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Title: Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction

Journal Article · · Advanced Materials
 [1];  [1];  [2];  [1];  [3];  [1];  [4];  [4]; ORCiD logo [5];  [6];  [7]; ORCiD logo [5];  [1]
  1. Curtin Univ., Perth, WA (Australia)
  2. Australian Synchrotron, Clayton (Australia)
  3. Univ. of Western Australia, Perth, WA (Australia)
  4. Chinese Academy of Sciences (CAS), Shenyang (China)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Curtin Univ., Perth, WA (Australia); Univ. of Sunshine Coast, Queensland (Australia); Univ. of Queensland, Brisbane, QLD (Australia)
  7. Chinese Academy of Sciences (CAS), Shenyang (China); Tsinghua Univ., Shenzhua (China); King Abdulaziz Univ., Jeddah (Saudi Arabia)

Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Organization:
Australian Research Council; National Science Foundation (NSF); National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231; DP150102044; DP150102025; LE120100026; ACI-1053575; 51521091
OSTI ID:
1846560
Alternate ID(s):
OSTI ID: 1419993; OSTI ID: 1543459
Journal Information:
Advanced Materials, Vol. 30, Issue 13; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 467 works
Citation information provided by
Web of Science

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From Molecular Precursors to Nanoparticles—Tailoring the Adsorption Properties of Porous Carbon Materials by Controlled Chemical Functionalization journal January 2020
Carbon-Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage journal August 2018
Recent Advances in Electrochemical CO 2 -to-CO Conversion on Heterogeneous Catalysts journal August 2018
Harnessing the Wisdom in Colloidal Chemistry to Make Stable Single-Atom Catalysts journal July 2018
Synthesis and Applications of Graphdiyne‐Based Metal‐Free Catalysts journal September 2018
Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals journal December 2018
Iron‐Free Cathode Catalysts for Proton‐Exchange‐Membrane Fuel Cells: Cobalt Catalysts and the Peroxide Mitigation Approach journal December 2018
Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries journal March 2019
Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO 2 Electroreduction journal August 2019
Catalysis of a Single Transition Metal Site for Water Oxidation: From Mononuclear Molecules to Single Atoms journal December 2019
Enzymes Immobilized on Carbon Nitride (C 3 N 4 ) Cooperating with Metal Nanoparticles for Cascade Catalysis journal January 2019
Iron Single Atoms on Graphene as Nonprecious Metal Catalysts for High‐Temperature Polymer Electrolyte Membrane Fuel Cells journal March 2019
Orbital Interactions in Bi-Sn Bimetallic Electrocatalysts for Highly Selective Electrochemical CO 2 Reduction toward Formate Production journal September 2018
Densely Populated Isolated Single CoN Site for Efficient Oxygen Electrocatalysis journal April 2019
A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel journal November 2019
Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion journal November 2019
In Situ Thermal Atomization To Convert Supported Nickel Nanoparticles into Surface-Bound Nickel Single-Atom Catalysts journal October 2018
Isolated Diatomic Ni‐Fe Metal–Nitrogen Sites for Synergistic Electroreduction of CO 2 journal April 2019
When Nanozymes Meet Single‐Atom Catalysis journal October 2019
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Reaction Mechanisms of Well-Defined Metal-N 4 Sites in Electrocatalytic CO 2 Reduction journal November 2018
Metal-Organic-Framework-Derived Hollow N-Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion journal January 2019
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When Nanozymes Meet Single‐Atom Catalysis journal February 2020
Single Atom Catalysts on Carbon-Based Materials journal November 2018
Metal Ionic Liquids Produce Metal‐Dispersed Carbon‐Nitrogen Networks for Efficient CO 2 Electroreduction journal June 2019
Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO 2 Reduction journal October 2019
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Rational Design of Ag‐Based Catalysts for the Electrochemical CO 2 Reduction to CO: A Review journal December 2019
Electrochemical CO 2 Reduction to C 1 Products on Single Nickel/Cobalt/Iron‐Doped Graphitic Carbon Nitride: A DFT Study journal November 2019
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Supported Single Atoms as New Class of Catalysts for Electrochemical Reduction of Carbon Dioxide journal February 2019
Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application journal May 2019
Densely Populated Single Atom Catalysts journal November 2019
Microwave absorbing and infrared radiation properties of Al@multi-walled carbon nanotubes composites journal October 2019
In situ synthesis of surfactant-free Pt nanoparticles supported on multi-walled carbon nanotubes under visible light journal October 2019
A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts journal September 2018
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Unusual synergetic effect of nickel single atoms on the electrocatalytic activity of palladium for alcohol oxidation reactions in alkaline media journal January 2018
Atomically dispersed Ni as the active site towards selective hydrogenation of nitroarenes journal January 2019
Heteroatom-doped carbon materials and their composites as electrocatalysts for CO 2 reduction journal January 2018
Single Sb sites for efficient electrochemical CO 2 reduction journal January 2019
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Poly-phenylenediamine-derived atomically dispersed Ni sites for the electroreduction of CO 2 to CO journal January 2019
Cu x Ni y alloy nanoparticles embedded in a nitrogen–carbon network for efficient conversion of carbon dioxide journal January 2019
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Mesoporous Nitrogen‐Doped Carbon‐Nanosphere‐Supported Isolated Single‐Atom Pd Catalyst for Highly Efficient Semihydrogenation of Acetylene journal June 2019
Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn–Air Batteries journal April 2021
In Situ Thermal Atomization To Convert Supported Nickel Nanoparticles into Surface-Bound Nickel Single-Atom Catalysts journal October 2018
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Figures / Tables (4)