|
Title
|
|
|
|
Dopant-induced electron localization drives reduction to hydrocarbons
| |
|
Author
|
|
|
|
| |
|
Abstract
|
|
|
|
| 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. |
| |
|
Language
|
|
|
|
English
| |
|
Source (journal)
|
|
|
|
Nature chemistry
| |
|
Publication
|
|
|
|
2018
| |
|
ISSN
|
|
|
|
1755-4330
1755-4349
| |
|
DOI
|
|
|
|
10.1038/S41557-018-0092-X
| |
|
Volume/pages
|
|
|
|
10
:9
(2018)
, p. 974-980
| |
|
ISI
|
|
|
|
000442395200013
| |
|
Pubmed ID
|
|
|
|
30013194
| |
|
Full text (Publisher's DOI)
|
|
|
|
| |
|
Full text (open access)
|
|
|
|
| |
|
Full text (publisher's version - intranet only)
|
|
|
|
| |
|