Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts

Shengwen Liu, Maoyu Wang, Xiaoxuan Yang, Qiurong Shi, Zhi Qiao, Marcos Lucero, Qing Ma, Karren L. More, David A. Cullen, Zhenxing Feng, Gang Wu

Research output: Contribution to journalArticlepeer-review

159 Scopus citations

Abstract

Atomically dispersed and nitrogen coordinated single metal sites (M-N-C, M=Fe, Co, Ni, Mn) are the popular platinum group-metal (PGM)-free catalysts for many electrochemical reactions. Traditional wet-chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M-N-C catalysts. The deposition of gaseous 2-methylimidazole onto M-doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD-derived Fe-N-C catalyst exclusively contains atomically dispersed FeN4 sites with increased Fe loading relative to other catalysts from wet-chemistry synthesis. The catalyst exhibited outstanding oxygen-reduction activity in acidic electrolytes, which was further studied in proton-exchange membrane fuel cells with encouraging performance.

Original languageEnglish
Pages (from-to)21698-21705
Number of pages8
JournalAngewandte Chemie - International Edition
Volume59
Issue number48
DOIs
StatePublished - Nov 23 2020

Funding

The authors acknowledge the financial support from the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technology Office (DE‐EE0008075, DE‐EE0008076, and DE‐EE0008417) along with the National Science Foundation (CBET‐1604392, 1804326). Z.F. thanks for the startup funding from Oregon State University. This X‐ray absorption spectroscopy research used resources of the beamline 5‐BM, DND‐CAT at the Advanced Photon Source (APS) that is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE‐AC02‐06CH11357. DND‐CAT is supported through E. I. duPont de Nemours & Co., Northwestern University, and The Dow Chemical Company. The authors acknowledge the financial support from the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technology Office (DE-EE0008075, DE-EE0008076, and DE-EE0008417) along with the National Science Foundation (CBET-1604392, 1804326). Z.F. thanks for the startup funding from Oregon State University. This X-ray absorption spectroscopy research used resources of the beamline 5-BM, DND-CAT at the Advanced Photon Source (APS) that is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. DND-CAT is supported through E. I. duPont de Nemours & Co., Northwestern University, and The Dow Chemical Company.

Keywords

  • Fe-N-C
  • chemical vapor deposition
  • electrocatalysis
  • oxygen reduction reaction
  • single metal sites

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