TY - JOUR
T1 - Electron-rich isolated Pt active sites in ultrafine PtFe3 intermetallic catalyst for efficient alkene hydrosilylation
AU - Han, Yunhu
AU - Xiong, Yu
AU - Liu, Chuangwei
AU - Zhang, Hongwei
AU - Zhao, Meiqi
AU - Chen, Wen
AU - Chen, Wenxing
AU - Huang, Wei
N1 - Publisher Copyright:
© 2021 Elsevier Inc.
PY - 2021/4
Y1 - 2021/4
N2 - Regulating electronic structure of active centres to improve the performance of catalysts has always been a notable research topic, in which many challenges still need to be solved urgently. Herein, we report a PtFe3 intermetallic catalyst anchored on N-doped carbon spheres (PtFe3/CN) with electron-rich isolated Pt active sites. The electron-rich nature of isolated Pt sites is attributed to the coordination of low electronegativity iron atoms. The PtFe3/CN catalyst showed a catalytic performance for the hydrosilylation of alkene superior to traditional single-atom Pt catalyst (coordinate with N etc. atoms) loading on N-doped graphene carbon (Pt1/CN) with electron-deficient isolated Pt sites and Pt nanoparticles supported N-doped carbon spheres (Pt NPs/CN) catalysts with the contiguous Pt sites. More importantly, turnover number (TON) of alkene hydrosilylation can reach a striking ca. 740,000 and no Pt leaching was detected. The opinion has been substantiated by both experimental and theoretical results that the PtFe3/CN catalyst can completely catalyze conversion of alkene and exhibit a high selectivity for anti-Markovnikov addition under environmentally friendly and mild conditions.
AB - Regulating electronic structure of active centres to improve the performance of catalysts has always been a notable research topic, in which many challenges still need to be solved urgently. Herein, we report a PtFe3 intermetallic catalyst anchored on N-doped carbon spheres (PtFe3/CN) with electron-rich isolated Pt active sites. The electron-rich nature of isolated Pt sites is attributed to the coordination of low electronegativity iron atoms. The PtFe3/CN catalyst showed a catalytic performance for the hydrosilylation of alkene superior to traditional single-atom Pt catalyst (coordinate with N etc. atoms) loading on N-doped graphene carbon (Pt1/CN) with electron-deficient isolated Pt sites and Pt nanoparticles supported N-doped carbon spheres (Pt NPs/CN) catalysts with the contiguous Pt sites. More importantly, turnover number (TON) of alkene hydrosilylation can reach a striking ca. 740,000 and no Pt leaching was detected. The opinion has been substantiated by both experimental and theoretical results that the PtFe3/CN catalyst can completely catalyze conversion of alkene and exhibit a high selectivity for anti-Markovnikov addition under environmentally friendly and mild conditions.
KW - Electron-rich feature
KW - Hydrosilylation of alkene
KW - Intermetallics
KW - Isolated-Pt-sites catalyst
KW - Size-atomic design strategy
UR - http://www.scopus.com/inward/record.url?scp=85103236575&partnerID=8YFLogxK
U2 - 10.1016/j.jcat.2021.03.004
DO - 10.1016/j.jcat.2021.03.004
M3 - Article
AN - SCOPUS:85103236575
SN - 0021-9517
VL - 396
SP - 351
EP - 359
JO - Journal of Catalysis
JF - Journal of Catalysis
ER -