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Title: Nanocluster and single-atom catalysts for thermocatalytic conversion of CO and CO2

Abstract

In this Minireview, we discuss recent advances in understanding nanocluster and single-atom catalysts for CO and CO2 emissions control applications. Through analyzing thermocatalytic CO oxidation and CO2 reduction, two fundamentally and industrially important reactions, we compare representative nanocluster and single-atom catalytic systems from perspectives of intrinsic chemistry and reaction engineering. Generally, nanoclusters and single atoms display different catalytic performances (i.e., activity, selectivity, and stability) for these reactions depending on the synthesis methods, support materials, and reaction conditions. Key observations of activity and selectivity tradeoffs between nanoclusters and single-atom catalysts are highlighted. Here, the dynamic structural responses of these catalytic species under CO oxidation or CO2 reduction reaction conditions are also discussed. Synthetic control and detailed experimental and computational characterization of single-atom and nanocluster catalysts for CO and CO2 conversion have led to exciting progress over the past decade. Still, more efforts are needed to understand and develop catalysts that meet the environmental, energy, and technical requirements to power a sustainable global economy.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]
  1. University of Michigan, Ann Arbor, MI (United States)
  2. Tianjin University of Technology (China)
  3. General Motors Global Research and Development, Warren, MI (United States); Clemson University, SC (United States)
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Fusion Energy Sciences (FES)
OSTI Identifier:
1658251
Alternate Identifier(s):
OSTI ID: 1647267
Grant/Contract Number:  
SC0020232
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Science and Technology
Additional Journal Information:
Journal Volume: 10; Journal Issue: 17; Journal ID: ISSN 2044-4753
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 03 NATURAL GAS; Heterogeneous catalysis

Citation Formats

Doherty, Francis, Wang, Hui, Yang, Ming, and Goldsmith, Bryan R. Nanocluster and single-atom catalysts for thermocatalytic conversion of CO and CO2. United States: N. p., 2020. Web. doi:10.1039/d0cy01316a.
Doherty, Francis, Wang, Hui, Yang, Ming, & Goldsmith, Bryan R. Nanocluster and single-atom catalysts for thermocatalytic conversion of CO and CO2. United States. https://doi.org/10.1039/d0cy01316a
Doherty, Francis, Wang, Hui, Yang, Ming, and Goldsmith, Bryan R. Wed . "Nanocluster and single-atom catalysts for thermocatalytic conversion of CO and CO2". United States. https://doi.org/10.1039/d0cy01316a. https://www.osti.gov/servlets/purl/1658251.
@article{osti_1658251,
title = {Nanocluster and single-atom catalysts for thermocatalytic conversion of CO and CO2},
author = {Doherty, Francis and Wang, Hui and Yang, Ming and Goldsmith, Bryan R.},
abstractNote = {In this Minireview, we discuss recent advances in understanding nanocluster and single-atom catalysts for CO and CO2 emissions control applications. Through analyzing thermocatalytic CO oxidation and CO2 reduction, two fundamentally and industrially important reactions, we compare representative nanocluster and single-atom catalytic systems from perspectives of intrinsic chemistry and reaction engineering. Generally, nanoclusters and single atoms display different catalytic performances (i.e., activity, selectivity, and stability) for these reactions depending on the synthesis methods, support materials, and reaction conditions. Key observations of activity and selectivity tradeoffs between nanoclusters and single-atom catalysts are highlighted. Here, the dynamic structural responses of these catalytic species under CO oxidation or CO2 reduction reaction conditions are also discussed. Synthetic control and detailed experimental and computational characterization of single-atom and nanocluster catalysts for CO and CO2 conversion have led to exciting progress over the past decade. Still, more efforts are needed to understand and develop catalysts that meet the environmental, energy, and technical requirements to power a sustainable global economy.},
doi = {10.1039/d0cy01316a},
journal = {Catalysis Science and Technology},
number = 17,
volume = 10,
place = {United States},
year = {Wed Aug 05 00:00:00 EDT 2020},
month = {Wed Aug 05 00:00:00 EDT 2020}
}

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  • Kattel, Shyam; Liu, Ping; Chen, Jingguang G.
  • Journal of the American Chemical Society, Vol. 139, Issue 29
  • DOI: 10.1021/jacs.7b05362

Electrochemical Reduction of CO 2 on Metal-Nitrogen-Doped Carbon Catalysts
journal, June 2019


Theoretical Insights into Heterogeneous (Photo)electrochemical CO 2 Reduction
journal, October 2018


Surface strategies for catalytic CO 2 reduction: from two-dimensional materials to nanoclusters to single atoms
journal, January 2019

  • Wang, Liming; Chen, Wenlong; Zhang, Doudou
  • Chemical Society Reviews, Vol. 48, Issue 21
  • DOI: 10.1039/C9CS00163H

Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2
journal, July 2014


Mechanisms of Hydrogen-Assisted CO 2 Reduction on Nickel
journal, March 2017

  • Lin, Wei; Stocker, Kelsey M.; Schatz, George C.
  • Journal of the American Chemical Society, Vol. 139, Issue 13
  • DOI: 10.1021/jacs.7b01538

CO 2 Reduction on Supported Ru/Al 2 O 3 Catalysts: Cluster Size Dependence of Product Selectivity
journal, October 2013

  • Kwak, Ja Hun; Kovarik, Libor; Szanyi, János
  • ACS Catalysis, Vol. 3, Issue 11
  • DOI: 10.1021/cs400381f

Catalytic CO2 valorization into CH4 on Ni-based ceria-zirconia. Reaction mechanism by operando IR spectroscopy
journal, October 2013


Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal-Support Interaction
journal, August 2017

  • Li, Siwei; Xu, Yao; Chen, Yifu
  • Angewandte Chemie International Edition, Vol. 56, Issue 36
  • DOI: 10.1002/anie.201705002

Single Atom and Nanoclustered Pt Catalysts for Selective CO 2 Reduction
journal, October 2018

  • Wang, Yuan; Arandiyan, Hamidreza; Scott, Jason
  • ACS Applied Energy Materials, Vol. 1, Issue 12
  • DOI: 10.1021/acsaem.8b00817

Single-atom catalysts for CO 2 electroreduction with significant activity and selectivity improvements
journal, January 2017

  • Back, Seoin; Lim, Juhyung; Kim, Na-Young
  • Chemical Science, Vol. 8, Issue 2
  • DOI: 10.1039/C6SC03911A

Heterogeneous Catalysis on Atomically Dispersed Supported Metals: CO 2 Reduction on Multifunctional Pd Catalysts
journal, August 2013

  • Kwak, Ja Hun; Kovarik, Libor; Szanyi, János
  • ACS Catalysis, Vol. 3, Issue 9
  • DOI: 10.1021/cs4001392

Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts
journal, September 2016

  • Matsubu, John C.; Zhang, Shuyi; DeRita, Leo
  • Nature Chemistry, Vol. 9, Issue 2
  • DOI: 10.1038/nchem.2607

Structural evolution of atomically dispersed Pt catalysts dictates reactivity
journal, April 2019


Fluxionality of Catalytic Clusters: When It Matters and How to Address It
journal, February 2017


A genetic algorithm for first principles global structure optimization of supported nano structures
journal, July 2014

  • Vilhelmsen, Lasse B.; Hammer, Bjørk
  • The Journal of Chemical Physics, Vol. 141, Issue 4
  • DOI: 10.1063/1.4886337

Genetic algorithms for computational materials discovery accelerated by machine learning
journal, April 2019

  • Jennings, Paul C.; Lysgaard, Steen; Hummelshøj, Jens Strabo
  • npj Computational Materials, Vol. 5, Issue 1
  • DOI: 10.1038/s41524-019-0181-4

Revised Basin-Hopping Monte Carlo Algorithm for Structure Optimization of Clusters and Nanoparticles
journal, August 2013

  • Rondina, Gustavo G.; Da Silva, Juarez L. F.
  • Journal of Chemical Information and Modeling, Vol. 53, Issue 9
  • DOI: 10.1021/ci400224z

Automatic Prediction of Surface Phase Diagrams Using Ab Initio Grand Canonical Monte Carlo
journal, January 2019

  • Wexler, Robert B.; Qiu, Tian; Rappe, Andrew M.
  • The Journal of Physical Chemistry C, Vol. 123, Issue 4
  • DOI: 10.1021/acs.jpcc.8b11093

Reagent-Triggered Isomerization of Fluxional Cluster Catalyst via Dynamic Coupling
journal, March 2020

  • Guo, Han; Sautet, Philippe; Alexandrova, Anastassia N.
  • The Journal of Physical Chemistry Letters, Vol. 11, Issue 8
  • DOI: 10.1021/acs.jpclett.0c00548

Dynamics of Subnanometer Pt Clusters Can Break the Scaling Relationships in Catalysis
journal, January 2019

  • Zandkarimi, Borna; Alexandrova, Anastassia N.
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 3
  • DOI: 10.1021/acs.jpclett.8b03680

CO 2 Hydrogenation to Formate and Formic Acid by Bimetallic Palladium–Copper Hydride Clusters
journal, April 2020

  • Liu, Gaoxiang; Poths, Patricia; Zhang, Xinxing
  • Journal of the American Chemical Society, Vol. 142, Issue 17
  • DOI: 10.1021/jacs.0c01855

Ultrasmall Au clusters supported on pristine and defected CeO 2 : Structure and stability
journal, November 2019

  • Huang, Si-Da; Shang, Cheng; Liu, Zhi-Pan
  • The Journal of Chemical Physics, Vol. 151, Issue 17
  • DOI: 10.1063/1.5126187

Ensemble-Average Representation of Pt Clusters in Conditions of Catalysis Accessed through GPU Accelerated Deep Neural Network Fitting Global Optimization
journal, November 2016

  • Zhai, Huanchen; Alexandrova, Anastassia N.
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 12
  • DOI: 10.1021/acs.jctc.6b00994

Machine learning for heterogeneous catalyst design and discovery
journal, May 2018

  • Goldsmith, Bryan R.; Esterhuizen, Jacques; Liu, Jin-Xun
  • AIChE Journal, Vol. 64, Issue 7
  • DOI: 10.1002/aic.16198