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

Shan Gao, Zhongti Sun, Wei Liu, Xingchen Jiao, Xiaolong Zu, Qitao Hu, Yongfu Sun (), Tao Yao, Wenhua Zhang (), Shiqiang Wei and Yi Xie ()
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Shan Gao: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Zhongti Sun: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Wei Liu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xingchen Jiao: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Xiaolong Zu: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Qitao Hu: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Yongfu Sun: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Tao Yao: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wenhua Zhang: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China
Shiqiang Wei: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yi Xie: Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: 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.

Date: 2017
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DOI: 10.1038/ncomms14503

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