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Title
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Dopant-induced electron localization drives reduction to hydrocarbons
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Author
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Abstract
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| The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C-2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C-2 products. Here, we use boron to tune the ratio of Cu delta+ to Cu-0 active sites and improve both stability and C-2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C-2 products. We report experimentally a C-2 Faradaic efficiency of 79 +/- 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of similar to 40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons. |
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Language
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English
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Source (journal)
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Nature chemistry
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Publication
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2018
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ISSN
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1755-4330
1755-4349
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Volume/pages
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10
:9
(2018)
, p. 974-980
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ISI
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000442395200013
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Pubmed ID
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30013194
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Full text (Publisher's DOI)
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Full text (open access)
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Full text (publisher's version - intranet only)
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