Reconstructing the Coordination Environment of Fe/Co Dual-atom Sites towards Efficient Oxygen Electrocatalysis for Zn-Air Batteries

Hengqi Liu; Jinzhen Huang; Kun Feng; Rui Xiong; Shengyu Ma; Ran Wang; Qiang Fu; Moniba Rafique; Zhiguo Liu; Jiecai Han; Daxing Hua; Jiajie Li; Jun Zhong; Xianjie Wang; Zhonglong Zhao; Tai Yao; Sida Jiang; Ping Xu; Zhihua Zhang; Bo Song

doi:10.1002/anie.202419595

Reconstructing the Coordination Environment of Fe/Co Dual-atom Sites towards Efficient Oxygen Electrocatalysis for Zn-Air Batteries

Angew Chem Int Ed Engl. 2024 Nov 14:e202419595. doi: 10.1002/anie.202419595. Online ahead of print.

Authors

Hengqi Liu^{1

2}, Jinzhen Huang^{3

4}, Kun Feng⁵, Rui Xiong⁶, Shengyu Ma², Ran Wang³, Qiang Fu², Moniba Rafique³, Zhiguo Liu², Jiecai Han³, Daxing Hua², Jiajie Li⁷, Jun Zhong⁵, Xianjie Wang², Zhonglong Zhao⁸, Tai Yao³, Sida Jiang⁹, Ping Xu¹⁰, Zhihua Zhang¹¹, Bo Song^{1

2

3

12

13}

Affiliations

¹ National Key Laboratory of Laser Spatial Information, Harbin Institute of Technology, Harbin, 150001, China.
² School of Physics, Harbin Institute of Technology, Harbin, 150001, China.
³ National Key Laboratory of Science and Technology on Advanced Composites in Special Environments, Harbin Institute of Technology, Harbin, 150001, China.
⁴ Electrochemistry Laboratory, Paul Scherrer Institute, CH-5232, Villigen PSI, Switzerland.
⁵ Institute of Functional Nano and Soft Materials Laboratory, Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China.
⁶ School of future technology, Harbin Institute of Technology, Harbin, 150001, China.
⁷ School of Materials Science and Engineering, University of Jinan, Jinan, 250022, China.
⁸ School of Physical Science and Technology, Inner Mongolia University, Hohhot, 010021, China.
⁹ National Key Laboratory of Space Environment and Matter Behaviors, Harbin Institute of Technology, Harbin, 150001, China.
¹⁰ State Key Laboratory of Space Power-Sources, School of Chemistry, Chemical Engineering Harbin Institute of Technology, Harbin, 150001, China.
¹¹ School of Materials Science, Engineering, Dalian Jiaotong University, Dalian, 116028, China.
¹² Laboratory for Space Environment and Physical Sciences, Frontiers Science Center for Matter Behave in Space Environment, Harbin Institute of Technology, Harbin, 150001, China.
¹³ Zhengzhou Research Institute, Harbin Institute of Technology, Zhengzhou, 450046, China.

PMID: 39540704
DOI: 10.1002/anie.202419595

Abstract

Dual-atom catalysts with nitrogen-coordinated metal sites embedded in carbon can drive the oxygen reduction and evolution reactions (ORR/OER) in rechargeable zinc-air batteries (ZABs), and the further improvement is limited by the linear scaling relationship of intermediate binding energies in the absorbate evolution mechanism (AEM). Triggering the lattice oxygen mechanism (LOM) is promising to overcome this challenge, but has yet been verified since the lacking of bridge oxygen (O) in the rigid coordination environment of the metal centers. Here, we demonstrate that suitably tailored dual-atom catalysts of FeCo-N-C can undergo out-plane and in-plane reconstruction to form the both axial O and bridge O at the metal centers, and thus activate the LOM pathway. The tailored FeCo-N-C with shortened Fe-N bonds also favors the ORR process, therefore is a promising dual-atom oxygen catalyst. The assembled rechargeable ZABs demonstrate a peak power density of 332 mW cm^-2, and exhibit no notable decline after ~720 h of continuous cycling.

Keywords: Tailoring coordination environment; lattice oxygen mechanism; oxygen evolution reaction; oxygen reduction reaction; rechargeable zinc–air batteries.

Grants and funding

52225201/National Science Fund for Distinguished Young Scholars