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Title: Tailoring Surface Frustrated Lewis Pairs of In 2 O 3− x (OH) y for Gas‐Phase Heterogeneous Photocatalytic Reduction of CO 2 by Isomorphous Substitution of In 3+ with Bi 3+

Abstract

Abstract Frustrated Lewis pairs (FLPs) created by sterically hindered Lewis acids and Lewis bases have shown their capacity for capturing and reacting with a variety of small molecules, including H 2 and CO 2 , and thereby creating a new strategy for CO 2 reduction. Here, the photocatalytic CO 2 reduction behavior of defect‐laden indium oxide (In 2 O 3− x (OH) y ) is greatly enhanced through isomorphous substitution of In 3+ with Bi 3+ , providing fundamental insights into the catalytically active surface FLPs (i.e., InOH···In) and the experimentally observed “volcano” relationship between the CO production rate and Bi 3+ substitution level. According to density functional theory calculations at the optimal Bi 3+ substitution level, the 6s 2 electron pair of Bi 3+ hybridizes with the oxygen in the neighboring InOH Lewis base site, leading to mildly increased Lewis basicity without influencing the Lewis acidity of the nearby In Lewis acid site. Meanwhile, Bi 3+ can act as an extra acid site, serving to maximize the heterolytic splitting of reactant H 2 , and results in a more hydridic hydride for more efficient CO 2 reduction. This study demonstrates that isomorphous substitution can effectively optimize the reactivity ofmore » surface catalytic active sites in addition to influencing optoelectronic properties, affording a better understanding of the photocatalytic CO 2 reduction mechanism.« less

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [2];  [2];  [6];  [7];  [8];  [1];  [9];  [1];  [10];  [1];  [1];  [4];  [11];  [2] more »; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Department of Chemistry University of Toronto 80 St. George Street, Rm 326 Toronto Ontario M5S 3H6 Canada
  2. Department of Materials Science and Engineering University of Toronto 184 College Street, Suite 140 Toronto Ontario M5S 3E4 Canada
  3. Laboratory for Electron Microscopy (LEM) Karlsruhe Institute of Technology (KIT) Engesserstr. 7 76131 Karlsruhe Germany
  4. Department of Chemistry Dalhousie University 6274 Coburg Road, P.O. Box 15000 Halifax B3H 4R2 Canada
  5. The Edward S. Rogers Sr. Department of Electrical and Computer Engineering University of Toronto 10 King's College Road Toronto Ontario M5S 3G4 Canada
  6. Institute of Nanotechnology and Karlsruhe Nano Micro Facility Karlsruhe Institute of Technology Hermann‐von‐Helmholtz Platz 1 76344 Eggenstein‐Leopoldshafen Germany
  7. Helmholtz‐Institute Ulm for Electrochemical Energy Storage (HIU) Karlsruhe Institute of Technology (KIT) 89081 Ulm Germany
  8. Institute of Nanotechnology and Karlsruhe Nano Micro Facility Karlsruhe Institute of Technology Hermann‐von‐Helmholtz Platz 1 76344 Eggenstein‐Leopoldshafen Germany, Helmholtz‐Institute Ulm for Electrochemical Energy Storage (HIU) Karlsruhe Institute of Technology (KIT) 89081 Ulm Germany
  9. Institute of Functional Nano and Soft Materials (FUNSOM) Soochow University Suzhou 215123 Jiangsu China
  10. Institute of Coal Chemistry Chinese Academy of Science 27 Taoyuan South Road Taiyuan 030001 Shanxi China
  11. Department of Materials Science and Engineering University of Toronto 184 College Street, Suite 140 Toronto Ontario M5S 3E4 Canada, The Edward S. Rogers Sr. Department of Electrical and Computer Engineering University of Toronto 10 King's College Road Toronto Ontario M5S 3G4 Canada
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1425539
Alternate Identifier(s):
OSTI ID: 1425541
Resource Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Name: Advanced Science Journal Volume: 5 Journal Issue: 6; Journal ID: ISSN 2198-3844
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Dong, Yuchan, Ghuman, Kulbir Kaur, Popescu, Radian, Duchesne, Paul N., Zhou, Wenjie, Loh, Joel Y. Y., Ali, Feysal M., Jia, Jia, Wang, Di, Mu, Xiaoke, Kübel, Christian, Wang, Lu, He, Le, Ghoussoub, Mireille, Wang, Qiang, Wood, Thomas E., Reyes, Laura M., Zhang, Peng, Kherani, Nazir P., Singh, Chandra Veer, and Ozin, Geoffrey A. Tailoring Surface Frustrated Lewis Pairs of In 2 O 3− x (OH) y for Gas‐Phase Heterogeneous Photocatalytic Reduction of CO 2 by Isomorphous Substitution of In 3+ with Bi 3+. Germany: N. p., 2018. Web. doi:10.1002/advs.201700732.
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Dong, Yuchan, Ghuman, Kulbir Kaur, Popescu, Radian, Duchesne, Paul N., Zhou, Wenjie, Loh, Joel Y. Y., Ali, Feysal M., Jia, Jia, Wang, Di, Mu, Xiaoke, Kübel, Christian, Wang, Lu, He, Le, Ghoussoub, Mireille, Wang, Qiang, Wood, Thomas E., Reyes, Laura M., Zhang, Peng, Kherani, Nazir P., Singh, Chandra Veer, & Ozin, Geoffrey A. Tailoring Surface Frustrated Lewis Pairs of In 2 O 3− x (OH) y for Gas‐Phase Heterogeneous Photocatalytic Reduction of CO 2 by Isomorphous Substitution of In 3+ with Bi 3+. Germany. https://doi.org/10.1002/advs.201700732
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Dong, Yuchan, Ghuman, Kulbir Kaur, Popescu, Radian, Duchesne, Paul N., Zhou, Wenjie, Loh, Joel Y. Y., Ali, Feysal M., Jia, Jia, Wang, Di, Mu, Xiaoke, Kübel, Christian, Wang, Lu, He, Le, Ghoussoub, Mireille, Wang, Qiang, Wood, Thomas E., Reyes, Laura M., Zhang, Peng, Kherani, Nazir P., Singh, Chandra Veer, and Ozin, Geoffrey A. Mon . "Tailoring Surface Frustrated Lewis Pairs of In 2 O 3− x (OH) y for Gas‐Phase Heterogeneous Photocatalytic Reduction of CO 2 by Isomorphous Substitution of In 3+ with Bi 3+". Germany. https://doi.org/10.1002/advs.201700732.
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@article{osti_1425539,
title = {Tailoring Surface Frustrated Lewis Pairs of In 2 O 3− x (OH) y for Gas‐Phase Heterogeneous Photocatalytic Reduction of CO 2 by Isomorphous Substitution of In 3+ with Bi 3+},
author = {Dong, Yuchan and Ghuman, Kulbir Kaur and Popescu, Radian and Duchesne, Paul N. and Zhou, Wenjie and Loh, Joel Y. Y. and Ali, Feysal M. and Jia, Jia and Wang, Di and Mu, Xiaoke and Kübel, Christian and Wang, Lu and He, Le and Ghoussoub, Mireille and Wang, Qiang and Wood, Thomas E. and Reyes, Laura M. and Zhang, Peng and Kherani, Nazir P. and Singh, Chandra Veer and Ozin, Geoffrey A.},
abstractNote = {Abstract Frustrated Lewis pairs (FLPs) created by sterically hindered Lewis acids and Lewis bases have shown their capacity for capturing and reacting with a variety of small molecules, including H 2 and CO 2 , and thereby creating a new strategy for CO 2 reduction. Here, the photocatalytic CO 2 reduction behavior of defect‐laden indium oxide (In 2 O 3− x (OH) y ) is greatly enhanced through isomorphous substitution of In 3+ with Bi 3+ , providing fundamental insights into the catalytically active surface FLPs (i.e., InOH···In) and the experimentally observed “volcano” relationship between the CO production rate and Bi 3+ substitution level. According to density functional theory calculations at the optimal Bi 3+ substitution level, the 6s 2 electron pair of Bi 3+ hybridizes with the oxygen in the neighboring InOH Lewis base site, leading to mildly increased Lewis basicity without influencing the Lewis acidity of the nearby In Lewis acid site. Meanwhile, Bi 3+ can act as an extra acid site, serving to maximize the heterolytic splitting of reactant H 2 , and results in a more hydridic hydride for more efficient CO 2 reduction. This study demonstrates that isomorphous substitution can effectively optimize the reactivity of surface catalytic active sites in addition to influencing optoelectronic properties, affording a better understanding of the photocatalytic CO 2 reduction mechanism.},
doi = {10.1002/advs.201700732},
journal = {Advanced Science},
number = 6,
volume = 5,
place = {Germany},
year = {Mon Mar 12 00:00:00 EDT 2018},
month = {Mon Mar 12 00:00:00 EDT 2018}
}
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