In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate

Xiaoyan Jin, Taehun Lee, Wilson Tamakloe, Sharad B. Patil, Aloysius Soon, Yong Mook Kang, Seong Ju Hwang

Research output: Contribution to journalArticlepeer-review

Abstract

A defect engineering of inorganic solids garners great deal of research activities because of its high efficacy to optimize diverse energy-related functionalities of nanostructured materials. In this study, a novel in situ defect engineering route to maximize electrocatalytic redox activity of inorganic nanosheet is developed by using holey nanostructured substrate with strong interfacial electronic coupling. Density functional theory calculations and in situ spectroscopic analyses confirm that efficient interfacial charge transfer takes place between holey TiN and Ni−Fe-layered double hydroxide (LDH), leading to the feedback formation of nitrogen vacancies and a maximization of cation redox activity. The holey TiN−LDH nanohybrid is found to exhibit a superior functionality as an oxygen electrocatalyst and electrode for Li−O2 batteries compared to its non-holey homologues. The great impact of hybridization-driven vacancy introduction on the electrochemical performance originates from an efficient electrochemical activation of both Fe and Ni ions during electrocatalytic process, a reinforcement of interfacial electronic coupling, an increase in electrochemical active sites, and an improvement in electrocatalysis/charge-transfer kinetics.

Original languageEnglish
Article number2103368
JournalAdvanced Science
Volume9
Issue number1
DOIs
Publication statusPublished - 2022 Jan 5

Bibliographical note

Funding Information:
X.J., T.L., and W.T. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. NRF-2017R1A5A1015365, No. NRF-2020R1A2C3008671). This work was also supported by National R&D Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (No. 2021M3H4A1A03049662). The experiments at PAL were supported in part by MOST and POSTECH. S.B.P. was supported by RP-Grant 2019 of Ewha Womans University. T.L. and A.S. are partially supported by the 2019 Yonsei University Research Fund (2019-22-0099). Computational resources have been kindly provided by the KISTI Supercomputing Center (KSC-2020-CRE-0256).

Funding Information:
X.J., T.L., and W.T. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. NRF‐2017R1A5A1015365, No. NRF‐2020R1A2C3008671). This work was also supported by National R&D Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (No. 2021M3H4A1A03049662). The experiments at PAL were supported in part by MOST and POSTECH. S.B.P. was supported by RP‐Grant 2019 of Ewha Womans University. T.L. and A.S. are partially supported by the 2019 Yonsei University Research Fund (2019‐22‐0099). Computational resources have been kindly provided by the KISTI Supercomputing Center (KSC‐2020‐CRE‐0256).

Publisher Copyright:
© 2021 The Authors. Advanced Science published by Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

  • Medicine (miscellaneous)
  • Chemical Engineering(all)
  • Materials Science(all)
  • Biochemistry, Genetics and Molecular Biology (miscellaneous)
  • Engineering(all)
  • Physics and Astronomy(all)

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