skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis

Journal Article · · Nature Catalysis
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5];  [6];  [7];  [8];  [3]; ORCiD logo [3];  [9]; ORCiD logo [9]; ORCiD logo [10];  [10]; ORCiD logo [3];  [8];  [8];  [3]; ORCiD logo [11]; ORCiD logo [12] more »; ORCiD logo [13]; ORCiD logo [14];  [15]; ORCiD logo [16] « less
  1. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering, and Dept. of Chemistry
  2. Univ. of California, Los Angeles, CA (United States). Dept. of Chemical and Biomolecular Engineering
  3. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry
  4. California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center; Soochow Univ., Suzhou, Jiangsu (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices, Joint International Research Lab. of Carbon-Based Functional Materials and Devices
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Univ. of California, Irvine, CA (United States). Dept. of Materials Science and Engineering
  7. Tsinghua Univ., Beijing (China). Dept. of Chemistry
  8. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
  9. Tsinghua Univ. Beijing (China). 9National Center for Electron; Microscopy in Beijing, School of Materials Science and Engineering
  10. Tianjin Univ. of Technology, Tianjin (China). Center for Electron Microscopy
  11. Soochow Univ., Suzhou, Jiangsu (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials & Devices, Joint International Research Lab. of Carbon-Based Functional Materials and Devices
  12. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Irvine, CA (United States). Irvine Materials Research Institute (IMRI)
  13. California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center
  14. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry, and Dept. of Chemical and Biomolecular Engineering; Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.
  15. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering; Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.
  16. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry; Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.

Platinum-based nanocatalysts play a crucial role in various electrocatalytic systems that are important for renewable, clean energy conversion, storage and utilization. However, the scarcity and high cost of Pt seriously limit the practical application of these catalysts. Decorating Pt catalysts with other transition metals offers an effective pathway to tailor their catalytic properties, but often at the sacrifice of the electrochemical active surface area (ECSA). Here we report a single-atom tailoring strategy to boost the activity of Pt nanocatalysts with minimal loss in surface active sites. By starting with PtNi alloy nanowires and using a partial electrochemical dealloying approach, we create single-nickel-atom-modified Pt nanowires with an optimum combination of specific activity and ECSA for the hydrogen evolution, methanol oxidation and ethanol oxidation reactions. The single-atom tailoring approach offers an effective strategy to optimize the activity of surface Pt atoms and enhance the mass activity for diverse reactions, opening a general pathway to the design of highly efficient and durable precious metal-based catalysts.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1559808
Journal Information:
Nature Catalysis, Vol. 2, Issue 6; ISSN 2520-1158
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 317 works
Citation information provided by
Web of Science

References (48)

Enhancing the Alkaline Hydrogen Evolution Reaction Activity through the Bifunctionality of Ni(OH) 2 /Metal Catalysts journal November 2012
Generalized Gradient Approximation Made Simple journal October 1996
White lines and d -electron occupancies for the 3 d and 4 d transition metals journal April 1993
Trends in activity for the water electrolyser reactions on 3d M(Ni,Co,Fe,Mn) hydr(oxy)oxide catalysts journal May 2012
A highly active PtNi/C electrocatalyst for methanol electro-oxidation in alkaline media journal October 2010
Unique Electrochemical Adsorption Properties of Pt-Skin Surfaces journal February 2012
Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces journal February 2014
Beyond Strain and Ligand Effects: Microstrain-Induced Enhancement of the Oxygen Reduction Reaction Kinetics on Various PtNi/C Nanostructures journal December 2016
Enhancing Hydrogen Evolution Activity in Water Splitting by Tailoring Li+-Ni(OH)2-Pt Interfaces journal December 2011
Highly active and durable methanol oxidation electrocatalyst based on the synergy of platinum–nickel hydroxide–graphene journal November 2015
Finding optimal surface sites on heterogeneous catalysts by counting nearest neighbors journal October 2015
Pt-rich shell coated Ni nanoparticles as catalysts for methanol electro-oxidation in alkaline media journal August 2009
High-performance transition metal-doped Pt3Ni octahedra for oxygen reduction reaction journal June 2015
Finite Bias Calculations to Model Interface Dipoles in Electrochemical Cells at the Atomic Scale journal June 2016
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Ultrathin platinum nanowires grown on single-layered nickel hydroxide with high hydrogen evolution activity journal March 2015
Platinum Monolayer on Nonnoble Metal−Noble Metal Core−Shell Nanoparticle Electrocatalysts for O2 Reduction journal December 2005
Surface distortion as a unifying concept and descriptor in oxygen reduction reaction electrocatalysis journal July 2018
Octahedral PtNi Nanoparticle Catalysts Exceptional Oxygen Reduction Activity by Tuning the Alloy Particle Surface Composition journal October 2012
One-pot synthesis of a RGO-supported ultrafine ternary PtAuRu catalyst with high electrocatalytic activity towards methanol oxidation in alkaline medium journal January 2013
Compositional segregation in shaped Pt alloy nanoparticles and their structural behaviour during electrocatalysis journal June 2013
Oxygen Evolution Reaction Electrocatalysis on Transition Metal Oxides and (Oxy)hydroxides: Activity Trends and Design Principles journal October 2015
Ultrafine jagged platinum nanowires enable ultrahigh mass activity for the oxygen reduction reaction journal November 2016
Facile Synthesis of Free-Standing Pd-Based Nanomembranes with Enhanced Catalytic Performance for Methanol/Ethanol Oxidation journal February 2012
Effect of Atomic Vacancies on the Structure and the Electrocatalytic Activity of Pt-rich/C Nanoparticles: A Combined Experimental and Density Functional Theory Study journal May 2017
Clean Method for the Synthesis of Reduced Graphene Oxide-Supported PtPd Alloys with High Electrocatalytic Activity for Ethanol Oxidation in Alkaline Medium journal February 2014
Single-atom catalysts for CO 2 electroreduction with significant activity and selectivity improvements journal January 2017
Ab initiomolecular dynamics for liquid metals journal January 1993
One-Pot Synthesis of Highly Anisotropic Five-Fold-Twinned PtCu Nanoframes Used as a Bifunctional Electrocatalyst for Oxygen Reduction and Methanol Oxidation journal August 2016
Trends in the Exchange Current for Hydrogen Evolution journal January 2005
Platinum-nickel alloy excavated nano-multipods with hexagonal close-packed structure and superior activity towards hydrogen evolution reaction journal April 2017
Precise tuning in platinum-nickel/nickel sulfide interface nanowires for synergistic hydrogen evolution catalysis journal February 2017
Surface-Engineered PtNi-O Nanostructure with Record-High Performance for Electrocatalytic Hydrogen Evolution Reaction journal June 2018
Synthesis and Characterization of 9 nm Pt–Ni Octahedra with a Record High Activity of 3.3 A/mg Pt for the Oxygen Reduction Reaction journal June 2013
Charge-Transfer Effects in Ni–Fe and Ni–Fe–Co Mixed-Metal Oxides for the Alkaline Oxygen Evolution Reaction journal December 2015
Significantly enhanced electrocatalytic activity for methanol electro-oxidation on Ag oxide-promoted PtAg/C catalysts in alkaline electrolyte journal June 2012
General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities journal January 2018
Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation journal January 2018
Atomic Structure of Pt 3 Ni Nanoframe Electrocatalysts by in Situ X-ray Absorption Spectroscopy journal December 2015
Single-Atom Catalysts: Emerging Multifunctional Materials in Heterogeneous Catalysis journal September 2017
Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facets journal July 2015
Why conclusions from platinum model surfaces do not necessarily lead to enhanced nanoparticle catalysts for the oxygen reduction reaction journal January 2017
Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts journal April 2010
Crystal Phase and Architecture Engineering of Lotus-Thalamus-Shaped Pt-Ni Anisotropic Superstructures for Highly Efficient Electrochemical Hydrogen Evolution journal June 2018
Unique Electrochemical Adsorption Properties of Pt-Skin Surfaces journal February 2012
Enhancing the Alkaline Hydrogen Evolution Reaction Activity through the Bifunctionality of Ni(OH) 2 /Metal Catalysts journal November 2012
Platinum Monolayer on Nonnoble Metal—Noble Metal Core—Shell Nanoparticle Electrocatalysts for O2 Reduction. journal February 2006
Trends in the Exchange Current for Hydrogen Evolution. journal June 2005

Cited By (9)

Tuning Surface Structure of Pd 3 Pb/Pt n Pb Nanocrystals for Boosting the Methanol Oxidation Reaction journal October 2019
Heterogeneous Single Atom Electrocatalysis, Where “Singles” Are “Married” journal January 2020
A Supported Nickel Catalyst Stabilized by a Surface Digging Effect for Efficient Methane Oxidation journal November 2019
Hollow Nanotube Ru/Cu 2+1 O Supported on Copper Foam as a Bifunctional Catalyst for Overall Water Splitting journal November 2019
Recover the activity of sintered supported catalysts by nitrogen-doped carbon atomization journal January 2020
A metal-catalyzed thermal polymerization strategy toward atomically dispersed catalysts journal January 2019
Platinum single-atom catalysts: a comparative review towards effective characterization journal January 2019
A sacrificial Zn strategy enables anchoring of metal single atoms on the exposed surface of holey 2D molybdenum carbide nanosheets for efficient electrocatalysis journal January 2020
A Supported Nickel Catalyst Stabilized by a Surface Digging Effect for Efficient Methane Oxidation journal November 2019