Synergistic Control of Structural Disorder and Surface Bonding Nature to Optimize the Functionality of Manganese Oxide as an Electrocatalyst and a Cathode for Li–O2 Batteries

Xiaoyan Jin, Mihui Park, Seung Jae Shin, Yujin Jo, Min Gyu Kim, Hyungjun Kim, Yong Mook Kang, Seong Ju Hwang

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

An efficient way to improve the electrocatalyst and Li–O2 battery performances of metal oxide is developed by an exquisite synergistic control over structural disorder and surface bonding nature. The effects of amorphous nature and surface chemical environment on the functionalities of metal oxide are systematically investigated with well-crystalline and amorphous MnO2 nanocrystals with/without surface anchoring of highly oxidized iodate clusters. The amorphous MnO2 nanocrystal containing anchored iodate clusters shows much better performance as an oxygen evolution electrocatalyst and cathode catalyst for Li–O2 batteries than both iodate-free amorphous and well-crystalline homologues, underscoring the remarkable advantage of simultaneous enhancement of structural disorder and surface electron density. In situ X-ray absorption spectroscopic analysis demonstrates the promoted formation of double (MnO) bond, a critical step of oxygen evolution reaction, upon amorphization caused by the poor orbital overlap inside highly disordered crystallites. The beneficial effects of iodate anchoring and amorphization on electrocatalyst functionality are attributable to the alteration of surface bonding character, stabilization of Jahn–Teller active Mn3+ species, and enhanced charge transfer of interfaces. The present study underscores that fine-tuning of structural disorder and surface bonding nature provides an effective methodology to explore efficient metal oxide-based electrocatalysts.

Original languageEnglish
Article number1903265
JournalSmall
DOIs
Publication statusAccepted/In press - 2019 Jan 1

Fingerprint

Iodates
Manganese oxide
Electrocatalysts
Electrodes
Cathodes
Oxides
Metals
Nanoparticles
Amorphization
Oxygen
Nanocrystals
Crystalline materials
Spectroscopic analysis
X ray absorption
X-Rays
Electrons
Crystallites
Carrier concentration
manganese oxide
Charge transfer

All Science Journal Classification (ASJC) codes

  • Biotechnology
  • Biomaterials
  • Chemistry(all)
  • Materials Science(all)

Cite this

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title = "Synergistic Control of Structural Disorder and Surface Bonding Nature to Optimize the Functionality of Manganese Oxide as an Electrocatalyst and a Cathode for Li–O2 Batteries",
abstract = "An efficient way to improve the electrocatalyst and Li–O2 battery performances of metal oxide is developed by an exquisite synergistic control over structural disorder and surface bonding nature. The effects of amorphous nature and surface chemical environment on the functionalities of metal oxide are systematically investigated with well-crystalline and amorphous MnO2 nanocrystals with/without surface anchoring of highly oxidized iodate clusters. The amorphous MnO2 nanocrystal containing anchored iodate clusters shows much better performance as an oxygen evolution electrocatalyst and cathode catalyst for Li–O2 batteries than both iodate-free amorphous and well-crystalline homologues, underscoring the remarkable advantage of simultaneous enhancement of structural disorder and surface electron density. In situ X-ray absorption spectroscopic analysis demonstrates the promoted formation of double (MnO) bond, a critical step of oxygen evolution reaction, upon amorphization caused by the poor orbital overlap inside highly disordered crystallites. The beneficial effects of iodate anchoring and amorphization on electrocatalyst functionality are attributable to the alteration of surface bonding character, stabilization of Jahn–Teller active Mn3+ species, and enhanced charge transfer of interfaces. The present study underscores that fine-tuning of structural disorder and surface bonding nature provides an effective methodology to explore efficient metal oxide-based electrocatalysts.",
author = "Xiaoyan Jin and Mihui Park and Shin, {Seung Jae} and Yujin Jo and Kim, {Min Gyu} and Hyungjun Kim and Kang, {Yong Mook} and Hwang, {Seong Ju}",
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Synergistic Control of Structural Disorder and Surface Bonding Nature to Optimize the Functionality of Manganese Oxide as an Electrocatalyst and a Cathode for Li–O2 Batteries. / Jin, Xiaoyan; Park, Mihui; Shin, Seung Jae; Jo, Yujin; Kim, Min Gyu; Kim, Hyungjun; Kang, Yong Mook; Hwang, Seong Ju.

In: Small, 01.01.2019.

Research output: Contribution to journalArticle

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AU - Shin, Seung Jae

AU - Jo, Yujin

AU - Kim, Min Gyu

AU - Kim, Hyungjun

AU - Kang, Yong Mook

AU - Hwang, Seong Ju

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N2 - An efficient way to improve the electrocatalyst and Li–O2 battery performances of metal oxide is developed by an exquisite synergistic control over structural disorder and surface bonding nature. The effects of amorphous nature and surface chemical environment on the functionalities of metal oxide are systematically investigated with well-crystalline and amorphous MnO2 nanocrystals with/without surface anchoring of highly oxidized iodate clusters. The amorphous MnO2 nanocrystal containing anchored iodate clusters shows much better performance as an oxygen evolution electrocatalyst and cathode catalyst for Li–O2 batteries than both iodate-free amorphous and well-crystalline homologues, underscoring the remarkable advantage of simultaneous enhancement of structural disorder and surface electron density. In situ X-ray absorption spectroscopic analysis demonstrates the promoted formation of double (MnO) bond, a critical step of oxygen evolution reaction, upon amorphization caused by the poor orbital overlap inside highly disordered crystallites. The beneficial effects of iodate anchoring and amorphization on electrocatalyst functionality are attributable to the alteration of surface bonding character, stabilization of Jahn–Teller active Mn3+ species, and enhanced charge transfer of interfaces. The present study underscores that fine-tuning of structural disorder and surface bonding nature provides an effective methodology to explore efficient metal oxide-based electrocatalysts.

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