C2N-supported single metal ion catalysts for HCOOH dehydrogenation

Wenhui Zhong; Yuxia Liu; Mingsen Deng; Yachao Zhang; Chuanyi Jia; Oleg V. Prezhdo; Jianyong Yuan; Jun Jiang

doi:10.1039/C8TA02299B

C₂N-supported single metal ion catalysts for HCOOH dehydrogenation†

Wenhui Zhong,^a Yuxia Liu,^b Mingsen Deng,

^a Yachao Zhang,

^a Chuanyi Jia,^a Oleg V. Prezhdo,

^c Jianyong Yuan^d and Jun Jiang

*^e

Author affiliations

* Corresponding authors

^a Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Institute of Applied Physics, Guizhou Synergetic Innovation Center of Scientific Big Data for Advanced Manufacturing Technology, Guizhou Education University, Gaoxin Road 115, Guiyang, Guizhou 550018, P. R. China

^b School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, P. R. China

^c Department of Chemistry, University of Southern California, Los Angeles, California 90089, USA

^d Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Key Laboratory of Advanced Polymeric Materials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China

^e Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), CAS Key Laboratory of Mechanical Behavior and Design of Materials, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, China
E-mail: jiangj1@ustc.edu.cn

Abstract

High catalytic performance of a single-atom transition metal ion (TM^x+) anchored on the two-dimensional (2D) C₂N lattice is predicted for HCOOH dehydrogenation. Considering the Co²⁺, Cu²⁺ and Ni²⁺ non-noble metal ions supported by C₂N, we use density functional theory to demonstrate dehydrogenation energy barriers as low as those for pure Pt and Pd catalysts. The high catalytic performance is ascribed to the reaction occurring through a dual-active center composed of TM^x+ and a nearby N atom of C₂N. Specifically, C₂N–Co²⁺ in the low spin state (S = 1/2) greatly promotes HCOOH dehydrogenation by decreasing the barrier of the rate-determining step to only 0.30 eV, mainly due to the strong ability of TM^x+ to extract charges from HCOOH and C₂N. The obtained mechanistic insights help the rational design of single-atom based transition metal ion catalysts supported by 2D materials.

Supplementary files

Article information

DOI: https://doi.org/10.1039/C8TA02299B
Article type: Communication
Submitted: 12 Mar 2018
Accepted: 15 May 2018
First published: 17 May 2018

Download Citation

J. Mater. Chem. A, 2018,6, 11105-11112

Author version available

Download author version (PDF)

Permissions

Request permissions

C₂N-supported single metal ion catalysts for HCOOH dehydrogenation

W. Zhong, Y. Liu, M. Deng, Y. Zhang, C. Jia, O. V. Prezhdo, J. Yuan and J. Jiang, J. Mater. Chem. A, 2018, 6, 11105 DOI: 10.1039/C8TA02299B

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Journal of Materials Chemistry A