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

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:
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  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:
Report Number(s):
BNL-114817-2017-JA
Journal ID: ISSN 2198-3844; R&D Project: MA015MACA; KC0201010
Grant/Contract Number:
SC0012704; AC02-06CH11357; SC0012575
Type:
Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; CO2 conversion; photothermal catalysts; size effects; tunable selectivity
OSTI Identifier:
1372496
Alternate Identifier(s):
OSTI ID: 1372497; OSTI ID: 1412791