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

Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper

Journal Article · · Nature Energy
 [1];  [1];  [2];  [3];  [3];  [3];  [3];  [4];  [3];  [3];  [5];  [6]
  1. Argonne National Lab. (ANL), Lemont, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)
  2. Valparaiso Univ., IN (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, IL (United States)
  6. Northern Illinois Univ., DeKalb, IL (United States)
+ Show Author Affiliations
Direct electrochemical conversion of CO2 to ethanol offers a promising strategy of lowering CO2 emission while storing energy from renewable electricity. However, current electrocatalysts offer only limited selectivity toward ethanol. Here we report a copper catalyst synthesized by a unique Cu-Li amalgm method over a commercial carbon support that achieved Faradaic efficiency (FE) higher than 91% at -0.7 V (RHE) and the active potential as low as -0.4 V (RHE) during direct electrocatalytic CO2-to-ethanol conversion. The catalyst also demonstrated stability over an extended period of operation. A strong correlation between the catalytic selectivity and the initial Cu atoms dispersion was found and Operando X-ray absorption spectroscopy identified a dynamic and reversible transformation from atomically dispersed copper atoms to Cun (n = 3 and 4) under the electrochemical reaction. Frist-principles calculations further elucidate the possible catalytic mechanism of CO2 reduction over Cun.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1671779
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 8 Vol. 5; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (37)

Amorphizing of Cu Nanoparticles toward Highly Efficient and Robust Electrocatalyst for CO 2 Reduction to Liquid Fuels with High Faradaic Efficiencies journal February 2018
Inside Cover: Ultra-Tuning of the Aperture Size in Stiffened ZIF-8_Cm Frameworks with Mixed-Linker Strategy for Enhanced CO 2 /CH 4 Separation (Angew. Chem. Int. Ed. 1/2019) journal December 2018
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Sulfur-Modulated Tin Sites Enable Highly Selective Electrochemical Reduction of CO2 to Formate journal December 2017
Cu-based nanocatalysts for electrochemical reduction of CO2 journal August 2018
Rhenium(I) Phosphazane Complexes for Electrocatalytic CO 2 Reduction journal March 2019
Electrochemical Reduction of CO 2 Using Copper Single-Crystal Surfaces: Effects of CO* Coverage on the Selective Formation of Ethylene journal February 2017
Achieving Highly Efficient, Selective, and Stable CO 2 Reduction on Nitrogen-Doped Carbon Nanotubes journal April 2015
Selective Electrochemical Reduction of Carbon Dioxide to Ethylene and Ethanol on Copper(I) Oxide Catalysts journal March 2015
Use of X-ray Absorption Spectroscopy To Speciate Manganese in Airborne Particulate Matter from Five Counties Across the United States journal March 2012
Tin Oxide Dependence of the CO 2 Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts journal January 2012
Synthesis of Supported Platinum Nanoparticles from Li−Pt Solid Solution journal February 2010
Electrochemical Reduction of CO 2 at Functionalized Au Electrodes journal February 2017
Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts journal January 2012
A handful of carbon journal May 2007
Understanding trends in electrochemical carbon dioxide reduction rates journal May 2017
Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles journal September 2014
FeOx-supported platinum single-atom and pseudo-single-atom catalysts for chemoselective hydrogenation of functionalized nitroarenes journal December 2014
Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction journal January 2018
Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons journal July 2018
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction journal February 2018
Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction journal January 2018
Recycling of carbon dioxide to methanol and derived products – closing the loop journal January 2014
Amino acid modified copper electrodes for the enhanced selective electroreduction of carbon dioxide towards hydrocarbons journal January 2016
Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction journal January 2018
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels journal January 2010
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces journal January 2012
Copper nanoparticle ensembles for selective electroreduction of CO 2 to C 2 –C 3 products journal September 2017
CO 2 reduction to acetate in mixtures of ultrasmall (Cu) n ,(Ag) m bimetallic nanoparticles journal December 2017
Ab initiomolecular dynamics for liquid metals journal January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
First principles studies on the growth of small Cu clusters and the dissociative chemisorption of H 2 journal April 2006
Generalized Gradient Approximation Made Simple journal October 1996
Carbon-Negative Biofuels from Low-Input High-Diversity Grassland Biomass journal December 2006
Covalent organic frameworks comprising cobalt porphyrins for catalytic CO 2 reduction in water journal August 2015
Identification of single-site gold catalysis in acetylene hydrochlorination journal March 2017
High–performance Activated Carbons Prepared by KOH Activation of Gulfweed for Supercapacitors journal February 2018

Similar Records

Atomically Dispersed CuNx Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation
Journal Article · Tue Aug 23 20:00:00 EDT 2022 · ACS Applied Energy Materials · OSTI ID:1903197

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2
catalysis
conversion
electrochemical
ethanol