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Atomic layer confined vacancies for atomic-level insights into carbon dioxide electroreduction.


ABSTRACT: The role of oxygen vacancies in carbon dioxide electroreduction remains somewhat unclear. Here we construct a model of oxygen vacancies confined in atomic layer, taking the synthetic oxygen-deficient cobalt oxide single-unit-cell layers as an example. Density functional theory calculations demonstrate the main defect is the oxygen(II) vacancy, while X-ray absorption fine structure spectroscopy reveals their distinct oxygen vacancy concentrations. Proton transfer is theoretically/experimentally demonstrated to be a rate-limiting step, while energy calculations unveil that the presence of oxygen(II) vacancies lower the rate-limiting activation barrier from 0.51 to 0.40 eV via stabilizing the formate anion radical intermediate, confirmed by the lowered onset potential from 0.81 to 0.78 V and decreased Tafel slope from 48 to 37 mV dec-1. Hence, vacancy-rich cobalt oxide single-unit-cell layers exhibit current densities of 2.7 mA cm-2 with ca. 85% formate selectivity during 40-h tests. This work establishes a clear atomic-level correlation between oxygen vacancies and carbon dioxide electroreduction.

SUBMITTER: Gao S 

PROVIDER: S-EPMC5321757 | biostudies-literature | 2017 Feb

REPOSITORIES: biostudies-literature

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Atomic layer confined vacancies for atomic-level insights into carbon dioxide electroreduction.

Gao Shan S   Sun Zhongti Z   Liu Wei W   Jiao Xingchen X   Zu Xiaolong X   Hu Qitao Q   Sun Yongfu Y   Yao Tao T   Zhang Wenhua W   Wei Shiqiang S   Xie Yi Y  

Nature communications 20170221


The role of oxygen vacancies in carbon dioxide electroreduction remains somewhat unclear. Here we construct a model of oxygen vacancies confined in atomic layer, taking the synthetic oxygen-deficient cobalt oxide single-unit-cell layers as an example. Density functional theory calculations demonstrate the main defect is the oxygen(II) vacancy, while X-ray absorption fine structure spectroscopy reveals their distinct oxygen vacancy concentrations. Proton transfer is theoretically/experimentally d  ...[more]

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