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Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity

Journal Article · · Nature Communications
 [1];  [2];  [2];  [3];  [4];  [5];  [2];  [6];  [4];  [4];  [7];  [7];  [2];  [2]
  1. Univ. of Central Florida, Orlando, FL (United States); Nanjing Univ. (China)
  2. Univ. of Central Florida, Orlando, FL (United States)
  3. Villanova Univ., PA (United States)
  4. Nanjing Univ. (China)
  5. BASF Corporation, Iselin, NJ (United States)
  6. Brewton-Parker College, Mount Vernon, GA (United States)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO2 supported Pt single atom catalysts with precisely controlled coordination environments are successfully fabricated. The joint experimental and theoretical analysis reveals that the Pt single atoms on Pt1/CeO2 prepared at 550 °C (Pt/CeO2-550) are mainly located at the edge sites of CeO2 with a Pt–O coordination number of ca. 5, while those prepared at 800 °C (Pt/CeO2-800) are predominantly located at distorted Ce substitution sites on CeO2 terrace with a Pt–O coordination number of ca. 4. Pt/CeO2-550 and Pt/CeO2-800 with different Pt1-CeO2 coordination environments exhibit a reversal of activity trend in CO oxidation and NH3 oxidation due to their different privileges in reactants activation and H2O desorption, suggesting that the catalytic performance of Pt single atom catalysts in different target reactions can be maximized by optimizing their local coordination structures.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1922809
Report Number(s):
BNL-223945-2023-JAAM
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (66)

CO Oxidation as a Prototypical Reaction for Heterogeneous Processes journal September 2011
Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum journal June 2014
Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts journal August 2016
Dual Metal Active Sites in an Ir 1 /FeO x Single‐Atom Catalyst: A Redox Mechanism for the Water‐Gas Shift Reaction journal May 2020
Controlling the Oxidation State of Pt Single Atoms for Maximizing Catalytic Activity journal September 2020
Activating Lattice Oxygen at the Twisted Surface in a Mesoporous CeO 2 Single Crystal for Efficient and Durable Catalytic CO Oxidation journal January 2021
Rational Fabrication of Low‐Coordinate Single‐Atom Ni Electrocatalysts by MOFs for Highly Selective CO 2 Reduction journal February 2021
Tailoring the Local Environment of Platinum in Single‐Atom Pt 1 /CeO 2 Catalysts for Robust Low‐Temperature CO Oxidation journal September 2021
Highly Stable and Reactive Platinum Single Atoms on Oxygen Plasma‐Functionalized CeO 2 Surfaces: Nanostructuring and Peroxo Effects journal March 2022
Tuning Single‐atom Pt 1 −CeO 2 Catalyst for Efficient CO and C 3 H 6 Oxidation: Size Effect of Ceria on Pt Structural Evolution journal October 2020
Kinetics of NH3 oxidation on Pt, Rh, and Pd*1 journal November 1975
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
The smart surface modification of Fe2O3 by WO for significantly promoting the selective catalytic reduction of NO with NH3 journal August 2018
Stabilizing platinum atoms on CeO2 oxygen vacancies by metal-support interaction induced interface distortion: Mechanism and application journal December 2020
Local structure in CeO2 and CeO2–ZrO2 nanoparticles probed by Eu luminescence journal September 2015
Insights into formation of Pt species in Pt/CeO2 catalysts: Effect of treatment conditions and metal-support interaction journal September 2021
Enhanced photocatalytic activity of Pt-doped TiO2 for NOx oxidation both under UV and visible light irradiation: A synergistic effect of lattice Pt4+ and surface PtO journal August 2015
Transformation of CeO2 into a mixed phase CeO2/Ce2O3 nanohybrid by liquid phase pulsed laser ablation for enhanced photocatalytic activity through Z-scheme pattern journal December 2016
Effect of the CeO2 synthesis method on the behaviour of Pt/CeO2 catalysis for the water-gas shift reaction journal August 2019
Gas phase sulfation of ceria-zirconia solid solutions for generating highly efficient and SO2 resistant NH3-SCR catalysts for NO removal journal April 2020
First principles phonon calculations in materials science journal November 2015
Single-Atom Catalysts across the Periodic Table journal October 2020
Single-Atom Catalysts Based on the Metal–Oxide Interaction journal October 2020
Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles journal April 2018
Transformation of Highly Stable Pt Single Sites on Defect Engineered Ceria into Robust Pt Clusters for Vehicle Emission Control journal September 2021
Vacancy Generation and Oxygen Uptake in Cu-Doped Pr-CeO2 Materials using Neutron and in Situ X-ray Diffraction journal December 2016
Catalytic CO Oxidation on MgAl 2 O 4 -Supported Iridium Single Atoms: Ligand Configuration and Site Geometry journal May 2021
How Pt Interacts with CeO 2 under the Reducing and Oxidizing Environments at Elevated Temperature: The Origin of Improved Thermal Stability of Pt/CeO 2 Compared to CeO 2 journal November 2016
Theoretical Investigations of Pt 1 @CeO 2 Single-Atom Catalyst for CO Oxidation journal May 2017
Unravelling the Different Reaction Pathways for Low Temperature CO Oxidation on Pt/CeO 2 and Pt/Al 2 O 3 by Spatially Resolved Structure–Activity Correlations journal November 2019
Revealing the Correlation between Catalytic Selectivity and the Local Coordination Environment of Pt Single Atom journal August 2020
Conflicting Roles of Coordination Number on Catalytic Performance of Single-Atom Pt Catalysts journal April 2021
Strong Local Coordination Structure Effects on Subnanometer PtO x Clusters over CeO 2 Nanowires Probed by Low-Temperature CO Oxidation journal August 2015
Water-Mediated Mars–Van Krevelen Mechanism for CO Oxidation on Ceria-Supported Single-Atom Pt 1 Catalyst journal December 2016
Identifying Size Effects of Pt as Single Atoms and Nanoparticles Supported on FeO x for the Water-Gas Shift Reaction journal January 2018
Nanosize Effect of Al 2 O 3 in Ag/Al 2 O 3 Catalyst for the Selective Catalytic Oxidation of Ammonia journal February 2018
Tuning the Pt/CeO 2 Interface by in Situ Variation of the Pt Particle Size journal April 2018
Insights into the Activation Effect of H2 Pretreatment on Ag/Al2O3 Catalyst for the Selective Oxidation of Ammonia journal January 2019
Theoretical Approach To Predict the Stability of Supported Single-Atom Catalysts journal March 2019
Tailoring of the Proximity of Platinum Single Atoms on CeO 2 Using Phosphorus Boosts the Hydrogenation Activity journal July 2019
Crystal-Plane Effects of CeO2{110} and CeO2{100} on Photocatalytic CO2 Reduction: Synergistic Interactions of Oxygen Defects and Hydroxyl Groups journal August 2020
Surface Engineering Protocol To Obtain an Atomically Dispersed Pt/CeO 2 Catalyst with High Activity and Stability for CO Oxidation journal September 2018
Platinum Ion-Doped TiO 2 : High Catalytic Activity of Pt 2+ with Oxide Ion Vacancy in Ti 4+ 1– x Pt 2+ x O 2– x Compared to Pt 4+ without Oxide Ion Vacancy in Ti 4+ 1– x Pt 4+ x O 2 journal September 2013
Characterization of Cerium(IV) Oxide Ultrafine Particles Prepared Using Reversed Micelles journal October 1997
Probing the Surface Sites of CeO 2 Nanocrystals with Well-Defined Surface Planes via Methanol Adsorption and Desorption journal September 2012
Toward a Visible Light-Driven Photocatalyst: The Effect of Midgap-States-Induced Energy Gap of Undoped TiO 2 Nanoparticles journal November 2014
Insights into the Mechanism of n -Hexane Reforming over a Single-Site Platinum Catalyst journal September 2020
In Situ Raman Observation of Oxygen Activation and Reaction at Platinum–Ceria Interfaces during CO Oxidation journal September 2021
Tuning the Coordination Environment in Single-Atom Catalysts to Achieve Highly Efficient Oxygen Reduction Reactions journal December 2019
Efficient Hydrogen Production from Methanol Using a Single-Site Pt 1 /CeO 2 Catalyst journal October 2019
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen journal March 2019
Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation journal September 2019
Resolving the puzzle of single-atom silver dispersion on nanosized γ-Al2O3 surface for high catalytic performance journal January 2020
Identification of the active complex for CO oxidation over single-atom Ir-on-MgAl2O4 catalysts journal December 2018
The effect of coordination environment on the kinetic and thermodynamic stability of single-atom iron catalysts journal January 2020
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal December 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Communication: Improving the density functional theory+ U description of CeO 2 by including the contribution of the O 2 p electrons journal January 2012
Revealing the catalytic kinetics and dynamics of individual Pt atoms at the single-molecule level journal March 2022
Projector augmented-wave method journal December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Composition and structure of the RuO 2 ( 110 ) surface in an O 2 and CO environment: Implications for the catalytic formation of CO 2 journal July 2003
Generalized Gradient Approximation Made Simple journal October 1996
Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation journal December 2017

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