Graphene-supported single atom catalysts for high performance lithium-oxygen batteries

Wong, Hoilun; Liu, Tongchao; Tamtaji, Mohsen; Huang, Xiaozhou; Tang, Tsz Wing; Hossain, Md Delowar; Wang, Jun; Cai, Yuting; Liu, Zhenjing; Liu, Hongwei; Amine, Khalil; Goddard, III, William A.; Luo, Zhengtang

doi:10.1016/j.nanoen.2024.109279

Graphene-supported single atom catalysts for high performance lithium-oxygen batteries

Journal Article · Thu Jan 11 00:00:00 EST 2024 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2024.109279· OSTI ID:2500314

Wong, Hoilun ^[1]; Liu, Tongchao ^[2]; Tamtaji, Mohsen ^[1]; Huang, Xiaozhou ^[2]; Tang, Tsz Wing ^[1]; Hossain, Md Delowar ^[1]; Wang, Jun ^[1]; Cai, Yuting ^[1]; Liu, Zhenjing ^[1]; Liu, Hongwei ^[1]; Amine, Khalil ^[2]; Goddard, III, William A. ^[3]; Luo, Zhengtang ^[1]

Hong Kong University of Science and Technology (HKUST) (Hong Kong)
Argonne National Laboratory (ANL), Argonne, IL (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)

The optimal choice of d-block metals in single atom catalysts (SACs) is crucial for designing efficient electrocatalysts for activating the Oxygen reduction reaction (ORR)/ Oxygen evolution reaction (OER) in lithiumoxygen batteries (LOBs). Herein, we used the Quantum Mechanics methods to understand the origin of reactivity for a series of 16 d-block metals supported on nitrogen-doped graphene as SACs for ORR and OER in LOBs. Based on the Gibbs free energy calculations, we found that among the 16 SACs investigated, Zn-SAC exhibits the highest electrochemical activity with the lowest overpotential of 0.17 V. Here we then used machine learning (ML) to develop an intrinsic descriptor, phi, that correlates the catalytic activity with electronic and chemical properties of the catalytic centers at the M-N₄ active site on graphene surface. We established a linear relationship between phi and the catalytic activity that provides guidance for designing efficient SACs for electrocatalysis in LOBs. To validate these predictions, we report electrochemical measurements showing that Zn-SAC exhibits an ultra-stable cyclability with reduced overpotentials over Mo-SAC and nitrogen-doped graphene (NG), confirming our theoretical prediction. This fundamental work provides a deep understanding on the rational design of efficient SACs for OER/ ORR in LOBs.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2500314

Journal Information:: Nano Energy, Journal Name: Nano Energy Vol. 121; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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