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Title: Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis

Journal Article · · Small
 [1];  [2];  [2];  [3];  [3];  [3];  [2];  [1];  [1];  [4];  [5]; ORCiD logo [2]
  1. Chinese Academy of Sciences, Shanghai (People's Republic of China); Univ. of Chinese Academy of Sciences, Beijing (People's Republic of China)
  2. Chinese Academy of Sciences, Shanghai (People's Republic of China)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Illinois Institute of Technology, Chicago, IL (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)

In this paper, the development of cost-effective catalysts to replace noble metal is attracting increasing interests in many fields of catalysis and energy, and intensive efforts are focused on the integration of transition-metal sites in carbon as noble-metal-free candidates. Recently, the discovery of single-atom dispersed catalyst (SAC) provides a new frontier in heterogeneous catalysis. However, the electrocatalytic application of SAC is still subject to several theoretical and experimental limitations. Further advances depend on a better design of SAC through optimizing its interaction with adsorbates during catalysis. Here, distinctive from previous studies, favorable 3d electronic occupation and enhanced metal-adsorbates interactions in single-atom centers via the construction of nonplanar coordination is achieved, which is confirmed by advanced X-ray spectroscopic and electrochemical studies. The as-designed atomically dispersed cobalt sites within nonplanar coordination show significantly improved catalytic activity and selectivity toward the oxygen reduction reaction, approaching the benchmark Pt-based catalysts. More importantly, the illustration of the active sites in SAC indicates metal-natured catalytic sites and a media-dependent catalytic pathway. Achieving structural and electronic engineering on SAC that promotes its catalytic performances provides a paradigm to bridge the gap between single-atom catalysts design and electrocatalytic applications.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Key Basic Research Program of China; USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1474147
Alternate ID(s):
OSTI ID: 1423700
Journal Information:
Small, Vol. 14, Issue 15; ISSN 1613-6810
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 96 works
Citation information provided by
Web of Science

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Toward Efficient Carbon and Water Cycles: Emerging Opportunities with Single‐Site Catalysts Made of 3d Transition Metals journal November 2019
Atomically Dispersed Binary Co‐Ni Sites in Nitrogen‐Doped Hollow Carbon Nanocubes for Reversible Oxygen Reduction and Evolution journal October 2019
Palladium Dimer Supported on Mo 2 CO 2 (MXene) for Direct Methane to Methanol Conversion journal September 2018
Atomically Dispersed Fe-N x /C Electrocatalyst Boosts Oxygen Catalysis via a New Metal-Organic Polymer Supramolecule Strategy journal July 2018
Rational Design of Graphene-Supported Single Atom Catalysts for Hydrogen Evolution Reaction journal January 2019
Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species journal June 2019
Die facettenreiche Reaktivität heterogener Einzelatom‐Katalysatoren journal November 2018
Nitrogen‐doped Carbon–CoO x Nanohybrids: A Precious Metal Free Cathode that Exceeds 1.0 W cm −2 Peak Power and 100 h Life in Anion‐Exchange Membrane Fuel Cells journal November 2018
The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts journal October 2018
Nitrogen-doped Carbon-CoO x Nanohybrids: A Precious Metal Free Cathode that Exceeds 1.0 W cm −2 Peak Power and 100 h Life in Anion-Exchange Membrane Fuel Cells journal November 2018
The Proportion of Fe‐N X , N Doping Species and Fe 3 C to Oxygen Catalytic Activity in Core‐Shell Fe‐N/C Electrocatalyst journal December 2019
N,P Co‐Coordinated Manganese Atoms in Mesoporous Carbon for Electrochemical Oxygen Reduction journal January 2019
Standing Carbon‐Supported Trace Levels of Metal Derived from Covalent Organic Framework for Electrocatalysis journal October 2019
Uniform Lithium Nucleation Guided by Atomically Dispersed Lithiophilic CoN x Sites for Safe Lithium Metal Batteries journal November 2018
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Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application journal May 2019
Unexpected monoatomic catalytic-host synergetic OER/ORR by graphitic carbon nitride: density functional theory journal January 2019
A review of non-precious metal single atom confined nanomaterials in different structural dimensions (1D–3D) as highly active oxygen redox reaction electrocatalysts journal January 2020
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Nanowrinkled Carbon Aerogels Embedded with FeN x Sites as Effective Oxygen Electrodes for Rechargeable Zinc-Air Battery journal December 2019
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Figures / Tables (4)