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

Synthesis of 2H/fcc-Heterophase AuCu Nanostructures for Highly Efficient Electrochemical CO2 Reduction at Industrial Current Densities

Journal Article · · Advanced Materials
 [1];  [1];  [1];  [2];  [3];  [4];  [1];  [1];  [1];  [1];  [1];  [5];  [1];  [1];  [6];  [1];  [6];  [1];  [1];  [1] more »;  [1];  [1];  [7];  [6];  [8];  [3];  [3];  [9];  [8];  [2];  [9] « less
  1. City Univ. of Hong Kong, Kowloon (Hong Kong)
  2. Hong Kong University of Science and Technology (HKUST) (Hong Kong)
  3. Southeast Univ., Nanjing (China)
  4. City Univ. of Hong Kong, Kowloon (Hong Kong); Chinese Academy of Sciences (CAS), Shenzhen (China)
  5. City Univ. of Hong Kong, Kowloon (Hong Kong); Chinese Academy of Sciences (CAS), Hefei (China)
  6. The Chinese University of Hong Kong, Ma Liu Shui, Shatin (Hong Kong)
  7. Nanyang Technological Univ. (Singapore)
  8. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  9. City Univ. of Hong Kong, Kowloon (Hong Kong); City Univ. of Hong Kong, Shenzhen (Hong Kong)
Structural engineering of nanomaterials offers a promising way for developing high-performance catalysts toward catalysis. However, the delicate modulation of thermodynamically unfavorable nanostructures with unconventional phases still remains a challenge. Here, in this study, the synthesis of hierarchical AuCu nanostructures is reported with hexagonal close-packed (2H-type)/face-centered cubic (fcc) heterophase, high-index facets, planar defects (e.g., stacking faults, twin boundaries, and grain boundaries), and tunable Cu content. The obtained 2H/fcc Au99Cu1 hierarchical nanosheets exhibit excellent performance for the electrocatalytic CO2 reduction to produce CO, outperforming the 2H/fcc Au91Cu9 and fcc Au99Cu1. The experimental results, especially those obtained by in-situ differential electrochemical mass spectroscopy and attenuated total reflection Fourier-transform infrared spectroscopy, suggest that the enhanced catalytic performance of 2H/fcc Au99Cu1 arises from the unconventional 2H/fcc heterophase, high-index facets, planar defects, and appropriate alloying of Cu. Impressively, the 2H/fcc Au99Cu1 shows CO Faradaic efficiencies of 96.6% and 92.6% at industrial current densities of 300 and 500 mA cm-2, respectively, as well as good durability, placing it among the best CO2 reduction electrocatalysts for CO production. The atomically structural regulation based on phase engineering of nanomaterials (PEN) provides an avenue for the rational design and preparation of high-performance electrocatalysts for various catalytic applications.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
Hong Kong Research Grants Council (RCG); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2432576
Report Number(s):
BNL--225955-2024-JAAM
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 51 Vol. 35; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (49)

Amorphous/Crystalline Hetero-Phase Pd Nanosheets: One-Pot Synthesis and Highly Selective Hydrogenation Reaction journal August 2018
Ligand‐Exchange‐Induced Amorphization of Pd Nanomaterials for Highly Efficient Electrocatalytic Hydrogen Evolution Reaction journal February 2020
Synthesis of Palladium‐Based Crystalline@Amorphous Core–Shell Nanoplates for Highly Efficient Ethanol Oxidation journal April 2020
Structure Sensitivity in the Electrocatalytic Reduction of CO 2 with Gold Catalysts journal February 2019
Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia journal March 2020
Engineering Bismuth–Tin Interface in Bimetallic Aerogel with a 3D Porous Structure for Highly Selective Electrocatalytic CO 2 Reduction to HCOOH journal April 2021
Atomically Precise Gold Nanoclusters as Model Catalysts for Identifying Active Sites for Electroreduction of CO 2 journal May 2021
Self‐Supported Nanoporous Au 3 Cu Electrode with Enriched Gold on Surface for Efficient Electrochemical Reduction of CO 2 journal January 2020
Gold Nanoparticles on Polymer-Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO 2 journal October 2017
Surface Molecular Functionalization of Unusual Phase Metal Nanomaterials for Highly Efficient Electrochemical Carbon Dioxide Reduction under Industry‐Relevant Current Density journal January 2022
Noble-Metal Nanocrystals with Controlled Shapes for Catalytic and Electrocatalytic Applications journal July 2020
Bimetallic Nanocrystals: Syntheses, Properties, and Applications journal July 2016
Two-Dimensional Metal Nanomaterials: Synthesis, Properties, and Applications journal June 2018
Surface and Interface Control in Nanoparticle Catalysis journal October 2019
Selective Electrocatalytic Reduction of CO 2 into CO at Small, Thiol-Capped Au/Cu Nanoparticles journal August 2018
Constructing a Graphene-Encapsulated Amorphous/Crystalline Heterophase NiFe Alloy by Microwave Thermal Shock for Boosting the Oxygen Evolution Reaction journal September 2021
Tuned Chemical Bonding Ability of Au at Grain Boundaries for Enhanced Electrochemical CO 2 Reduction journal June 2016
Probing the Catalytically Active Region in a Nanoporous Gold Gas Diffusion Electrode for Highly Selective Carbon Dioxide Reduction journal January 2022
Insights into the Low Overpotential Electroreduction of CO 2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer journal November 2017
Grain-Boundary-Dependent CO 2 Electroreduction Activity journal April 2015
Phase-Selective Epitaxial Growth of Heterophase Nanostructures on Unconventional 2H-Pd Nanoparticles journal October 2020
Preparation of Au@Pd Core–Shell Nanorods with fcc-2H-fcc Heterophase for Highly Efficient Electrocatalytic Alcohol Oxidation journal December 2021
Ultrathin Pd–Au Shells with Controllable Alloying Degree on Pd Nanocubes toward Carbon Dioxide Reduction journal March 2019
Synthesis of hexagonal close-packed gold nanostructures journal April 2011
Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles journal September 2014
Stabilization of 4H hexagonal phase in gold nanoribbons journal July 2015
Bismuthene for highly efficient carbon dioxide electroreduction reaction journal February 2020
Heterophase fcc-2H-fcc gold nanorods journal July 2020
Gold-in-copper at low *CO coverage enables efficient electromethanation of CO2 journal June 2021
Efficiency and selectivity of CO2 reduction to CO on gold gas diffusion electrodes in acidic media journal August 2021
Efficient CO2 electroreduction on facet-selective copper films with high conversion rate journal September 2021
Crystal phase-based epitaxial growth of hybrid noble metal nanostructures on 4H/fcc Au nanowires journal March 2018
Copper-catalysed exclusive CO2 to pure formic acid conversion via single-atom alloying journal September 2021
Phase engineering of nanomaterials journal April 2020
Crystal-phase and surface-structure engineering of ruthenium nanocrystals journal March 2020
PdMo bimetallene for oxygen reduction catalysis journal September 2019
Mastering the surface strain of platinum catalysts for efficient electrocatalysis journal October 2021
Metastable hexagonal close-packed palladium hydride in liquid cell TEM journal March 2022
Lithiation-induced amorphization of Pd3P2S8 for highly efficient hydrogen evolution journal May 2018
Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis journal December 2019
Highly active and stable stepped Cu surface for enhanced electrochemical CO2 reduction to C2H4 journal September 2020
P vacancies-enriched 3D hierarchical reduced cobalt phosphide as a precursor template for defect engineering for efficient water oxidation journal January 2018
An alkaline polymer electrolyte CO 2 electrolyzer operated with pure water journal January 2019
Electrochemical CO 2 to CO reduction at high current densities using a nanoporous gold catalyst journal November 2020
Evoking ordered vacancies in metallic nanostructures toward a vacated Barlow packing for high-performance hydrogen evolution journal March 2021
Selective increase in CO 2 electroreduction activity at grain-boundary surface terminations journal November 2017
Three-orders-of-magnitude variation of carrier lifetimes with crystal phase of gold nanoclusters journal April 2019
Shape regulation of high-index facet nanoparticles by dealloying journal September 2019
Sulfur-anchoring synthesis of platinum intermetallic nanoparticle catalysts for fuel cells journal October 2021

Similar Records

Phase-Selective Epitaxial Growth of Heterophase Nanostructures on Unconventional 2H-Pd Nanoparticles
Journal Article · Tue Oct 20 20:00:00 EDT 2020 · Journal of the American Chemical Society · OSTI ID:1798516

Heterophase fcc-2H-fcc gold nanorods
Journal Article · Thu Jul 02 20:00:00 EDT 2020 · Nature Communications · OSTI ID:1659725

Crystal Structural Effect of AuCu Alloy Nanoparticles on Catalytic CO Oxidation
Journal Article · Tue Jun 06 20:00:00 EDT 2017 · Journal of the American Chemical Society · OSTI ID:1399233

Related Subjects