Volume 59, Issue 23 pp. 8982-8990
Research Article

Synergistically Interactive Pyridinic-N–MoP Sites: Identified Active Centers for Enhanced Hydrogen Evolution in Alkaline Solution

Dr. Di Zhao

Dr. Di Zhao

Department of Chemistry, Tsinghua University, Beijing, 100084 China

These authors contributed equally to this work.

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Dr. Kaian Sun

Dr. Kaian Sun

Department of Chemistry, Tsinghua University, Beijing, 100084 China

State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580 China

These authors contributed equally to this work.

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Dr. Weng-Chon Cheong

Dr. Weng-Chon Cheong

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Lirong Zheng

Prof. Lirong Zheng

Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049 China

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Dr. Chao Zhang

Dr. Chao Zhang

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Dr. Shoujie Liu

Dr. Shoujie Liu

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Xing Cao

Xing Cao

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Konglin Wu

Konglin Wu

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Dr. Yuan Pan

Dr. Yuan Pan

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Zewen Zhuang

Zewen Zhuang

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Botao Hu

Botao Hu

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Dingsheng Wang

Prof. Dingsheng Wang

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Qing Peng

Prof. Qing Peng

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Chen Chen

Corresponding Author

Prof. Chen Chen

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Prof. Yadong Li

Prof. Yadong Li

Department of Chemistry, Tsinghua University, Beijing, 100084 China

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First published: 13 September 2019
Citations: 325

Graphical Abstract

The effect of the dopant: In the electrocatalyst comprising MoP nanoparticles encapsulated by nitrogen-doped carbon, the sites where MoP interacts with pyridinic N (but not pyrrolic N or graphitic N) lead to increased electron density on the nitrogen-doped carbon, as well as optimized adsorption of H* and OH*, all of which help to accelerate the hydrogen evolution reaction in alkaline media.

Abstract

For electrocatalysts for the hydrogen evolution reaction (HER), encapsulating transition metal phosphides (TMPs) into nitrogen-doped carbon materials has been known as an effective strategy to elevate the activity and stability. Yet still, it remains unclear how the TMPs work synergistically with the N-doped support, and which N configuration (pyridinic N, pyrrolic N, or graphitic N) contributes predominantly to the synergy. Here we present a HER electrocatalyst (denoted as MoP@NCHSs) comprising MoP nanoparticles encapsulated in N-doped carbon hollow spheres, which displays excellent activity and stability for HER in alkaline media. Results of experimental investigations and theoretical calculations indicate that the synergy between MoP and the pyridinic N can most effectively promote the HER in alkaline media.

Conflict of interest

The authors declare no conflict of interest.

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