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Title: Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction

Journal Article · · Chemistry of Materials
DOI:https://doi.org/10.1021/cm5037502· OSTI ID:1185918
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Rice Univ., Houston, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Rice Univ., Houston, TX (United States); Beihang Univ., Beijing (China)

Here, we show that nanoribbons of boron- and nitrogen-substituted graphene can be used as efficient electrocatalysts for the oxygen reduction reaction (ORR). Optimally doped graphene nanoribbons made into three-dimensional porous constructs exhibit the highest onset and half-wave potentials among the reported metal-free catalysts for this reaction and show superior performance compared to commercial Pt/C catalyst. Moreover, this catalyst possesses high kinetic current density and four-electron transfer pathway with low hydrogen peroxide yield during the reaction. Finally, first-principles calculations suggest that such excellent electrocatalytic properties originate from the abundant edges of boron- and nitrogen-codoped graphene nanoribbons, which significantly reduce the energy barriers of the rate-determining steps of the ORR reaction.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725; DMR-0928297; W911NF-11-1-032; FA9550-09-1-0581; FA9550-12-1-0035; N000014-09-1-1066; OCI-0959097
OSTI ID:
1185918
Journal Information:
Chemistry of Materials, Vol. 27, Issue 4; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 200 works
Citation information provided by
Web of Science

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Cited By (37)

Rational Design of Fe 1− x S/Fe 3 O 4 /Nitrogen and Sulfur-Doped Porous Carbon with Enhanced Oxygen Reduction Reaction Catalytic Activity journal January 2018
Surface Electrochemical Stability and Strain-Tunable Lithium Storage of Highly Flexible 2D Transition Metal Carbides journal September 2018
Emerging new generation electrocatalysts for the oxygen reduction reaction journal January 2016
Application of Nanomaterials Prepared by Thermolysis of Metal Chelates book January 2018
Metal-Free N, P-Codoped Porous Carbon Fibers for Oxygen Reduction Reactions journal January 2019
An Fe–N co-doped tube-in-tube carbon nanostructure used as an efficient catalyst for the electrochemical oxygen reduction reaction journal September 2019
Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis journal September 2019
Web-Like Interconnected Carbon Networks from NaCl-Assisted Pyrolysis of ZIF-8 for Highly Efficient Oxygen Reduction Catalysis journal March 2018
Tuning the Electrochemical Reactivity of Boron- and Nitrogen-Substituted Graphene journal March 2016
Recent Progress of Carbon-Based Materials in Oxygen Reduction Reaction Catalysis journal January 2018
Co 3 O 4 Nanoparticles-Modified α-MnO 2 Nanorods Supported on Reduced Graphene Oxide as Cathode Catalyst for Oxygen Reduction Reaction in Alkaline Media journal October 2016
Graphene-wrapped nitrogen-doped hollow carbon spheres for high-activity oxygen electroreduction journal January 2018
Biomass-derived synthesis of nitrogen and phosphorus Co-doped mesoporous carbon spheres as catalysts for oxygen reduction reaction journal August 2016
Multifunctional nitrogen-doped graphene nanoribbon aerogels for superior lithium storage and cell culture journal January 2016
Al-coordination polymer-derived nanoporous nitrogen-doped carbon microfibers as metal-free catalysts for oxygen electroreduction and acetalization reactions journal January 2015
Sulfur-doping achieves efficient oxygen reduction in pyrolyzed zeolitic imidazolate frameworks journal January 2016
Oxygen reduction reaction mechanism on P, N co-doped graphene: a density functional theory study journal January 2019
Atomic Fe hetero-layered coordination between g-C 3 N 4 and graphene nanomeshes enhances the ORR electrocatalytic performance of zinc–air batteries journal January 2019
Transfer‐Free Synthesis of Lateral Graphene–Hexagonal Boron Nitride Heterostructures from Chemically Converted Epitaxial Graphene journal July 2019
One-pot Synthesis of Nitrogen and Phosphorus Co-doped Graphene and Its Use as High-performance Electrocatalyst for Oxygen Reduction Reaction journal September 2015
Electronic structure and ultrafast charge transfer dynamics of phosphorous doped graphene layers on a copper substrate: a combined spectroscopic study journal January 2015
Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells journal June 2017
Chemical Approaches to Carbon‐Based Metal‐Free Catalysts journal January 2019
Synergistic Effect of B and N Dopants in Catalytic Transfer Hydrogenation journal May 2018
Recent Progress in Oxygen Electrocatalysts for Zinc-Air Batteries journal November 2017
Efficient Synthesis of Nitrogen- and Sulfur-co-Doped Ketjenblack with a Single-Source Precursor for Enhancing Oxygen Reduction Reaction Activity journal February 2017
Confinement Catalysis with 2D Materials for Energy Conversion journal July 2019
Surface Engineering of Two-Dimensional Materials journal June 2018
Complementary behaviour of EDL and HER activity in functionalized graphene nanoplatelets journal January 2020
Preparation and Study of Multi-Heteroatom Carbon Nanotube as Excellent Electrocatalyst for Oxygen Reduction Reaction Using Polydopamine Derivative journal January 2018
Carbon dots with tunable concentrations of trapped anti-oxidant as an efficient metal-free catalyst for electrochemical water oxidation journal January 2016
A Mechanochemical‐Assisted Synthesis of Boron, Nitrogen Co‐Doped Porous Carbons as Metal‐Free Catalysts journal January 2020
Sustainable metal-free carbogels as oxygen reduction electrocatalysts journal January 2017
Bifunctional Oxygen Electrocatalysis through Chemical Bonding of Transition Metal Chalcogenides on Conductive Carbons journal March 2017
Highly dual-doped multilayer nanoporous graphene: efficient metal-free electrocatalysts for the hydrogen evolution reaction journal January 2015
Mechanistic Study of the Conversion of Superoxide to Oxygen and Hydrogen Peroxide in Carbon Nanoparticles journal June 2016
Hydrolytic Unzipping of Boron Nitride Nanotubes in Nitric Acid journal February 2017

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