One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation

Youqi Zhu; Tai Cao; Chuanbao Cao; Jun Luo; Wenxing Chen; Lirong Zheng; Juncai Dong; Jian Zhang; Yunhu Han; Zhi Li; Chen Chen; Qing Peng; Dingsheng Wang; Yadong Li

doi:10.1021/acscatal.8b02624

One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation

Youqi Zhu, Tai Cao, Chuanbao Cao^*, Jun Luo, Wenxing Chen, Lirong Zheng, Juncai Dong, Jian Zhang, Yunhu Han, Zhi Li, Chen Chen, Qing Peng, Dingsheng Wang, Yadong Li

^*Corresponding author for this work

School of Material Science and Engineering

Research output: Contribution to journal › Article › peer-review

125 Citations (Scopus)

Abstract

Development of noble-metal single atomic site catalysts with high metal loading is highly required for many important chemical reactions but proves to be very challenging. Herein, we report a Na₂CO₃ salt-assisted one-pot pyrolysis strategy from EDTA-Pt complex to N-doped graphene with isolated Pt single atomic sites (Pt-ISA/NG) with Pt loading up to 5.3 wt %. The X-ray absorption fine structure analysis and spherical aberration-correction electron microscopy demonstrate an atomic dispersion of single Pt species on graphene support and stabilized by nitrogen in Pt-N₄ structure. The Pt-ISA/NG catalyst exhibits high catalytic activity and reusability for anti-Markovnikov hydrosilylation of various terminal alkenes with industrially relevant tertiary silanes under mild conditions. In hydrosilylation of 1-octene, the Pt-ISA/NG catalyst delivers an overall turnover frequency of 180 h^-1, which is a 4-fold enhancement compared with commercial Pt/C.

Original language	English
Pages (from-to)	10004-10011
Number of pages	8
Journal	ACS Catalysis
Volume	8
Issue number	11
DOIs	https://doi.org/10.1021/acscatal.8b02624
Publication status	Published - 2 Nov 2018

Keywords

N-doped graphene
hydrosilylation
platinum
single atomic site catalyst
two-dimensional nanostructure

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10.1021/acscatal.8b02624

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title = "One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation",

abstract = "Development of noble-metal single atomic site catalysts with high metal loading is highly required for many important chemical reactions but proves to be very challenging. Herein, we report a Na2CO3 salt-assisted one-pot pyrolysis strategy from EDTA-Pt complex to N-doped graphene with isolated Pt single atomic sites (Pt-ISA/NG) with Pt loading up to 5.3 wt %. The X-ray absorption fine structure analysis and spherical aberration-correction electron microscopy demonstrate an atomic dispersion of single Pt species on graphene support and stabilized by nitrogen in Pt-N4 structure. The Pt-ISA/NG catalyst exhibits high catalytic activity and reusability for anti-Markovnikov hydrosilylation of various terminal alkenes with industrially relevant tertiary silanes under mild conditions. In hydrosilylation of 1-octene, the Pt-ISA/NG catalyst delivers an overall turnover frequency of 180 h-1, which is a 4-fold enhancement compared with commercial Pt/C.",

keywords = "N-doped graphene, hydrosilylation, platinum, single atomic site catalyst, two-dimensional nanostructure",

author = "Youqi Zhu and Tai Cao and Chuanbao Cao and Jun Luo and Wenxing Chen and Lirong Zheng and Juncai Dong and Jian Zhang and Yunhu Han and Zhi Li and Chen Chen and Qing Peng and Dingsheng Wang and Yadong Li",

note = "Publisher Copyright: {\textcopyright} 2018 American Chemical Society.",

year = "2018",

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doi = "10.1021/acscatal.8b02624",

language = "English",

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T1 - One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation

AU - Zhu, Youqi

AU - Cao, Tai

AU - Cao, Chuanbao

AU - Luo, Jun

AU - Chen, Wenxing

AU - Zheng, Lirong

AU - Dong, Juncai

AU - Zhang, Jian

AU - Han, Yunhu

AU - Li, Zhi

AU - Chen, Chen

AU - Peng, Qing

AU - Wang, Dingsheng

AU - Li, Yadong

PY - 2018/11/2

Y1 - 2018/11/2

N2 - Development of noble-metal single atomic site catalysts with high metal loading is highly required for many important chemical reactions but proves to be very challenging. Herein, we report a Na2CO3 salt-assisted one-pot pyrolysis strategy from EDTA-Pt complex to N-doped graphene with isolated Pt single atomic sites (Pt-ISA/NG) with Pt loading up to 5.3 wt %. The X-ray absorption fine structure analysis and spherical aberration-correction electron microscopy demonstrate an atomic dispersion of single Pt species on graphene support and stabilized by nitrogen in Pt-N4 structure. The Pt-ISA/NG catalyst exhibits high catalytic activity and reusability for anti-Markovnikov hydrosilylation of various terminal alkenes with industrially relevant tertiary silanes under mild conditions. In hydrosilylation of 1-octene, the Pt-ISA/NG catalyst delivers an overall turnover frequency of 180 h-1, which is a 4-fold enhancement compared with commercial Pt/C.

AB - Development of noble-metal single atomic site catalysts with high metal loading is highly required for many important chemical reactions but proves to be very challenging. Herein, we report a Na2CO3 salt-assisted one-pot pyrolysis strategy from EDTA-Pt complex to N-doped graphene with isolated Pt single atomic sites (Pt-ISA/NG) with Pt loading up to 5.3 wt %. The X-ray absorption fine structure analysis and spherical aberration-correction electron microscopy demonstrate an atomic dispersion of single Pt species on graphene support and stabilized by nitrogen in Pt-N4 structure. The Pt-ISA/NG catalyst exhibits high catalytic activity and reusability for anti-Markovnikov hydrosilylation of various terminal alkenes with industrially relevant tertiary silanes under mild conditions. In hydrosilylation of 1-octene, the Pt-ISA/NG catalyst delivers an overall turnover frequency of 180 h-1, which is a 4-fold enhancement compared with commercial Pt/C.

KW - N-doped graphene

KW - hydrosilylation

KW - platinum

KW - single atomic site catalyst

KW - two-dimensional nanostructure

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U2 - 10.1021/acscatal.8b02624

DO - 10.1021/acscatal.8b02624

M3 - Article

AN - SCOPUS:85054373744

SN - 2155-5435

VL - 8

SP - 10004

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JO - ACS Catalysis

JF - ACS Catalysis

IS - 11

ER -

One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation

Abstract

Keywords

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