Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst

Journal Article · · Advanced Functional Materials
 [1]; ORCiD logo [2];  [3];  [2];  [4];  [5]; ORCiD logo [6];  [7];  [8]; ORCiD logo [9]
  1. Columbia Univ., New York, NY (United States); Univ. of Science and Technology of China, Hefei (China)
  2. Columbia Univ., New York, NY (United States)
  3. Nanyang Technological Univ. (Singapore)
  4. Department of Chemical EngineeringColumbia University New York NY 10027 USA
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  7. Florida A & M University, Tallahassee, FL (United States)
  8. Univ. of Science and Technology of China, Hefei (China)
  9. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
+ Show Author Affiliations

The electrochemical conversion of carbon dioxide (CO2) into value-added chemicals is regarded as one of the promising routes to mitigate CO2 emission. A nitrogen-doped carbon-supported palladium (Pd) single-atom catalyst that can catalyze CO2 into CO with far higher mass activity than its Pd nanoparticle counterpart, for example, 373.0 and 28.5 mA mg–1Pd, respectively, at –0.8 V versus reversible hydrogen electrode, is reported herein. A combination of in situ X-ray characterization and density functional theory (DFT) calculation reveals that the Pd–N4 site is the most likely active center for CO production without the formation of palladium hydride (PdH), which is essential for typical Pd nanoparticle catalysts. Furthermore, the well-dispersed Pd–N4 single-atom site facilitates the stabilization of the adsorbed CO2 intermediate, thereby enhancing electrocatalytic CO2 reduction capability at low overpotentials. This work provides important insights into the structure-activity relationship for single-atom based electrocatalysts.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II) and Center for Functional Nanomaterials (CFN); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Key Research and Development Program of China; China Scholarship Council (CSC)
Grant/Contract Number:
SC0012704; FG02-13ER16381; ACI-1548562; AC02-05CH11231
OSTI ID:
1604621
Alternate ID(s):
OSTI ID: 1602349
Report Number(s):
BNL-213730-2020-JAAM
Journal Information:
Advanced Functional Materials, Vol. 30, Issue 17; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 157 works
Citation information provided by
Web of Science

References (48)

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides journal April 2019
Adult-born hippocampal neurons bidirectionally modulate entorhinal inputs into the dentate gyrus journal May 2019
Unveiling Active Sites of CO 2 Reduction on Nitrogen-Coordinated and Atomically Dispersed Iron and Cobalt Catalysts journal March 2018
Oriented electron transmission in polyoxometalate-metalloporphyrin organic framework for highly selective electroreduction of CO2 journal October 2018
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts journal August 2019
Projector augmented-wave method journal December 1994
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles journal September 2018
Theoretical Insights into Heterogeneous (Photo)electrochemical CO 2 Reduction journal October 2018
Isolated Diatomic Ni-Fe Metal-Nitrogen Sites for Synergistic Electroreduction of CO 2 journal April 2019
Promoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces journal February 2019
Special points for Brillouin-zone integrations journal June 1976
Understanding the Roadmap for Electrochemical Reduction of CO 2 to Multi-Carbon Oxygenates and Hydrocarbons on Copper-Based Catalysts journal April 2019
Ab initio molecular dynamics for open-shell transition metals journal November 1993
What Should We Make with CO2 and How Can We Make It? journal May 2018
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Active Sites Engineering toward Superior Carbon-Based Oxygen Reduction Catalysts via Confinement Pyrolysis journal April 2018
Net reduction of CO2 via its thermocatalytic and electrocatalytic transformation reactions in standard and hybrid processes journal April 2019
Inhomogeneous Electron Gas journal November 1964
Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices journal September 2019
Electrochemical reduction of CO 2 to synthesis gas with controlled CO/H 2 ratios journal January 2017
Electrochemical Conversion of CO 2 to Syngas with Controllable CO/H 2 Ratios over Co and Ni Single-Atom Catalysts journal January 2020
Single Atom Hot-Spots at Au–Pd Nanoalloys for Electrocatalytic H 2 O 2 Production journal December 2011
Active Sites on Heterogeneous Single-Iron-Atom Electrocatalysts in CO 2 Reduction Reaction journal June 2019
Understanding of Strain Effects in the Electrochemical Reduction of CO 2 : Using Pd Nanostructures as an Ideal Platform journal February 2017
Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis journal December 2017
Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO journal October 2013
Active and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires journal November 2014
Facet design promotes electroreduction of carbon dioxide to carbon monoxide on palladium nanocrystals journal February 2019
Bio-inspired hydrophobicity promotes CO2 reduction on a Cu surface journal August 2019
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction journal February 2018
General π-Electron-Assisted Strategy for Ir, Pt, Ru, Pd, Fe, Ni Single-Atom Electrocatalysts with Bifunctional Active Sites for Highly Efficient Water Splitting journal July 2019
Stability, Electronic and Magnetic Properties of In-Plane Defects in Graphene: A First-Principles Study journal March 2012
Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel journal January 2016
Density functional studies of functionalized graphitic materials with late transition metals for oxygen reduction reactions journal January 2011
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode journal November 2004
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal March 2019
Direct conversion of CO2 into liquid fuels with high selectivity over a bifunctional catalyst journal June 2017
Atomically dispersed Fe 3+ sites catalyze efficient CO 2 electroreduction to CO journal June 2019
Visible-light-driven methane formation from CO2 with a molecular iron catalyst journal July 2017
Tuning Metal Catalyst with Metal–C 3 N 4 Interaction for Efficient CO 2 Electroreduction journal October 2018
Ultrathin Pd–Au Shells with Controllable Alloying Degree on Pd Nanocubes toward Carbon Dioxide Reduction journal March 2019
Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction journal January 2018
In situ trapped high-density single metal atoms within graphene: Iron-containing hybrids as representatives for efficient oxygen reduction journal March 2018
Achieving Selective and Efficient Electrocatalytic Activity for CO 2 Reduction Using Immobilized Silver Nanoparticles journal October 2015
Covalent organic frameworks comprising cobalt porphyrins for catalytic CO 2 reduction in water journal August 2015
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels journal January 2014

Similar Records

Related Subjects

25 ENERGY STORAGE
CO2 electroreduction
density functional theory
palladium
single‐atom catalysis
X‐ray absorption spectroscopy