Fe Single Atoms and Fe2O3 Clusters Liberated from N-Doped Polyhedral Carbon for Chemoselective Hydrogenation under Mild Conditions

Ruirui Yun; Feiyang Zhan; Na Li; Beibei Zhang; Wanjiao Ma; Lirui Hong; Tian Sheng; Liting Du; Baishu Zheng; Shoujie Liu

doi:10.1021/acsami.0c09124

Fe Single Atoms and Fe₂O₃ Clusters Liberated from N-Doped Polyhedral Carbon for Chemoselective Hydrogenation under Mild Conditions

ACS Appl Mater Interfaces. 2020 Jul 29;12(30):34122-34129. doi: 10.1021/acsami.0c09124. Epub 2020 Jul 20.

Authors

Ruirui Yun¹, Feiyang Zhan¹, Na Li¹, Beibei Zhang¹, Wanjiao Ma¹, Lirui Hong¹, Tian Sheng¹, Liting Du², Baishu Zheng³, Shoujie Liu¹

Affiliations

¹ The Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 214001, P. R. China.
² Advanced Analysis and Testing Center, Nanjing Forestry University, Nanjing 210037, P. R. China.
³ Key Laboratory of Theoretical Chemistry and Molecular Simulation, Ministry of Education, School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, P. R. China.

PMID: 32631045
DOI: 10.1021/acsami.0c09124

Abstract

In the area of catalysis, selective reduction of nitro compounds to amino compounds is a colossal challenge due to the existence of competitive reducible functional groups. Herein, an Fe-based catalyst Fe_SAs/Fe₂O_3ACs/N-doped polyhedral carbon (NPC) has been designed and synthesized. As we expected, compared with Fe_SAs and Fe_NPs, Fe_SAs/Fe₂O_3ACs/NPC shows excellent catalytic performance (turnover frequency up to 1923 h^-1, calculated with nitrobenzene), chemoselectivity, and tolerance during the hydrogenation reaction of nitro compounds under room temperature because of the synergistic effects between Fe_SAs and Fe₂O_3ACs. The theoretical calculations show that Fe_SAs prefers to undergo hydrazine decomposition to generate hydrogen and the Fe₂O_3ACs surface is more active toward the nitrobenzene reduction to aniline.

Keywords: Fe single atoms; Fe2O3 clusters; chemoselectivity; synergistic effect; theoretical calculation.