Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis

Gold inverse opal (Au-IO) thin films are active for CO[subscript 2] reduction to CO with high efficiency at modest overpotentials and high selectivity relative to hydrogen evolution. The specific activity for hydrogen evolution diminishes by 10-fold with increasing porous film thickness, while CO ev...

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Main Authors: Hall, Anthony Shoji, Yoon, Youngmin, Wuttig, Anna, Surendranath, Yogesh
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: American Chemical Society (ACS) 2016
Online Access:http://hdl.handle.net/1721.1/105469
https://orcid.org/0000-0003-4134-4160
https://orcid.org/0000-0002-8683-975X
https://orcid.org/0000-0001-9519-7907
https://orcid.org/0000-0003-1016-3420
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author Hall, Anthony Shoji
Yoon, Youngmin
Wuttig, Anna
Surendranath, Yogesh
author2 Massachusetts Institute of Technology. Department of Chemistry
author_facet Massachusetts Institute of Technology. Department of Chemistry
Hall, Anthony Shoji
Yoon, Youngmin
Wuttig, Anna
Surendranath, Yogesh
author_sort Hall, Anthony Shoji
collection MIT
description Gold inverse opal (Au-IO) thin films are active for CO[subscript 2] reduction to CO with high efficiency at modest overpotentials and high selectivity relative to hydrogen evolution. The specific activity for hydrogen evolution diminishes by 10-fold with increasing porous film thickness, while CO evolution activity is largely unchanged. We demonstrate that the origin of hydrogen suppression in Au-IO films stems from the generation of diffusional gradients within the pores of the mesostructured electrode rather than changes in surface faceting or Au grain size. For electrodes with optimal mesoporosity, 99% selectivity for CO evolution can be obtained at overpotentials as low as 0.4 V. These results establish electrode mesostructuring as a complementary method for tuning selectivity in CO[subscript 2] -to-fuels catalysis.
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spelling mit-1721.1/1054692022-10-01T22:24:44Z Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis Mesostructure-Induced Selectivity in CO2 Reduction Catalysis Hall, Anthony Shoji Yoon, Youngmin Wuttig, Anna Surendranath, Yogesh Massachusetts Institute of Technology. Department of Chemistry Surendranath, Yogesh Hall, Anthony Shoji Yoon, Youngmin Wuttig, Anna Surendranath, Yogesh Gold inverse opal (Au-IO) thin films are active for CO[subscript 2] reduction to CO with high efficiency at modest overpotentials and high selectivity relative to hydrogen evolution. The specific activity for hydrogen evolution diminishes by 10-fold with increasing porous film thickness, while CO evolution activity is largely unchanged. We demonstrate that the origin of hydrogen suppression in Au-IO films stems from the generation of diffusional gradients within the pores of the mesostructured electrode rather than changes in surface faceting or Au grain size. For electrodes with optimal mesoporosity, 99% selectivity for CO evolution can be obtained at overpotentials as low as 0.4 V. These results establish electrode mesostructuring as a complementary method for tuning selectivity in CO[subscript 2] -to-fuels catalysis. 2016-11-30T14:54:09Z 2016-11-30T14:54:09Z 2015-11 2015-08 Article http://purl.org/eprint/type/JournalArticle 0002-7863 1520-5126 http://hdl.handle.net/1721.1/105469 Hall, Anthony Shoji et al. “Mesostructure-Induced Selectivity in CO 2 Reduction Catalysis.” Journal of the American Chemical Society 137.47 (2015): 14834–14837. https://orcid.org/0000-0003-4134-4160 https://orcid.org/0000-0002-8683-975X https://orcid.org/0000-0001-9519-7907 https://orcid.org/0000-0003-1016-3420 en_US http://dx.doi.org/10.1021/jacs.5b08259 Journal of the American Chemical Society Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) Prof. Surendranath via Erja Kajosalo
spellingShingle Hall, Anthony Shoji
Yoon, Youngmin
Wuttig, Anna
Surendranath, Yogesh
Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title_full Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title_fullStr Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title_full_unstemmed Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title_short Mesostructure-Induced Selectivity in CO[subscript 2] Reduction Catalysis
title_sort mesostructure induced selectivity in co subscript 2 reduction catalysis
url http://hdl.handle.net/1721.1/105469
https://orcid.org/0000-0003-4134-4160
https://orcid.org/0000-0002-8683-975X
https://orcid.org/0000-0001-9519-7907
https://orcid.org/0000-0003-1016-3420
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AT surendranathyogesh mesostructureinducedselectivityincosubscript2reductioncatalysis
AT hallanthonyshoji mesostructureinducedselectivityinco2reductioncatalysis
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