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

Title: Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO 2 with High Activity and Tailored Selectivity

Abstract

This study has designed and implemented a library of hetero-nanostructured catalysts, denoted as Pd@Nb 2O 5, comprised of size-controlled Pd nanocrystals interfaced with Nb 2O 5 nanorods. This study also demonstrates that the catalytic activity and selectivity of CO 2 reduction to CO and CH 4 products can be systematically tailored by varying the size of the Pd nanocrystals supported on the Nb 2O 5 nanorods. Using large Pd nanocrystals, this study achieves CO and CH 4 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 CO 2 reduction. In conclusion, the remarkable control over the catalytic performance of Pd@Nb 2O 5 is demonstrated to stem from a combination of photothermal, electronic and size effects, which is rationally tunable through nanochemistry.

Authors:
 [1];  [1];  [1];  [2];  [1];  [3];  [1];  [1];  [4];  [1];  [1];  [1];  [1];  [5];  [1];  [1];  [1];  [1];  [1];  [6] more »;  [7];  [1];  [3];  [1];  [1];  [1];  [1]; ORCiD logo [1] « less
  1. Univ. of Toronto, Toronto, ON (Canada)
  2. York Univ., Toronto (Canada)
  3. Dalhousie Univ., Halifax, NS (Canada)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Temple Univ., Philadelphia, PA (United States)
  5. The Chinese Academy of Sciences, Taiyuan (People's Republic of China)
  6. Zhejiang Univ., Hangzhou (People's Republic of China)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (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; R&D Project: MA015MACA; KC0201010
Grant/Contract Number:
SC0012704; AC02-06CH11357; SC0012575
Resource Type:
Journal Article: Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
United States
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. United States: 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. United States. 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". United States. 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 = 10,
volume = 4,
place = {United States},
year = {Tue Jul 25 00:00:00 EDT 2017},
month = {Tue Jul 25 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/advs.201700252

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share: