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

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 inorg...

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Autores principales: Jin, Xiaoyan, Lee, Taehun, Tamakloe, Wilson, Patil, Sharad B., Soon, Aloysius, Kang, Yong‐Mook, Hwang, Seong‐Ju
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8728845/
https://www.ncbi.nlm.nih.gov/pubmed/34713617
http://dx.doi.org/10.1002/advs.202103368
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author Jin, Xiaoyan
Lee, Taehun
Tamakloe, Wilson
Patil, Sharad B.
Soon, Aloysius
Kang, Yong‐Mook
Hwang, Seong‐Ju
author_facet Jin, Xiaoyan
Lee, Taehun
Tamakloe, Wilson
Patil, Sharad B.
Soon, Aloysius
Kang, Yong‐Mook
Hwang, Seong‐Ju
author_sort Jin, Xiaoyan
collection PubMed
description 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−O(2) 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.
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spelling pubmed-87288452022-01-11 In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate Jin, Xiaoyan Lee, Taehun Tamakloe, Wilson Patil, Sharad B. Soon, Aloysius Kang, Yong‐Mook Hwang, Seong‐Ju Adv Sci (Weinh) Research Articles 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−O(2) 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. John Wiley and Sons Inc. 2021-10-28 /pmc/articles/PMC8728845/ /pubmed/34713617 http://dx.doi.org/10.1002/advs.202103368 Text en © 2021 The Authors. Advanced Science published by Wiley‐VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Jin, Xiaoyan
Lee, Taehun
Tamakloe, Wilson
Patil, Sharad B.
Soon, Aloysius
Kang, Yong‐Mook
Hwang, Seong‐Ju
In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title_full In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title_fullStr In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title_full_unstemmed In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title_short In Situ Defect Engineering Route to Optimize the Cationic Redox Activity of Layered Double Hydroxide Nanosheet via Strong Electronic Coupling with Holey Substrate
title_sort in situ defect engineering route to optimize the cationic redox activity of layered double hydroxide nanosheet via strong electronic coupling with holey substrate
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8728845/
https://www.ncbi.nlm.nih.gov/pubmed/34713617
http://dx.doi.org/10.1002/advs.202103368
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