Cargando…

Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation

[Image: see text] The development of efficient water-oxidizing electrocatalysts is a key issue for achieving high performance in the overall water electrolysis technique. However, the complexity of multiple electron transfer processes and large activation energies have been regarded as major bottlen...

Descripción completa

Detalles Bibliográficos
Autores principales: Seo, Hongmin, Park, Sunghak, Cho, Kang Hee, Choi, Seungwoo, Ko, Changwan, Randriamahazaka, Hyacinthe, Nam, Ki Tae
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8296608/
https://www.ncbi.nlm.nih.gov/pubmed/34308071
http://dx.doi.org/10.1021/acsomega.1c02397
_version_ 1783725677369884672
author Seo, Hongmin
Park, Sunghak
Cho, Kang Hee
Choi, Seungwoo
Ko, Changwan
Randriamahazaka, Hyacinthe
Nam, Ki Tae
author_facet Seo, Hongmin
Park, Sunghak
Cho, Kang Hee
Choi, Seungwoo
Ko, Changwan
Randriamahazaka, Hyacinthe
Nam, Ki Tae
author_sort Seo, Hongmin
collection PubMed
description [Image: see text] The development of efficient water-oxidizing electrocatalysts is a key issue for achieving high performance in the overall water electrolysis technique. However, the complexity of multiple electron transfer processes and large activation energies have been regarded as major bottlenecks for efficient water electrolysis. Thus, complete electrochemical processes, including electron transport, charge accumulation, and chemical bond formation/dissociation, need to be analyzed for establishing a design rule for film-type electrocatalysts. In light of this, complex capacitance analysis is an effective tool for investigating the charge accumulation and dissipation processes of film-type electrocatalysts. Here, we conduct complex capacitance analysis for the Mn(3)O(4) nanocatalyst, which exhibits superb catalytic activity for water oxidation under neutral conditions. Charge was accumulated on the catalyst surface by the change in Mn valence between Mn(II) and Mn(IV) prior to the rate-determining O–O bond forming step. Furthermore, we newly propose the dissipation ratio (D) for understanding the energy balance between charge accumulation and charge consumption for chemical O–O bond formation. From this analysis, we reveal the potential- and thickness-dependent contribution of the charge accumulation process on the overall catalytic efficiency. We think that an understanding of complex capacitance analysis could be an effective methodology for investigating the charge accumulation process on the surface of general film-type electrocatalysts.
format Online
Article
Text
id pubmed-8296608
institution National Center for Biotechnology Information
language English
publishDate 2021
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-82966082021-07-23 Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation Seo, Hongmin Park, Sunghak Cho, Kang Hee Choi, Seungwoo Ko, Changwan Randriamahazaka, Hyacinthe Nam, Ki Tae ACS Omega [Image: see text] The development of efficient water-oxidizing electrocatalysts is a key issue for achieving high performance in the overall water electrolysis technique. However, the complexity of multiple electron transfer processes and large activation energies have been regarded as major bottlenecks for efficient water electrolysis. Thus, complete electrochemical processes, including electron transport, charge accumulation, and chemical bond formation/dissociation, need to be analyzed for establishing a design rule for film-type electrocatalysts. In light of this, complex capacitance analysis is an effective tool for investigating the charge accumulation and dissipation processes of film-type electrocatalysts. Here, we conduct complex capacitance analysis for the Mn(3)O(4) nanocatalyst, which exhibits superb catalytic activity for water oxidation under neutral conditions. Charge was accumulated on the catalyst surface by the change in Mn valence between Mn(II) and Mn(IV) prior to the rate-determining O–O bond forming step. Furthermore, we newly propose the dissipation ratio (D) for understanding the energy balance between charge accumulation and charge consumption for chemical O–O bond formation. From this analysis, we reveal the potential- and thickness-dependent contribution of the charge accumulation process on the overall catalytic efficiency. We think that an understanding of complex capacitance analysis could be an effective methodology for investigating the charge accumulation process on the surface of general film-type electrocatalysts. American Chemical Society 2021-07-06 /pmc/articles/PMC8296608/ /pubmed/34308071 http://dx.doi.org/10.1021/acsomega.1c02397 Text en © 2021 The Authors. Published by American Chemical Society Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Seo, Hongmin
Park, Sunghak
Cho, Kang Hee
Choi, Seungwoo
Ko, Changwan
Randriamahazaka, Hyacinthe
Nam, Ki Tae
Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title_full Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title_fullStr Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title_full_unstemmed Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title_short Complex Impedance Analysis on Charge Accumulation Step of Mn(3)O(4) Nanoparticles during Water Oxidation
title_sort complex impedance analysis on charge accumulation step of mn(3)o(4) nanoparticles during water oxidation
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8296608/
https://www.ncbi.nlm.nih.gov/pubmed/34308071
http://dx.doi.org/10.1021/acsomega.1c02397
work_keys_str_mv AT seohongmin compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT parksunghak compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT chokanghee compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT choiseungwoo compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT kochangwan compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT randriamahazakahyacinthe compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation
AT namkitae compleximpedanceanalysisonchargeaccumulationstepofmn3o4nanoparticlesduringwateroxidation