skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides

Journal Article · · Nature Communications

Akin to single-site homogeneous catalysis, a long sought-after goal is to achieve reaction site precision in heterogeneous catalysis for chemical control over patterns of activity, selectivity and stability. Herein, we report on metal phosphides as a class of material capable of realizing these attributes and unlock their potential in solar-driven CO2 hydrogenation. Selected as an archetype, Ni12P5 affords a structure based upon highly dispersed nickel nanoclusters integrated into a phosphorus lattice that harvest light intensely across the entire solar spectral range. Motivated by its panchromatic absorption and unique linearly bonded nickel-carbonyl-dominated reaction route, Ni12P5 is found to be a photothermal catalyst for the reverse water gas shift reaction, offering a CO production rate of 960 ± 12 mmol gcat–1 h–1, near 100% selectivity and long-term stability. Successful extension of this idea to Co2P analogs implies that metal phosphide materials are poised as a universal platform for high-rate and highly selective photothermal CO2 catalysis.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
Ontario Ministry of Research and Innovation; Ministry of Economic Development, Employment and Infrastructure; Ministry of the Environment and Climate Change; Best in Science; Ministry of Research Innovation and Science Low Carbon Innovation Fund; Ontario Centre of Excellence Solutions 2030 Challenge Fund; Alexander von Humboldt Foundation; Imperial Oil; University of Toronto Connaught Innovation Fund; Connaught Global Challenge Fund; Natural Sciences and Engineering Research Council of Canada (NSERC); National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1682338
Journal Information:
Nature Communications, Vol. 11; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
ENGLISH

References (39)

Catalytic CO2 reduction by palladium-decorated silicon–hydride nanosheets journal December 2018
Cu2O nanocubes with mixed oxidation-state facets for (photo)catalytic hydrogenation of carbon dioxide journal September 2019
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal March 2019
From Solar Energy to Fuels: Recent Advances in Light-Driven C 1 Chemistry journal September 2019
Alumina‐Supported CoFe Alloy Catalysts Derived from Layered‐Double‐Hydroxide Nanosheets for Efficient Photothermal CO 2 Hydrogenation to Hydrocarbons journal December 2017
Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles journal April 2018
Unravelling structure sensitivity in CO2 hydrogenation over nickel journal January 2018
Tuning of catalytic sites in Pt/TiO2 catalysts for the chemoselective hydrogenation of 3-nitrostyrene journal September 2019
Well-Defined Materials for Heterogeneous Catalysis: From Nanoparticles to Isolated Single-Atom Sites journal December 2019
Design of atomically dispersed catalytic sites for photocatalytic CO 2 reduction journal January 2019
Recent advances in transition metal phosphide nanomaterials: synthesis and applications in hydrogen evolution reaction journal January 2016
Transition metal phosphide hydroprocessing catalysts: A review journal May 2009
Nanoscaled Metal Borides and Phosphides: Recent Developments and Perspectives journal June 2013
N-induced lattice contraction generally boosts the hydrogen evolution catalysis of P-rich metal phosphides journal January 2020
A Highly Active Molybdenum Phosphide Catalyst for Methanol Synthesis from CO and CO 2 journal October 2018
Ultradispersed Nickel Phosphide on Phosphorus-Doped Carbon with Tailored d-Band Center for Efficient and Chemoselective Hydrogenation of Nitroarenes journal August 2018
Visible and Near-Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO 2 over Nanostructured Pd@Nb 2 O 5 journal July 2016
Thiophene hydrodesulfurization over nickel phosphide catalysts: effect of the precursor composition and support journal April 2005
Infrared Spectroscopic Investigation of CO Adsorption on Silica-Supported Nickel Phosphide Catalysts journal July 2004
Metal Phosphides Derived from Hydrotalcite Precursors toward the Selective Hydrogenation of Phenylacetylene journal August 2015
Structure and reactivity of plasma treated Ni/Al2O3 catalyst for CO2 reforming of methane journal May 2008
Nature of active sites in Ni2P hydrotreating catalysts as probed by iron substitution journal March 2015
Stable Active Sites on Ni 12 P 5 Surfaces for the Hydrogen Evolution Reaction journal May 2019
The ensemble effect of formic acid oxidation on platinum–gold electrode studied by first-principles calculations journal March 2015
Golden single-atomic-site platinum electrocatalysts journal September 2018
Catalysts for Hydrogen Evolution from the [NiFe] Hydrogenase to the Ni 2 P(001) Surface:  The Importance of Ensemble Effect journal October 2005
Nanostructured Nickel Phosphide as an Electrocatalyst for the Hydrogen Evolution Reaction journal June 2013
Water–gas-shift reaction on a Ni2P(001) catalyst: Formation of oxy-phosphides and highly active reaction sites journal March 2009
Theoretical Insights of Ni 2 P (0001) Surface toward Its Potential Applicability in CO 2 Conversion via Dry Reforming of Methane journal March 2019
Theoretical Insights and the Corresponding Construction of Supported Metal Catalysts for Highly Selective CO 2 to CO Conversion journal June 2017
Methanation of carbon dioxide on Ni-incorporated MCM-41 catalysts: The influence of catalyst pretreatment and study of steady-state reaction journal July 2007
Methanation of CO 2 and reverse water gas shift reactions on Ni/SiO 2 catalysts: the influence of particle size on selectivity and reaction pathway journal January 2015
Ni Single Atom Catalysts for CO 2 Activation journal January 2019
Development of Tandem Catalysts for CO 2 Hydrogenation to Olefins journal February 2019
In situ intermediate-energy X-ray catalysis research at the advanced photon source beamline 9-BM journal April 2013
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
WinXAS a Program for X-ray Absorption Spectroscopy Data Analysis under MS-Windows journal March 1998
Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure journal September 1998
Crystallography Open Database (COD): an open-access collection of crystal structures and platform for world-wide collaboration journal November 2011