Optimizing Microenvironment of Asymmetric N,S-Coordinated Single-Atom Fe via Axial Fifth Coordination toward Efficient Oxygen Electroreduction

Li, Longbin; Huang, Senhe; Cao, Rui; Yuan, Kai; Lu, Chenbao; Huang, Bingyu; Tang, Xiannong; Hu, Ting; Zhuang, Xiaodong; Chen, Yiwang

doi:10.1002/smll.202105387

Optimizing Microenvironment of Asymmetric N,S-Coordinated Single-Atom Fe via Axial Fifth Coordination toward Efficient Oxygen Electroreduction

Journal Article · Sat Nov 20 04:00:00 EST 2021 · Small

DOI:https://doi.org/10.1002/smll.202105387· OSTI ID:1889786

Li, Longbin ^[1]; Huang, Senhe ^[2]; Cao, Rui ^[3]; Yuan, Kai ^[4]; Lu, Chenbao ^[2]; Huang, Bingyu ^[4]; Tang, Xiannong ^[4]; Hu, Ting ^[4]; Zhuang, Xiaodong ^[2]; ^[4]

Nanchang University (China); SLAC
Shanghai Jiao Tong University (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Nanchang University (China)

We report single-atom catalysts (SACs) are attractive candidates for oxygen reduction reaction (ORR). The catalytic performances of SACs are mainly determined by the surrounding microenvironment of single metal sites. Microenvironment engineering of SACs and understanding of the structure–activity relation-ship is critical, which remains challenging. Herein, a self-sacrificing strategy is developed to synthesize asymmetric N,S-coordinated single-atom Fe with axial fifth hydroxy (OH) coordination (Fe-N₃S₁OH) embedded in N,S codoped porous carbon nanospheres (Fe-N/S-C). Such unique penta-coordination microenvironment is determined by cutting-edge techonologies aiding of systematic simulations. The as-obtained Fe-;N/S-C exhibits superior catalytic ORR activity, and showcases a half-wave potential of 0.882 V surpassing the benchmark Pt/C. Moreover, theoretical calculations confirmed the axial OH in Fe-N₃S₁OH can optimize 3d orbitals of Fe center to strengthen O₂ adsorption and enhance O₂ activation on Fe site, thus reducing the ORR barrier and accelerating ORR dynamics. Furthermore, Fe-N/S-C containing H₂-O₂ fuel cell performs a high peak power density of 512 mW cm^-2, and Fe-N/S-C based Zn-air batteries show the peak power density of 203 and 49 mW cm^-2in liquid and flexible all-solid-state configurations, respectively. This study offers a new platform for fundamentally understand the axial fifth coordination in asymmetrical planar single-atom metal sites for electrocatalysis.

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Natural Science Foundation of China; Natural Science Foundation of Jiangxi Province; German Research Foundation

DOE Contract Number:: AC02-76SF00515

OSTI ID:: 1889786

Journal Information:: Small, Journal Name: Small Journal Issue: 2 Vol. 18; ISSN 1613-6810

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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Optimizing Microenvironment of Asymmetric N,S-Coordinated Single-Atom Fe via Axial Fifth Coordination toward Efficient Oxygen Electroreduction

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