Citation: Guifang Ge, Xiaojing Wei, Hongchen Guo, Zhongkui Zhao. An efficient nanodiamond-based monolithic foam catalyst prepared by a facile thermal impregnation strategy for direct dehydrogenation of ethylbenzene to styrene[J]. Chinese Chemical Letters, ;2023, 34(5): 107808. doi: 10.1016/j.cclet.2022.107808 shu

An efficient nanodiamond-based monolithic foam catalyst prepared by a facile thermal impregnation strategy for direct dehydrogenation of ethylbenzene to styrene

State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China

zkzhao@dlut.edu.cn

Received Date: 5 January 2022
Revised Date: 23 August 2022
Accepted Date: 5 September 2022
Available Online: 9 September 2022

Figures(4)

Nanodiamond (ND) has long been recognized as an effective carbocatalyst for synthesizing styrene via direct dehydrogenation (DDH). However, the induced drastic pressure drop of its powder form limits its industrial application in heterogeneous catalytic process. In this work, we report a facile hexamethylenetetramine nitrate (HN)-assisted thermal impregnation (HNTI) strategy for fabricating a novel nanodiamond-based monolithic foam (ND/CNT-SiC-ms-HN) catalyst through a two-step approach: One is to soak the carbon nanotube-modified SiC foam (CNT-SiC) with the slurry composed of HN, KCl, LiCl, and dispersed ND, and the other is to heat the slurry-soaked CNT-SiC (ND-HN-KCl-LiCl/CNT-SiC) in N₂ atmosphere at 750 ℃. The as-synthesized ND/CNT–SiC-ms-HN monolithic foam features the enriched surface kenotic CO by promoted ND dispersion and O-doping, abundant stuctural defects, and improved nucleophilicity by N-doping, originating from the promoted ND dispersion by thermal impregnation (TI) in KCl-LiCl molten salt (MS) and the presence of HN in the annealing process. As a result, the ND/CNT–SiC-ms-HN monolithic foam catalyst by HNTI strategy exhibits 1.5 folds higher steady-state styrene rate (5.49 mmol g⁻¹ h⁻¹) associated with 98.4% of styrene selectivity compared to the ND-based monolithic foam catalyst (ND/CNT-SiC). Moreover, the ND/CNT–SiC-ms-HN monolithic foam shows excellent long-term stability for the direct dehydrogenation of ethylbenzene to styrene. This work also comes up with a novel way of preparing other highly-dispersed nanocarbons-based monolithic foam catalysts with promising catalytic performance for diverse transformations.
- Nanodiamond-based monolithic foam,
- Heterogeneous catalysis,
- Thermal impregnation,
- Ethylbenzene direct dehydrogenation,
- Styrene production
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