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Title: Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity

Abstract

This study has designed and implemented a library of hetero-nanostructured catalysts, denoted as Pd@Nb2O5, comprised of size-controlled Pd nanocrystals interfaced with Nb2O5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb2O5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH4 production rates as high as 0.75 and 0.11 mol h–1 gPd–1, respectively. By contrast, using small Pd nanocrystals, a CO production rate surpassing 18.8 mol h–1 gPd–1 is observed with 99.5% CO selectivity. These performance metrics establish a new milestone in the champion league of catalytic nanomaterials that can enable solar-powered gas-phase heterogeneous CO2 reduction. In conclusion, the remarkable control over the catalytic performance of Pd@Nb2O5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.

Authors:
 [1];  [2];  [3];  [4];  [2];  [5];  [2];  [1];  [6];  [2];  [3];  [2];  [2];  [7];  [1];  [3];  [2];  [2];  [1];  [8] more »;  [9];  [1];  [5];  [10];  [1];  [11];  [1]; ORCiD logo [2] « less
  1. Department of Materials Science and Engineering, University of Toronto, 184 College Street Toronto Ontario M5S 3E4 Canada
  2. Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, 80 St. George Street Toronto Ontario M5S 3H6 Canada
  3. Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street Toronto Ontario M5S 3E5 Canada
  4. Department of Mechanical Engineering, Lassonde School of Engineering, York University, Toronto M3J 1P3 Canada
  5. Department of Chemistry, Dalhousie University, 6274 Coburg Road, P.O. Box 15000 Halifax Nova Scotia B3H 4R2 Canada
  6. Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory, Upton NY 11973 USA, Department of Physics, Temple University, Philadelphia PA 19122 USA
  7. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, The Chinese Academy of Sciences, Taiyuan 030001 P. R. China
  8. Zhejiang Key Laboratory of Drinking Water Safety and Distribution Technology, Zhejiang University, Hangzhou 310058 P. R. China
  9. Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory, Upton NY 11973 USA
  10. Department of Electrical and Computing Engineering, University of Toronto, 10 King's College Road Toronto Ontario M5S 3G4 Canada
  11. Department of Materials Science and Engineering, University of Toronto, 184 College Street Toronto Ontario M5S 3E4 Canada, Department of Electrical and Computing Engineering, University of Toronto, 10 King's College Road Toronto Ontario M5S 3G4 Canada
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1372496
Alternate Identifier(s):
OSTI ID: 1372497; OSTI ID: 1412791
Report Number(s):
BNL-114817-2017-JA
Journal ID: ISSN 2198-3844
Grant/Contract Number:  
AC02-06CH11357; SC0012575; SC0012704
Resource Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Name: Advanced Science; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
Germany
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; CO2 conversion; photothermal catalysts; size effects; tunable selectivity

Citation Formats

Jia, Jia, Wang, Hong, Lu, Zhuole, O'Brien, Paul G., Ghoussoub, Mireille, Duchesne, Paul, Zheng, Ziqi, Li, Peicheng, Qiao, Qiao, Wang, Lu, Gu, Alan, Jelle, Abdinoor A., Dong, Yuchan, Wang, Qiang, Ghuman, Kulbir Kaur, Wood, Thomas, Qian, Chenxi, Shao, Yue, Qiu, Chenyue, Ye, Miaomiao, Zhu, Yimei, Lu, Zheng-Hong, Zhang, Peng, Helmy, Amr S., Singh, Chandra Veer, Kherani, Nazir P., Perovic, Doug D., and Ozin, Geoffrey A. Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity. Germany: N. p., 2017. Web. doi:10.1002/advs.201700252.
Jia, Jia, Wang, Hong, Lu, Zhuole, O'Brien, Paul G., Ghoussoub, Mireille, Duchesne, Paul, Zheng, Ziqi, Li, Peicheng, Qiao, Qiao, Wang, Lu, Gu, Alan, Jelle, Abdinoor A., Dong, Yuchan, Wang, Qiang, Ghuman, Kulbir Kaur, Wood, Thomas, Qian, Chenxi, Shao, Yue, Qiu, Chenyue, Ye, Miaomiao, Zhu, Yimei, Lu, Zheng-Hong, Zhang, Peng, Helmy, Amr S., Singh, Chandra Veer, Kherani, Nazir P., Perovic, Doug D., & Ozin, Geoffrey A. Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity. Germany. doi:10.1002/advs.201700252.
Jia, Jia, Wang, Hong, Lu, Zhuole, O'Brien, Paul G., Ghoussoub, Mireille, Duchesne, Paul, Zheng, Ziqi, Li, Peicheng, Qiao, Qiao, Wang, Lu, Gu, Alan, Jelle, Abdinoor A., Dong, Yuchan, Wang, Qiang, Ghuman, Kulbir Kaur, Wood, Thomas, Qian, Chenxi, Shao, Yue, Qiu, Chenyue, Ye, Miaomiao, Zhu, Yimei, Lu, Zheng-Hong, Zhang, Peng, Helmy, Amr S., Singh, Chandra Veer, Kherani, Nazir P., Perovic, Doug D., and Ozin, Geoffrey A. Tue . "Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity". Germany. doi:10.1002/advs.201700252.
@article{osti_1372496,
title = {Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity},
author = {Jia, Jia and Wang, Hong and Lu, Zhuole and O'Brien, Paul G. and Ghoussoub, Mireille and Duchesne, Paul and Zheng, Ziqi and Li, Peicheng and Qiao, Qiao and Wang, Lu and Gu, Alan and Jelle, Abdinoor A. and Dong, Yuchan and Wang, Qiang and Ghuman, Kulbir Kaur and Wood, Thomas and Qian, Chenxi and Shao, Yue and Qiu, Chenyue and Ye, Miaomiao and Zhu, Yimei and Lu, Zheng-Hong and Zhang, Peng and Helmy, Amr S. and Singh, Chandra Veer and Kherani, Nazir P. and Perovic, Doug D. and Ozin, Geoffrey A.},
abstractNote = {This study has designed and implemented a library of hetero-nanostructured catalysts, denoted as Pd@Nb2O5, comprised of size-controlled Pd nanocrystals interfaced with Nb2O5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb2O5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH4 production rates as high as 0.75 and 0.11 mol h–1 gPd–1, respectively. By contrast, using small Pd nanocrystals, a CO production rate surpassing 18.8 mol h–1 gPd–1 is observed with 99.5% CO selectivity. These performance metrics establish a new milestone in the champion league of catalytic nanomaterials that can enable solar-powered gas-phase heterogeneous CO2 reduction. In conclusion, the remarkable control over the catalytic performance of Pd@Nb2O5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.},
doi = {10.1002/advs.201700252},
journal = {Advanced Science},
number = ,
volume = ,
place = {Germany},
year = {2017},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1002/advs.201700252

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Cited by: 4 works
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    Works referencing / citing this record:

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    Dish-like higher-ordered palladium nanostructures through metal ion-ligand complexation
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