Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles

Yunhu Han, Ziyun Wang, Ruirui Xu, Wei Zhang, Wenxing Chen, Lirong Zheng, Jian Zhang, Jun Luo, Konglin Wu, Youqi Zhu, Chen Chen, Qing Peng, qiang Liu, Peijun Hu, Dingsheng Wang, Yadong Li

Research output: Contribution to journalArticle

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Abstract

Single-atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single-atom sites were stabilized on an ordered porous nitrogen-doped carbon matrix (ISAS-Co/OPNC). ISAS-Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N-heterocycles to release H 2 . ISAS-Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N-heterocycles to store H 2 , using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS-Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious-metal catalysts. The reaction mechanisms are systematically investigated using first-principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
Original languageEnglish
Pages (from-to)11262-11266
JournalAngewandte Chemie International Edition
Volume57
Issue number35
Early online date06 Jul 2018
DOIs
Publication statusPublished - 21 Aug 2018

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Dehydrogenation
Cobalt
Hydrogenation
Nitrogen
Carbon
Catalysts
formic acid
Hydrogen
Atoms
Formic acid
Precious metals
Catalyst activity

Cite this

Han, Yunhu ; Wang, Ziyun ; Xu, Ruirui ; Zhang, Wei ; Chen, Wenxing ; Zheng, Lirong ; Zhang, Jian ; Luo, Jun ; Wu, Konglin ; Zhu, Youqi ; Chen, Chen ; Peng, Qing ; Liu, qiang ; Hu, Peijun ; Wang, Dingsheng ; Li, Yadong. / Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles. In: Angewandte Chemie International Edition. 2018 ; Vol. 57, No. 35. pp. 11262-11266.
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title = "Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles",
abstract = "Single-atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single-atom sites were stabilized on an ordered porous nitrogen-doped carbon matrix (ISAS-Co/OPNC). ISAS-Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N-heterocycles to release H 2 . ISAS-Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N-heterocycles to store H 2 , using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS-Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious-metal catalysts. The reaction mechanisms are systematically investigated using first-principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. {\circledC} 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",
author = "Yunhu Han and Ziyun Wang and Ruirui Xu and Wei Zhang and Wenxing Chen and Lirong Zheng and Jian Zhang and Jun Luo and Konglin Wu and Youqi Zhu and Chen Chen and Qing Peng and qiang Liu and Peijun Hu and Dingsheng Wang and Yadong Li",
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Han, Y, Wang, Z, Xu, R, Zhang, W, Chen, W, Zheng, L, Zhang, J, Luo, J, Wu, K, Zhu, Y, Chen, C, Peng, Q, Liu, Q, Hu, P, Wang, D & Li, Y 2018, 'Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles', Angewandte Chemie International Edition, vol. 57, no. 35, pp. 11262-11266. https://doi.org/10.1002/anie.201805467

Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles. / Han, Yunhu; Wang, Ziyun; Xu, Ruirui; Zhang, Wei; Chen, Wenxing; Zheng, Lirong; Zhang, Jian; Luo, Jun; Wu, Konglin; Zhu, Youqi; Chen, Chen; Peng, Qing; Liu, qiang; Hu, Peijun; Wang, Dingsheng; Li, Yadong.

In: Angewandte Chemie International Edition, Vol. 57, No. 35, 21.08.2018, p. 11262-11266.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles

AU - Han, Yunhu

AU - Wang, Ziyun

AU - Xu, Ruirui

AU - Zhang, Wei

AU - Chen, Wenxing

AU - Zheng, Lirong

AU - Zhang, Jian

AU - Luo, Jun

AU - Wu, Konglin

AU - Zhu, Youqi

AU - Chen, Chen

AU - Peng, Qing

AU - Liu, qiang

AU - Hu, Peijun

AU - Wang, Dingsheng

AU - Li, Yadong

PY - 2018/8/21

Y1 - 2018/8/21

N2 - Single-atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single-atom sites were stabilized on an ordered porous nitrogen-doped carbon matrix (ISAS-Co/OPNC). ISAS-Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N-heterocycles to release H 2 . ISAS-Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N-heterocycles to store H 2 , using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS-Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious-metal catalysts. The reaction mechanisms are systematically investigated using first-principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

AB - Single-atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single-atom sites were stabilized on an ordered porous nitrogen-doped carbon matrix (ISAS-Co/OPNC). ISAS-Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N-heterocycles to release H 2 . ISAS-Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N-heterocycles to store H 2 , using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS-Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious-metal catalysts. The reaction mechanisms are systematically investigated using first-principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

U2 - 10.1002/anie.201805467

DO - 10.1002/anie.201805467

M3 - Article

VL - 57

SP - 11262

EP - 11266

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

SN - 1433-7851

IS - 35

ER -