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

Abstract

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.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
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  1. Univ. of Toronto, ON (Canada)
  2. Sun Yat-sen Univ., Guangzhou, Guangdong (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
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)
OSTI Identifier:
1682338
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Heterogeneous catalysis; Nanoparticles; Photocatalysis

Citation Formats

Xu, Yang-Fan, Duchesne, Paul N., Wang, Lu, Tavasoli, Alexandra, Jelle, Abdinoor A., Xia, Meikun, Liao, Jin-Feng, Kuang, Dai-Bin, and Ozin, Geoffrey A. High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides. United States: N. p., 2020. Web. doi:10.1038/s41467-020-18943-2.
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Xu, Yang-Fan, Duchesne, Paul N., Wang, Lu, Tavasoli, Alexandra, Jelle, Abdinoor A., Xia, Meikun, Liao, Jin-Feng, Kuang, Dai-Bin, & Ozin, Geoffrey A. High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides. United States. https://doi.org/10.1038/s41467-020-18943-2
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Xu, Yang-Fan, Duchesne, Paul N., Wang, Lu, Tavasoli, Alexandra, Jelle, Abdinoor A., Xia, Meikun, Liao, Jin-Feng, Kuang, Dai-Bin, and Ozin, Geoffrey A. Tue . "High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides". United States. https://doi.org/10.1038/s41467-020-18943-2. https://www.osti.gov/servlets/purl/1682338.
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@article{osti_1682338,
title = {High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides},
author = {Xu, Yang-Fan and Duchesne, Paul N. and Wang, Lu and Tavasoli, Alexandra and Jelle, Abdinoor A. and Xia, Meikun and Liao, Jin-Feng and Kuang, Dai-Bin and Ozin, Geoffrey A.},
abstractNote = {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.},
doi = {10.1038/s41467-020-18943-2},
journal = {Nature Communications},
number = ,
volume = 11,
place = {United States},
year = {Tue Oct 13 00:00:00 EDT 2020},
month = {Tue Oct 13 00:00:00 EDT 2020}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1038/s41467-020-18943-2
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