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Research Article

Electron modulation by atomic Ir site decoration in porous Co/N co-doped carbon for electrocatalytic hydrogen evolution

Youkui Zhang1,2( ), Zitong Yan1, Yeli Gao1, Yaqin Fu1, Wenhao Li1, Yunxiang Lin3, Chuanqiang Wu3, Yujuan Pu4, Tao Duan1, Li Song2( )
State Key Laboratory of Environment-Friendly Energy Materials, National Co-Innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang 621010, China
National Synchrotron Radiation Laboratory, Chinese Academy of Sciences (CAS) Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230029, China
Institute of Physical Science and Information Technology, School of Materials Science and Engineering, Anhui Key Laboratory of Information Materials and Devices, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei 230601, China
College of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331, China
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Graphical Abstract

A novel hybrid nanostructure with iridium (Ir) and cobalt (Co) atomic-pair configuration anchored in porous nitrogen-doped carbon (pNC) nanosheet (denoted as IrCo-pNC) is constructed for electrocatalytic hydrogen evolution reaction (HER). The interaction between Ir and Co atoms in pNC causes the locally asymmetric electron distribution, thus contributing to significantly improved HER performance.

Abstract

The rational design of materials at atomic scale as efficient and stable electrocatalysts for hydrogen evolution reaction (HER) is critical for energy conversion. Herein, we report a novel hybrid nanostructure with iridium (Ir) and cobalt (Co) atomic pair configuration anchored in porous nitrogen-doped carbon (pNC) nanosheets (denoted as IrCo-pNC) for electrocatalytic HER. Experimental investigations and theoretical calculations reveal that the interaction between Ir and Co species in pNC promotes electron accumulation and depletion around isolated Ir and Co atoms, respectively, resulting in a local asymmetry electron density distribution. Density functional theory calculations also suggest that the electrons transfer from Co to adjacent Ir atom causing the down shift of the d-band center of Ir 5d in IrCo-pNC catalyst, thus optimizing the adsorption of hydrogen on Ir sites. The as-prepared IrCo-pNC exhibits significant HER performance with an overpotential of 21 mV to achieve a current density of 10 mA·cm−2 in 0.5 M H2SO4. This work provides insight into the role of asymmetry electron density distribution in nanomaterials in regulating HER electrocatalysis.

Keywords

electron modulationiridium decorationporous carbonelectrocatalysishydrogen evolution reaction

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Nano Research
Volume 16 Issue 2,
February 2023
Pages 2011-2019
DOI: 10.1007/s12274-022-4855-8
Cite this article:
Zhang Y, Yan Z, Gao Y, et al. Electron modulation by atomic Ir site decoration in porous Co/N co-doped carbon for electrocatalytic hydrogen evolution. Nano Research, 2023, 16(2): 2011-2019. https://doi.org/10.1007/s12274-022-4855-8
Topics:
Electrocatalysis

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Received: 21 June 2022
Revised: 29 July 2022
Accepted: 02 August 2022
Published: 03 September 2022
© Tsinghua University Press 2022
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