Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Insights into the electronic origin of enhancing the catalytic activity of Co3O4 for oxygen evolution by single atom ruthenium

Journal Article · · Nano Today
 [1];  [2];  [3];  [3];  [4];  [5];  [5];  [3];  [4];  [6];  [2];  [4];  [7]
  1. Dalian Univ. of Technology (China). Liaoning Key Lab for Energy Materials and Chemical Engineering, School of Chemical Engineering, State Key Lab of Fine Chemicals, School of Chemical Engineering; Univ. of Western Ontario, London, ON (Canada). Dept. of Mechanical and Materials Engineering
  2. Tsinghua Univ., Beijing (China). Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Dept. of Chemistry
  3. Dalian Univ. of Technology (China). Liaoning Key Lab for Energy Materials and Chemical Engineering, School of Chemical Engineering, State Key Lab of Fine Chemicals, School of Chemical Engineering
  4. Univ. of Western Ontario, London, ON (Canada). Dept. of Mechanical and Materials Engineering
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  6. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics. Beijing National Lab. for Condensed Matter Physics (BNLCP-CAS)
  7. Dalian Univ. of Technology (China). Liaoning Key Lab for Energy Materials and Chemical Engineering, School of Chemical Engineering, State Key Lab of Fine Chemicals, School of Chemical Engineering; Chinese Academy of Sciences, Beijing (China). Beijing Univ. of Science and Technology, College of Chemical Engineering

The surface electronic structure of transition-metal oxide catalysts plays a decisive role in binding the intermediates of the oxygen evolution reaction (OER) to the oxide surface, in turn influencing the catalytic activity of these materials. However, the approaches to modulating the electronic structure of surface metal ions are rare and far behind the demands. Here, we report a surface single atom decoration for adjusting the surface electronic structure of Co3O4, leading to enhanced electrocatalytic activity for OER, in which the isolated Ru single atoms were uniformly deposited on the surface of Co3O4 by an atomic layer deposition technology. As the OER catalyst, the as-made catalysts have exhibited a significantly enhanced catalytic activity (with increasing to 95.5 times) and a dramatically decreased overpotential. The density functional theory calculations reveal that the single-atom Ru acts as a promotor to adjust the 3d electronic structure of adjacent Co atoms and to tune the binding energy between intermediates and activity sites, finally leading to enhanced catalytic activity.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1782093
Journal Information:
Nano Today, Journal Name: Nano Today Vol. 34; ISSN 1748-0132
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (43)

A Strongly Coupled Graphene and FeNi Double Hydroxide Hybrid as an Excellent Electrocatalyst for the Oxygen Evolution Reaction journal June 2014
Ultrathin Spinel-Structured Nanosheets Rich in Oxygen Deficiencies for Enhanced Electrocatalytic Water Oxidation journal May 2015
High-Performance Electrolytic Oxygen Evolution in Neutral Media Catalyzed by a Cobalt Phosphate Nanoarray journal December 2016
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces journal March 2011
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Single-atom ruthenium based catalyst for enhanced hydrogen evolution journal July 2019
Charge-Redistribution-Enhanced Nanocrystalline Ru@IrOx Electrocatalysts for Oxygen Evolution in Acidic Media journal February 2019
Co ion-intercalation amorphous and ultrathin microstructure for high-rate oxygen evolution journal January 2018
Electrolysis of water on oxide surfaces journal September 2007
Thermodynamic theory of multi-electron transfer reactions: Implications for electrocatalysis journal September 2011
Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications journal July 2018
DFT+U Study of the Surface Structure and Stability of Co 3 O 4 (110): Dependence on U journal April 2015
Water Oxidation on Pure and Doped Hematite (0001) Surfaces: Prediction of Co and Ni as Effective Dopants for Electrocatalysis journal August 2012
Theoretical Investigation of the Activity of Cobalt Oxides for the Electrochemical Oxidation of Water journal August 2013
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction journal October 2013
Metal–Organic Framework Derived Hybrid Co 3 O 4 -Carbon Porous Nanowire Arrays as Reversible Oxygen Evolution Electrodes journal September 2014
Electronic and Morphological Dual Modulation of Cobalt Carbonate Hydroxides by Mn Doping toward Highly Efficient and Stable Bifunctional Electrocatalysts for Overall Water Splitting journal June 2017
Single-Atom Au/NiFe Layered Double Hydroxide Electrocatalyst: Probing the Origin of Activity for Oxygen Evolution Reaction journal February 2018
Opportunities and challenges for a sustainable energy future journal August 2012
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
Platinum single-atom and cluster catalysis of the hydrogen evolution reaction journal November 2016
Exfoliation of layered double hydroxides for enhanced oxygen evolution catalysis journal July 2014
Electrodeposition of hierarchically structured three-dimensional nickel–iron electrodes for efficient oxygen evolution at high current densities journal March 2015
Reversible amorphization and the catalytically active state of crystalline Co3O4 during oxygen evolution journal October 2015
Atomic cobalt on nitrogen-doped graphene for hydrogen generation journal October 2015
A metal–organic framework-derived bifunctional oxygen electrocatalyst journal January 2016
Ultrathin metal–organic framework nanosheets for electrocatalytic oxygen evolution journal November 2016
Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution journal May 2018
Accelerating water dissociation kinetics by isolating cobalt atoms into ruthenium lattice journal November 2018
Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides journal April 2019
Heterogeneous single-atom catalysis journal May 2018
Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis journal March 2019
Triggering the electrocatalytic hydrogen evolution activity of the inert two-dimensional MoS 2 surface via single-atom metal doping journal January 2015
Density functional theory in surface chemistry and catalysis journal January 2011
First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method journal January 1997
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study journal January 1998
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Generalized Gradient Approximation Made Simple journal October 1996
In Situ Formation of an Oxygen-Evolving Catalyst in Neutral Water Containing Phosphate and Co2+ journal August 2008
A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles journal October 2011
Homogeneously dispersed multimetal oxygen-evolving catalysts journal March 2016
The Electrocatalysis of Oxygen Evolution on Perovskites journal January 1984