Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation

Zhang, Xiao; Li, Xueqian; Zhang, Du; Su, Neil Qiang; Yang, Weitao; Everitt, Henry O.; Liu, Jie

doi:10.1038/ncomms14542

Title: Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation

Journal Article · Thu Feb 23 00:00:00 EST 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms14542· OSTI ID:1367174

Zhang, Xiao ^[1];

^[1]; Zhang, Du ^[1]; Su, Neil Qiang ^[1]; Yang, Weitao ^[1];

^[2]; Liu, Jie ^[1]

Duke Univ., Durham, NC (United States)
Duke Univ., Durham, NC (United States); Army Aviation & Missile RD&E Center, Redstone Arsenal, AL (United States)

Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. As a result, the reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350°C.

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Research Organization:: Temple Univ., Philadelphia, PA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012575

OSTI ID:: 1367174

Journal Information:: Nature Communications, Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 1080 works

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Emerging Applications of Plasmons in Driving CO ₂ Reduction and N ₂ Fixation Yang, Jianhua; Guo, Yanzhen; Lu, Wenzheng Advanced Materials, Vol. 30, Issue 48 https://doi.org/10.1002/adma.201802227	journal	July 2018
Efficiency and Bond Selectivity in Plasmon-Induced Photochemistry Cortés, Emiliano Advanced Optical Materials, Vol. 5, Issue 15 https://doi.org/10.1002/adom.201700191	journal	June 2017
Mechanistic Studies of Plasmon Chemistry on Metal Catalysts Kazuma, Emiko; Kim, Yousoo Angewandte Chemie, Vol. 131, Issue 15 https://doi.org/10.1002/ange.201811234	journal	April 2019
Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C ₁ ‐Solarchemie Chen, Guangbo; Waterhouse, Geoffrey I. N.; Shi, Run Angewandte Chemie, Vol. 131, Issue 49 https://doi.org/10.1002/ange.201814313	journal	September 2019
Kopplung von Solarenergie und Wärmeenergie zur Kohlendioxidreduktion: Aktueller Stand und Perspektiven Wang, Zhou‐jun; Song, Hui; Liu, Huimin Angewandte Chemie, Vol. 132, Issue 21 https://doi.org/10.1002/ange.201907443	journal	February 2020
Synergy between Plasmonic and Electrocatalytic Activation of Methanol Oxidation on Palladium–Silver Alloy Nanotubes Huang, Lin; Zou, Jiasui; Ye, Jin‐Yu Angewandte Chemie International Edition, Vol. 58, Issue 26 https://doi.org/10.1002/anie.201903290	journal	June 2019
Thermo‐Photocatalysis: Environmental and Energy Applications Nair, Vaishakh; Muñoz‐Batista, Mario J.; Fernández‐García, Marcos ChemSusChem, Vol. 12, Issue 10 https://doi.org/10.1002/cssc.201900175	journal	April 2019
Chiroptically Active Metallic Nanohelices with Helical Anisotropy Huang, Zhifeng; Liu, Junjun Small, Vol. 13, Issue 43 https://doi.org/10.1002/smll.201701883	journal	September 2017
Understanding the roles of plasmonic Au nanocrystal size, shape, aspect ratio and loading amount in Au/g-C ₃ N ₄ hybrid nanostructures for photocatalytic hydrogen generation Guo, Yanzhen; Jia, Henglei; Yang, Jianhua Physical Chemistry Chemical Physics, Vol. 20, Issue 34 https://doi.org/10.1039/c8cp04241a	journal	January 2018
Using plasmonically generated carriers as redox equivalents Yu, Sungju; Mohan, Varun; Jain, Prashant K. MRS Bulletin, Vol. 45, Issue 1 https://doi.org/10.1557/mrs.2019.293	journal	January 2020
The Quest for Low Loss High Refractive Index Dielectric Materials for UV Photonic Applications Gutiérrez, Yael; Ortiz, Dolores; Saiz, José Applied Sciences, Vol. 8, Issue 11 https://doi.org/10.3390/app8112065	journal	October 2018
Biogenic Methane Strąpoć, Dariusz Encyclopedia of Earth Sciences Series https://doi.org/10.1007/978-3-319-39312-4_166	book	January 2018
A Photochemical Route towards Metal Sulfide Nanosheets from Layered Metal Thiolate Complexes Guo, Jiahao; Cao, Yitao; Shi, Run Angewandte Chemie https://doi.org/10.1002/ange.201902791	journal	May 2019
The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol Sarhan, Radwan M.; Koopman, Wouter; Schuetz, Roman Universität Potsdam https://doi.org/10.25932/publishup-42719	text	January 2019
Synergy between Plasmonic and Electrocatalytic Activation of Methanol Oxidation on Palladium–Silver Alloy Nanotubes Huang, Lin; Zou, Jiasui; Ye, Jin‐Yu Angewandte Chemie, Vol. 131, Issue 26 https://doi.org/10.1002/ange.201903290	journal	May 2019
Photothermal Catalyst Engineering: Hydrogenation of Gaseous CO ₂ with High Activity and Tailored Selectivity Jia, Jia; Wang, Hong; Lu, Zhuole Advanced Science, Vol. 4, Issue 10 https://doi.org/10.1002/advs.201700252	journal	July 2017
Self-Optimized Catalysts: Hot-Electron Driven Photosynthesis of Catalytic Photocathodes Kontoleta, Evgenia; Askes, Sven H. C.; Garnett, Erik C. ACS Applied Materials & Interfaces, Vol. 11, Issue 39 https://doi.org/10.1021/acsami.9b10913	journal	September 2019
Sunlight-Fueled, Low-Temperature Ru-Catalyzed Conversion of CO₂ and H₂ to CH₄ with a High Photon-to-Methane Efficiency Sastre, Francesc; Versluis, Caroline; Meulendijks, Nicole ACS Omega, Vol. 4, Issue 4 https://doi.org/10.1021/acsomega.9b00581	journal	April 2019
In-situ observation of plasmon-controlled photocatalytic dehydrogenation of individual palladium nanoparticles Vadai, Michal; Angell, Daniel K.; Hayee, Fariah Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-07108-x	journal	November 2018

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