4.8 Article

Defective Sn-Zn perovskites through bio-directed routes for modulating CO2RR

期刊

NANO ENERGY
卷 101, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.nanoen.2022.107593

关键词

Biomineralization; Perovskite tin-zinc oxides; Electrochemical CO2 reduction; In-situ X-ray absorption spectroscopy; Density-functional theory

资金

  1. Faculty of Engineering at UNSW
  2. DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
  3. Australian Government
  4. UNSW Digital Grid Futures Institute
  5. Materials Research Collaborative Access Team

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This study synthesized perovskite-type tin-zinc oxide catalysts using a biomineralization method and found that these catalysts have highly reactive active sites and tunable CO2RR selectivity. In-situ X-ray absorption spectroscopy measurements and density functional theory calculations revealed the impact of oxygen vacancies on the catalytic performance.
Sn and Zn oxides can catalyze electrochemical CO2 reduction reactions (CO2RR) to produce useful chemicals. Herein, we report on perovskite-type tin-zinc oxides (TZO) synthesized by a biomineralization approach under benign aqueous conditions. The resulting TZO catalysts are disordered and possess a high quantity of defects, which serve as highly reactive active sites in CO2RR. Selectively toward formate or CO is tunable toward the relative amounts of Sn and Zn and their associated O defects. In-situ X-ray absorption spectroscopy measurements reveal electronic and structural transformations consistent with oxygen vacancy formation at Sn-O-Zn bridges as a function of cathodic potential that strongly correlates to CO2RR selectivity. Density functional theory (DFT) calculations demonstrate that introducing an oxygen vacancy in TZO influences drastically influences formate/CO selectivity, consistent with our in-situ XAS findings and catalytic performance. Overall, these findings demonstrate the potential of biomineralization to fabricate perovskite-type metal oxides for energy conversion reactions.

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