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Title: Stone-Wales defect-rich carbon-supported dual-metal single atom sites for Zn-air batteries

Journal Article · · Nano Energy
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [6];  [7];  [3];  [5];  [3];  [8];  [2];  [1]
  1. Hong Kong University of Science and Technology (HKUST) (Hong Kong)
  2. Univ. of California, Irvine, CA (United States)
  3. Tsinghua Univ., Beijing (China)
  4. Washington Univ., St. Louis, MO (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Griffith University, Gold Coast, QLD (Australia)
  6. Argonne National Lab. (ANL), Argonne, IL (United States)
  7. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  8. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)

In this study, we aim to obtain a fundamental understanding of active sites near stone-wales (SW) defects rich nitrogen-doped graphene (DG) with specific coordination of carbon atom rings. It reveals that the SW rich defects (e.g., pentagon (5), pentagon—octagon—pentagon (i.e. 585), or pentagon-heptagon-heptagon-pentagon (5775) rings, appears correspondingly with carbon rings that brought active sites during catalytic reactions. Moreover, we anchored dual isolated metallic atoms (Ni/Fe) on DG support via linkers (O/N) called NiFe-DG. X-ray absorption spectroscopy indicates Ni/Fe metal single atoms are embedded via Fe-N4 and Ni-N4 coordination on DG surfaces. It exhibits high catalytic activity for oxygen reduction reaction (ORR) with an onset potential of 0.97 V, a half-wave potential of 0.86 V, and diffusion current density of 5.7 mA cm– 2, which is at par with commercial Pt/C. The catalyst shows superior stability, retained 82% of the initial current density even after 12 h under an applied potential of 0.86 V. Similarly, the oxygen evolution reaction (OER) overpotential of 358 mV was achieved at 10 mA cm– 2 with a lower Tafel slope value (76 mV/dec) than commercial Pt/C. It maintains 85% stability for 12 h at a constant potential of 1.588 V, shows better stability than commercial Pt/C.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC); Zhongshan City Bureau of Science and Technology; Guangdong-Hong Kong-Macao Intelligent Micro-Nano Optoelectronic Technology Joint Laboratory
Grant/Contract Number:
AC02-06CH11357; 2019AG018; 2020B1212030010
OSTI ID:
1878233
Journal Information:
Nano Energy, Vol. 90; ISSN 2211-2855
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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