243002, China

    Jun Tang & Qingping Ke

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  1. Yuxue Yue
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Correspondence to Bolin Wang, Qingping Ke or Wei Chen.

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Yue, Y., Zuo, F., Wang, B. et al. Highly efficient catalyst for 1,1,2-trichloroethane dehydrochlorination via BN3 frustrated Lewis acid-base pairs. Nano Res. 17, 4773–4781 (2024). https://doi.org/10.1007/s12274-024-6423-x

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