An electrochemically reversible lattice with redox active A-sites of double perovskite oxide nanosheets to reinforce oxygen electrocatalysis.

Chemical Science
Rahul MajeeSayan Bhattacharyya

Abstract

The catalyst surface undergoes reversible structural changes while influencing the rate of redox reactions, the atomistic structural details of which are often overlooked when the key focus is to enhance the catalytic activity and reaction yield. We achieve chemical synthesis of ∼5 unit cell thick double perovskite oxide nanosheets (NSs) and demonstrate their precise structural reversibility while catalyzing the successive oxygen evolution and reduction reactions (OER/ORR). 4.1 nm thick A-site ordered BaPrMn1.75Co0.25O5+δ (δ = 0.06-0.17) NSs with oxygen deficient PrO x terminated layers have flexible oxygen coordination of Pr3+ ions, which promotes the redox processes. When subjected to systematic oxidation and reduction cycles by cyclic voltammetry under small electrochemical bias, the PrO1.8 phase appears and disappears alternately at the NS surface, due to the intake and release of oxygen, respectively. The structural reversibility is attributed to the two-dimensional morphology and the A-site terminated surface with flexible anion stoichiometry. Although the underlying B-site cations are well-known active sites, this is the first demonstration of A(Pr3+)-site cations influencing the activity by reversibly altering their oxy...Continue Reading

References

Feb 28, 2017·Nature Communications·Bote ZhaoMeilin Liu
Nov 23, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Minoru Osada, Takayoshi Sasaki
Nov 24, 2017·Science Advances·Seung Sae HongHarold Y Hwang
Mar 20, 2018·Chemical Reviews·Huanyu JinShi-Zhang Qiao
May 28, 2019·Chemical Science·Kieren BradleyChris Vian
Jul 31, 2019·Chemical Science·Arghya BandyopadhyaySayan Bhattacharyya
Nov 30, 2019·Advanced Materials·Xiao TangGuoxiu Wang

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Citations

Sep 9, 2021·Chemical Communications : Chem Comm·Maoyu Wang, Zhenxing Feng

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Methods Mentioned

BETA
X-ray
electron microscopy
scanning electron microscopy
AFM
atomic force microscopy

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