Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media

DOI: 10.1038/s41467-024-48209-0

Authors: Longxiang Liu (University College London) , Liqun Kang (Max-Planck-Institute for Chemical Energy Conversion) , Jianrui Feng (University College London) , David G. Hopkinson (Diamond Light Source) , Christopher S. Allen (Diamond Light Source; University of Oxford) , Yeshu Tan (University College London) , Hao Gu (University College London) , Iuliia Mikulska (Diamond Light Source) , Veronica Celorrio (Diamond Light Source) , Diego Gianolio (Diamond Light Source) , Tianlei Wang (University College London) , Liquan Zhang (University College London) , Kaiqi Li (University College London) , Jichao Zhang (University College London) , Jiexin Zhu (University College London) , Georg Held (Diamond Light Source) , Pilar Ferrer (Diamond Light Source) , David Grinter (University College London) , June Callison (UK Catalysis Hub, Research Complex at Harwell) , Martin Wilding (UK Catalysis Hub, Research Complex at Harwell) , Sining Chen (University College London) , Ivan Parkin (University College London) , Guanjie He (University College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 15

State: Published (Approved)
Published: May 2024
Diamond Proposal Number(s): 30614 , 32058 , 32035 , 32117 , 33466 , 29271

Abstract: Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped carbon, have demonstrated considerable EHPP efficiency. However, their full potential, particularly regarding the correlation between structural configurations and performances in neutral media, remains underexplored. Herein, a series of ultralow metal-loading M-N-C electrocatalysts are synthesized and investigated for the EHPP process in the neutral electrolyte. CoNCB material with the asymmetric Co-C/N/O configuration exhibits the highest EHPP activity and selectivity among various as-prepared M-N-C electrocatalyst, with an outstanding mass activity (6.1 × 105 A gCo−1 at 0.5 V vs. RHE), and a high practical H2O2 production rate (4.72 mol gcatalyst−1 h−1 cm−2). Compared with the popularly recognized square-planar symmetric Co-N4 configuration, the superiority of asymmetric Co-C/N/O configurations is elucidated by X-ray absorption fine structure spectroscopy analysis and computational studies.

Subject Areas: Materials, Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B07-B1-Versatile Soft X-ray beamline: High Throughput ES1 , B18-Core EXAFS , E02-JEM ARM 300CF

Added On: 15/05/2024 13:27

Documents:
s41467-024-48209-0.pdf

Discipline Tags:

Physical Chemistry Chemistry Materials Science

Technical Tags:

Microscopy Spectroscopy Electron Microscopy (EM) Transmission Electron Microscopy (TEM) X-ray Absorption Spectroscopy (XAS) Near Edge X-ray Absorption Fine Structures (NEXAFS)