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 pro...
Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
Wiley
2017-10-01
|
Series: | Advanced Science |
Subjects: | |
Online Access: | https://doi.org/10.1002/advs.201700252 |
_version_ | 1797754215263633408 |
---|---|
author | Jia Jia Hong Wang Zhuole Lu Paul G. O'Brien Mireille Ghoussoub Paul Duchesne Ziqi Zheng Peicheng Li Qiao Qiao Lu Wang Alan Gu Feysal M. Ali Yuchan Dong Qiang Wang Kulbir Kaur Ghuman Thomas Wood Chenxi Qian Yue Shao Chenyue Qiu Miaomiao Ye Yimei Zhu Zheng‐Hong Lu Peng Zhang Amr S. Helmy Chandra Veer Singh Nazir P. Kherani Doug D. Perovic Geoffrey A. Ozin |
author_facet | Jia Jia Hong Wang Zhuole Lu Paul G. O'Brien Mireille Ghoussoub Paul Duchesne Ziqi Zheng Peicheng Li Qiao Qiao Lu Wang Alan Gu Feysal M. Ali Yuchan Dong Qiang Wang Kulbir Kaur Ghuman Thomas Wood Chenxi Qian Yue Shao Chenyue Qiu Miaomiao Ye Yimei Zhu Zheng‐Hong Lu Peng Zhang Amr S. Helmy Chandra Veer Singh Nazir P. Kherani Doug D. Perovic Geoffrey A. Ozin |
author_sort | Jia Jia |
collection | DOAJ |
description | 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. 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. |
first_indexed | 2024-03-12T17:29:29Z |
format | Article |
id | doaj.art-2e049711e8e54bd88538e38c656861ea |
institution | Directory Open Access Journal |
issn | 2198-3844 |
language | English |
last_indexed | 2024-03-12T17:29:29Z |
publishDate | 2017-10-01 |
publisher | Wiley |
record_format | Article |
series | Advanced Science |
spelling | doaj.art-2e049711e8e54bd88538e38c656861ea2023-08-05T03:41:05ZengWileyAdvanced Science2198-38442017-10-01410n/an/a10.1002/advs.201700252Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored SelectivityJia Jia0Hong Wang1Zhuole Lu2Paul G. O'Brien3Mireille Ghoussoub4Paul Duchesne5Ziqi Zheng6Peicheng Li7Qiao Qiao8Lu Wang9Alan Gu10Feysal M. Ali11Yuchan Dong12Qiang Wang13Kulbir Kaur Ghuman14Thomas Wood15Chenxi Qian16Yue Shao17Chenyue Qiu18Miaomiao Ye19Yimei Zhu20Zheng‐Hong Lu21Peng Zhang22Amr S. Helmy23Chandra Veer Singh24Nazir P. Kherani25Doug D. Perovic26Geoffrey A. Ozin27Department of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaDepartment of Chemical Engineering and Applied Chemistry University of Toronto 200 College Street Toronto Ontario M5S 3E5 CanadaDepartment of Mechanical Engineering Lassonde School of Engineering York University Toronto M3J 1P3 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaDepartment of Chemistry Dalhousie University 6274 Coburg Road, P.O. Box 15000 Halifax Nova Scotia B3H 4R2 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaCondensed Matter Physics and Materials Science Department Brookhaven National Laboratory Upton NY 11973 USAMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaDepartment of Chemical Engineering and Applied Chemistry University of Toronto 200 College Street Toronto Ontario M5S 3E5 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaState Key Laboratory of Coal Conversion Institute of Coal Chemistry The Chinese Academy of Sciences Taiyuan 030001 P. R. ChinaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaDepartment of Chemical Engineering and Applied Chemistry University of Toronto 200 College Street Toronto Ontario M5S 3E5 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaZhejiang Key Laboratory of Drinking Water Safety and Distribution Technology Zhejiang University Hangzhou 310058 P. R. ChinaCondensed Matter Physics and Materials Science Department Brookhaven National Laboratory Upton NY 11973 USADepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaDepartment of Chemistry Dalhousie University 6274 Coburg Road, P.O. Box 15000 Halifax Nova Scotia B3H 4R2 CanadaDepartment of Electrical and Computing Engineering University of Toronto 10 King's College Road Toronto Ontario M5S 3G4 CanadaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaDepartment of Materials Science and Engineering University of Toronto 184 College Street Toronto Ontario M5S 3E4 CanadaMaterials Chemistry and Nanochemistry Research Group Solar Fuels Cluster Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 CanadaAbstract 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. 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.https://doi.org/10.1002/advs.201700252CO2 conversionphotothermal catalystssize effectstunable selectivity |
spellingShingle | Jia Jia Hong Wang Zhuole Lu Paul G. O'Brien Mireille Ghoussoub Paul Duchesne Ziqi Zheng Peicheng Li Qiao Qiao Lu Wang Alan Gu Feysal M. Ali Yuchan Dong Qiang Wang Kulbir Kaur Ghuman Thomas Wood Chenxi Qian Yue Shao Chenyue Qiu Miaomiao Ye Yimei Zhu Zheng‐Hong Lu Peng Zhang Amr S. Helmy Chandra Veer Singh Nazir P. Kherani Doug D. Perovic Geoffrey A. Ozin Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity Advanced Science CO2 conversion photothermal catalysts size effects tunable selectivity |
title | Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity |
title_full | Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity |
title_fullStr | Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity |
title_full_unstemmed | Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity |
title_short | Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO2 with High Activity and Tailored Selectivity |
title_sort | photothermal catalyst engineering hydrogenation of gaseous co2 with high activity and tailored selectivity |
topic | CO2 conversion photothermal catalysts size effects tunable selectivity |
url | https://doi.org/10.1002/advs.201700252 |
work_keys_str_mv | AT jiajia photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT hongwang photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT zhuolelu photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT paulgobrien photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT mireilleghoussoub photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT paulduchesne photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT ziqizheng photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT peichengli photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT qiaoqiao photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT luwang photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT alangu photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT feysalmali photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT yuchandong photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT qiangwang photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT kulbirkaurghuman photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT thomaswood photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT chenxiqian photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT yueshao photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT chenyueqiu photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT miaomiaoye photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT yimeizhu photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT zhenghonglu photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT pengzhang photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT amrshelmy photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT chandraveersingh photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT nazirpkherani photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT dougdperovic photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity AT geoffreyaozin photothermalcatalystengineeringhydrogenationofgaseousco2withhighactivityandtailoredselectivity |