Saved in:
| Main Authors: | , , , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2024
|
| Subjects: | |
| Online Access: | https://arxiv.org/abs/2403.16455 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866929287608664064 |
|---|---|
| author | Wang, Yuchen Liu, Yaoyu Zhao, Zhiyue Zheng, Zhikeng Balu, Alina M. Luque, Rafael Yan, Kai |
| author_facet | Wang, Yuchen Liu, Yaoyu Zhao, Zhiyue Zheng, Zhikeng Balu, Alina M. Luque, Rafael Yan, Kai |
| contents | Electrocatalytic hydrogenation of nitrobenzene (Ph-NO2) reaction (EHNR) has been considered as a potential alternative to the traditional thermocatalytic process in the production of high-value aniline (Ph-NH2). However, due to the absence of robust catalyst and low surface H* coverage, the EHNR faces the challenges of undesired performance and indetermined mechanism. Herein, we construct a type of noble-metal free topological FeSi (M-FeSi) materials through a solvent-free microwave strategy for efficient EHNR in neutral medium. Impressively, benefiting from abundant active H* intermediates on the surface of M-FeSi catalyst, the topological M-FeSi catalyst exhibits 99.7% conversion of Ph-NO2 and 93.8% yield of Ph-NH2 after 200 C in neutral medium, which are superior to previous candidates and FeSi catalyst synthesized via the traditional arc-melting method under same conditions. Besides, theoretical calculations validate that high surface H* coverage over M-FeSi catalyst is conducive to switching the rate-determining step from Ph-NO2* Ph-NO* to Ph-NO* Ph-NHOH*, and thus decreasing the total energy barrier of electrocatalytic Ph-NH2 production. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2403_16455 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Topological iron silicide with H* intermediate modulated surface for efficient electrocatalytic hydrogenation of nitrobenzene in neutral medium Wang, Yuchen Liu, Yaoyu Zhao, Zhiyue Zheng, Zhikeng Balu, Alina M. Luque, Rafael Yan, Kai Chemical Physics Materials Science Electrocatalytic hydrogenation of nitrobenzene (Ph-NO2) reaction (EHNR) has been considered as a potential alternative to the traditional thermocatalytic process in the production of high-value aniline (Ph-NH2). However, due to the absence of robust catalyst and low surface H* coverage, the EHNR faces the challenges of undesired performance and indetermined mechanism. Herein, we construct a type of noble-metal free topological FeSi (M-FeSi) materials through a solvent-free microwave strategy for efficient EHNR in neutral medium. Impressively, benefiting from abundant active H* intermediates on the surface of M-FeSi catalyst, the topological M-FeSi catalyst exhibits 99.7% conversion of Ph-NO2 and 93.8% yield of Ph-NH2 after 200 C in neutral medium, which are superior to previous candidates and FeSi catalyst synthesized via the traditional arc-melting method under same conditions. Besides, theoretical calculations validate that high surface H* coverage over M-FeSi catalyst is conducive to switching the rate-determining step from Ph-NO2* Ph-NO* to Ph-NO* Ph-NHOH*, and thus decreasing the total energy barrier of electrocatalytic Ph-NH2 production. |
| title | Topological iron silicide with H* intermediate modulated surface for efficient electrocatalytic hydrogenation of nitrobenzene in neutral medium |
| topic | Chemical Physics Materials Science |
| url | https://arxiv.org/abs/2403.16455 |