Single Ir atom anchored in pyrrolic-N4 doped graphene as a promising bifunctional electrocatalyst for the ORR/OER: a computational study

Xinyi Li; Zhanhua Su; Zhifeng Zhao; Qinghai Cai; Yafei Li; Jingxiang Zhao

doi:10.1016/j.jcis.2021.09.045

Single Ir atom anchored in pyrrolic-N₄ doped graphene as a promising bifunctional electrocatalyst for the ORR/OER: a computational study

J Colloid Interface Sci. 2022 Feb;607(Pt 2):1005-1013. doi: 10.1016/j.jcis.2021.09.045. Epub 2021 Sep 11.

Authors

Xinyi Li¹, Zhanhua Su², Zhifeng Zhao³, Qinghai Cai⁴, Yafei Li⁵, Jingxiang Zhao⁶

Affiliations

¹ College of Chemistry and Chemical Engineering, and Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, China.
² College of Chemistry, Guangdong University of Petrochemical Technology, Maoming 525000, China.
³ College of Chemistry, Guangdong University of Petrochemical Technology, Maoming 525000, China. Electronic address: zfzhao@gdupt.edu.cn.
⁴ College of Chemistry and Chemical Engineering, and Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, China; Heilongjiang Province Collaborative Innovation Center of Cold Region Ecological Safety, Harbin 150025, China.
⁵ Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China.
⁶ College of Chemistry and Chemical Engineering, and Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, China. Electronic address: zhaojingxiang@hrbnu.edu.cn.

PMID: 34583028
DOI: 10.1016/j.jcis.2021.09.045

Abstract

The development of highly-efficient electrocatalysts with bifunctional catalytic activity for oxygen reduction reaction (ORR) and oxygen evolution reaction. (OER) still remains a great challenge for the large-scale application of renewable energy conversion and storage technologies. Herein, by means of comprehensive density functional theory (DFT) computations, we systematically explored the potential of pyrrolic-N doped graphene (pyrrolic-N₄-G) supported various transition metal atoms (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Mo, Ru, Pd, W, Os, Ir, and Pt) as electrocatalysts for the ORR and OER. Our results revealed that these TM/pyrrolic-N₄-G candidates exhibit high electrochemical stability due to their positive dissolution potentials. Especially, the Ir/pyrrolic-N₄-G can perform as a promising bifunctional electrocatalyst for both ORR and OER with the low overpotentials (η^ORR = 0.34 V and η^OER = 0.32 V). Interestingly, multiple-level descriptors, including energy descriptor (ΔG_OH* - ΔG_O*), (ΔG_OH*), structure descriptor (φ), and d-band center (ε) can well rationalize the origin of the high catalytic activity of Ir/pyrrolic-N₄-G for the ORR/OER. Our findings not only further enrich the SACs, but also open a new avenue to develop novel 2D materials-based SACs for highly efficient oxygen electrocatalysts.

Keywords: Bifunctional catalysts; DFT; ORR/OER; Single atom catalysts; TM-N/C materials.