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Title: A stable low-temperature H2-production catalyst by crowding Pt on α-MoC

Journal Article · · Nature (London)
ORCiD logo [1];  [2];  [2];  [3];  [4]; ORCiD logo [5];  [6];  [7];  [8];  [2];  [2];  [2];  [3]; ORCiD logo [5];  [5];  [9];  [10]; ORCiD logo [11];  [3];  [2] more »;  [7]; ORCiD logo [12];  [13]; ORCiD logo [13]; ORCiD logo [9]; ORCiD logo [7];  [3]; ORCiD logo [2] « less
  1. Peking Univ., Beijing (China). Beijing National Laboratory for Molecular Sciences; Dalian Univ. of Technology (China). State Key Laboratory of Fine Chemicals
  2. Peking Univ., Beijing (China). Beijing National Laboratory for Molecular Sciences
  3. Chinese Academy of Sciences (CAS), Beijing (China). CAS Key Laboratory of Vacuum Physics
  4. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  5. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Institute of Applied Physics; Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Advanced Research Institute, Shanghai Synchrotron Radiation Facility
  6. Chinese Academy of Sciences (CAS), Taiyuan (China). State Key Laboratory of Coal Conversion; Synfuels China, Beijing (China); Inner Mongolia Univ., Hohhot (China)
  7. Dalian Univ. of Technology (China). State Key Laboratory of Fine Chemicals
  8. Zhejiang Univ., Hangzhou (China). Key Laboratory of Biomass Chemical Engineering of Ministry of Education
  9. Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering
  10. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Science and Engineering Division; NOVA Chemicals Corporation, Calgary, AB (Canada)
  11. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Science and Engineering Division
  12. Paul Scherrer Inst. (PSI), Villigen (Switzerland); Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
  13. Chinese Academy of Sciences (CAS), Taiyuan (China). State Key Laboratory of Coal Conversion; Synfuels China, Beijing (China)

The water-gas shift (WGS) reaction is an industrially important source of pure hydrogen (H2) at the expense of carbon monoxide and water. This reaction is of interest for fuel-cell applications, but requires WGS catalysts that are durable and highly active at low temperatures. Here we demonstrate that the structure (Pt1Ptn)/α-MoC, where isolated platinum atoms (Pt1) and subnanometre platinum clusters (Pt-n) are stabilized on alpha-molybdenum carbide (α-MoC), catalyses the WGS reaction even at 313 kelvin, with a hydrogen-production pathway involving direct carbon monoxide dissociation identified. We find that it is critical to crowd the α-MoC surface with Pt1 and Ptn species, which prevents oxidation of the support that would cause catalyst deactivation, as seen with gold/α-MoC, and gives our system high stability and a high metal-normalized turnover number of 4,300,000 moles of hydrogen per mole of platinum. We anticipate that the strategy demonstrated here will be pivotal for the design of highly active and stable catalysts for effective activation of important molecules such as water and carbon monoxide for energy production.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1808272
Journal Information:
Nature (London), Vol. 589, Issue 7842; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (32)

“Redox” vs “associative formate with –OH group regeneration” WGS reaction mechanism on Pt/CeO2: Effect of platinum particle size journal April 2011
A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation journal February 2019
Water–gas shift catalysis over transition metals supported on molybdenum carbide journal November 2015
Introducing Time Resolution to Detect Ce 3+ Catalytically Active Sites at the Pt/CeO 2 Interface through Ambient Pressure X-ray Photoelectron Spectroscopy journal December 2016
Operando NAP-XPS unveils differences in MoO3 and Mo2C during hydrodeoxygenation journal November 2018
Molybdenum Carbide as Alternative Catalysts to Precious Metals for Highly Selective Reduction of CO 2 to CO journal May 2014
Dissociation of CO and H2O during water–gas shift reaction on carburized Mo/Al2O3 catalyst journal May 2011
Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction journal December 2007
Catalytically active Au-O(OH) x - species stabilized by alkali ions on zeolites and mesoporous oxides journal November 2014
Hydrogen Activation and Metal Hydride Formation Trigger Cluster Formation from Supported Iridium Complexes journal March 2012
High Activity Carbide Supported Catalysts for Water Gas Shift journal March 2011
Imaging Isolated Gold Atom Catalytic Sites in Zeolite NaY journal March 2012
Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts journal May 2016
Application of near ambient pressure gas-phase X-ray photoelectron spectroscopy to the investigation of catalytic properties of copper in methanol oxidation journal February 2016
Atomically Dispersed Au–(OH) x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction journal March 2013
A Common Single-Site Pt(II)–O(OH) x – Species Stabilized by Sodium on “Active” and “Inert” Supports Catalyzes the Water-Gas Shift Reaction journal March 2015
Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts journal August 2003
Activity and stability of low-content gold–cerium oxide catalysts for the water–gas shift reaction journal March 2005
The effect of gold particle size on AuAu bond length and reactivity toward oxygen in supported catalysts journal June 2006
Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy journal April 2013
Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction journal June 2017
Carbide-Supported Au Catalysts for Water–Gas Shift Reactions: A New Territory for the Strong Metal–Support Interaction Effect journal September 2018
Remarkable Performance of Ir 1 /FeO x Single-Atom Catalyst in Water Gas Shift Reaction journal October 2013
The Environmental Photochemistry of Oxide Surfaces and the Nature of Frozen Salt Solutions: A New in Situ XPS Approach journal January 2016
Probing the Low-Temperature Water–Gas Shift Activity of Alkali-Promoted Platinum Catalysts Stabilized on Carbon Supports journal February 2014
Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts journal September 2015
Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation journal September 2008
Mononuclear Au III and Au I Complexes Bonded to Zeolite NaY:  Catalysts for CO Oxidation at 298 K journal November 2004
Alkali-Stabilized Pt-OHx Species Catalyze Low-Temperature Water-Gas Shift Reactions journal September 2010
Reactive metal–support interactions at moderate temperature in two-dimensional niobium-carbide-supported platinum catalysts journal May 2018
Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts journal March 2017
Comparison of the activity of Au/CeO2 and Au/Fe2O3 catalysts for the CO oxidation and the water-gas shift reactions journal June 2007