Laser-Irradiated Holey Graphene-Supported Single-Atom Catalyst towards Hydrogen Evolution and Oxygen Reduction

Khan, Kishwar; Liu, Tangchao; Arif, Muhammad; Yan, Xingxu; Hossain, Md Delowar; Rehman, Faisal; Zhou, Sheng; Yang, Jing; Sun, Chengjun; Bae, Sang‐Hoon; Kim, Jeehwan; Amine, Khalil; Pan, Xiaoqing; Luo, Zhengtang

doi:10.1002/aenm.202101619

Title: Laser-Irradiated Holey Graphene-Supported Single-Atom Catalyst towards Hydrogen Evolution and Oxygen Reduction

Journal Article · Wed Sep 15 00:00:00 EDT 2021 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202101619· OSTI ID:1854518

Khan, Kishwar ^[1]; Liu, Tangchao ^[2]; Arif, Muhammad ^[3]; Yan, Xingxu ^[4]; Hossain, Md Delowar ^[1]; Rehman, Faisal ^[1]; Zhou, Sheng ^[5]; Yang, Jing ^[5]; Sun, Chengjun ^[2]; Bae, Sang‐Hoon ^[6]; Kim, Jeehwan ^[7]; Amine, Khalil ^[8]; Pan, Xiaoqing ^[4];

^[1]

The Hong Kong Univ. of Science and Technology, Kowloon (Hong Kong)
Argonne National Lab. (ANL), Lemont, IL (United States)
Northwestern Polytechnical Univ. (NPU), Xi'an (China)
Univ. of California, Irvine, CA (United States)
Tianjin Univ. (China)
Washington Univ., St. Louis, MO (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States); Stanford Univ., CA (United States); Imam Abdulrahman Bin Faisal Univ. (IAU), Dammam (Saudi Arabia)

Abstract Single‐atom catalysts (SAC) can boost the intrinsic catalytic activity of hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). However, the challenge remains due to the complex synthesis process and insufficient stability. A sustainable approach is applied to synthesizing SACs through laser irradiation and gaining mesoporous graphene oxide (MGO). The surface dangling bonds of nitrogen‐doped MGO (NMGO) extract metal atoms species from Co or Fe metal foams and convert them to SAC via an appropriate synthesis approach. Notably, the Co‐NMGO electrocatalyst requires low potentials of 146 mV to convey a current density of 10 mA cm ⁻² towards HER. Similarly, the Fe‐NMGO electrocatalyst offers an onset of 0.79 V towards ORR in acidic solution. The individual metal atoms are confirmed via aberration‐corrected scanning transmission electron microscopy, and X‐ray absorption near‐edge structure and extended X‐ray absorption fine structure. Density functional theory calculations by applying the grand canonical potential kinetics model revealed that Co‐NMGO shows the optimum free reaction energy of −0.17 eV at −0.1 V for HER, and Fe‐NMGO has less limiting potential than that of Co‐NMGO for ORR case. This work opens a new approach towards the synthesis of SAC and its mechanistic understandings.

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1854518

Alternate ID(s):: OSTI ID: 1820222

Journal Information:: Advanced Energy Materials, Vol. 11, Issue 40; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
dangling bonds
grand canonical potential kinetics
laser irradiation
nanocarbon support
porous structures
single-atom catalysts

Title: Laser-Irradiated Holey Graphene-Supported Single-Atom Catalyst towards Hydrogen Evolution and Oxygen Reduction

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