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Binary Atomically Dispersed Metal-Site Catalysts with Core–Shell Nanostructures for O2 and CO2 Reduction Reactions

Journal Article · · Small Science
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [2];  [5]
  1. Northeast Normal Univ., Changchun (China). Key Lab. of Polyoxometetalate Science; State Univ. of New York (SUNY), Buffalo, NY (United States)
  2. Oregon State Univ., Corvallis, OR (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. State Univ. of New York (SUNY), Buffalo, NY (United States)
  6. Northeast Normal Univ., Changchun (China). Key Lab. of Polyoxometetalate Science
Engineering atomically dispersed metal site catalysts with controlled local coordination environments and 3D nanostructures effectively improves the catalytic performance for the oxygen reduction reaction (ORR) and the carbon dioxide reduction reaction (CO2RR), which are critical for clean energy conversion and chemical production. Herein, an innovative approach for preparing core-shell nanostructured catalysts with different single-metal sites in the core and the shell, respectively, is developed. In particular, as the shell precursors, covalent organic polymers with a thin layered structure that is polymerized in situ and coated on a metal-doped ZIF-derived carbon core are used, followed by a controlled thermal activation. The selective combination and construction of different metal sites increase active site density in the surface layers, promote structural robustness, facilitate mass/charge transfer, and yield a possible synergy of active sites in the core and the shell. The p-FeNC(shell)@CoNC(core), consisting of a polymerized FeTPPCl-derived carbon layer (p-FeNC) on a Co-doped ZIF-derived carbon (CoNC), exhibits remarkable ORR activity and stability in acidic media along with encouraging durability in H2–air fuel cells. Likewise, a p-FeNC(shell)@NiNC(core) catalyst demonstrates outstanding CO2RR activity and stability. Hence, integrating two appropriate single-metal sites in core and shell precursors, respectively, can modulate morphological and catalytic properties for a possible synergy toward different electrocatalysis processes.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
Fundamental Research Funds for the Central Universities; Jilin Provincial Education Department; National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Natural Science Foundation of Jilin Province; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1813129
Journal Information:
Small Science, Journal Name: Small Science Journal Issue: 10 Vol. 1; ISSN 2688-4046
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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