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Title: Morphology inherence from hollow MOFs to hollow carbon polyhedrons in preparing carbon-based electrocatalysts

Abstract

Hollow carbon nanostructures are emerging as advanced electrocatalysts for the oxygen reduction reaction (ORR) due to the effective usage of active sites and the reduced dependence on expensive noble metals. Conventional preparation of these hollow structures is achieved through templates (e.g. SiO 2, CdS, and Ni 3C), which serve to retain the void interiors during carbonization, leading to an essential template-removal procedure using hazardous chemical etchants. Herein, we demonstrate the direct carbonization of unique hollow zeolitic imidazolate frameworks (ZIFs) for the synthesis of hollow carbon polyhedrons (HCPs) with well-defined morphologies. The hollow ZIF particles behave bi-functionally as a carbon source and a morphology directing agent. This method evidences the strong morphology inherence from the hollow ZIFs during the carbonization, advancing the significant simplicity and environmental friendliness of this synthesis strategy. The as-prepared HCPs show a uniform polyhedral morphology and large void interiors, which enable their superior ORR activity. Iron can be doped into the HCPs (Fe/HCPs), providing the Fe/HCPs with enhanced ORR properties ( E 1/2 = 0.850 V) in comparison with those of HCPs. As a result, we highlight the efficient structural engineering to transform ZIFs into advanced carbon nanostructures accomplishing morphological control and high electrocatalytic activity.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  2. Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1355895
Report Number(s):
IS-J-9313
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:
AC02-07CH11358
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 13; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Pei, Yuchen, Qi, Zhiyuan, Li, Xinle, Maligal-Ganesh, Raghu V., Goh, Tian Wei, Xiao, Chaoxian, Wang, Tianyu, and Huang, Wenyu. Morphology inherence from hollow MOFs to hollow carbon polyhedrons in preparing carbon-based electrocatalysts. United States: N. p., 2017. Web. doi:10.1039/C6TA10609A.
Pei, Yuchen, Qi, Zhiyuan, Li, Xinle, Maligal-Ganesh, Raghu V., Goh, Tian Wei, Xiao, Chaoxian, Wang, Tianyu, & Huang, Wenyu. Morphology inherence from hollow MOFs to hollow carbon polyhedrons in preparing carbon-based electrocatalysts. United States. doi:10.1039/C6TA10609A.
Pei, Yuchen, Qi, Zhiyuan, Li, Xinle, Maligal-Ganesh, Raghu V., Goh, Tian Wei, Xiao, Chaoxian, Wang, Tianyu, and Huang, Wenyu. Tue . "Morphology inherence from hollow MOFs to hollow carbon polyhedrons in preparing carbon-based electrocatalysts". United States. doi:10.1039/C6TA10609A. https://www.osti.gov/servlets/purl/1355895.
@article{osti_1355895,
title = {Morphology inherence from hollow MOFs to hollow carbon polyhedrons in preparing carbon-based electrocatalysts},
author = {Pei, Yuchen and Qi, Zhiyuan and Li, Xinle and Maligal-Ganesh, Raghu V. and Goh, Tian Wei and Xiao, Chaoxian and Wang, Tianyu and Huang, Wenyu},
abstractNote = {Hollow carbon nanostructures are emerging as advanced electrocatalysts for the oxygen reduction reaction (ORR) due to the effective usage of active sites and the reduced dependence on expensive noble metals. Conventional preparation of these hollow structures is achieved through templates (e.g. SiO2, CdS, and Ni3C), which serve to retain the void interiors during carbonization, leading to an essential template-removal procedure using hazardous chemical etchants. Herein, we demonstrate the direct carbonization of unique hollow zeolitic imidazolate frameworks (ZIFs) for the synthesis of hollow carbon polyhedrons (HCPs) with well-defined morphologies. The hollow ZIF particles behave bi-functionally as a carbon source and a morphology directing agent. This method evidences the strong morphology inherence from the hollow ZIFs during the carbonization, advancing the significant simplicity and environmental friendliness of this synthesis strategy. The as-prepared HCPs show a uniform polyhedral morphology and large void interiors, which enable their superior ORR activity. Iron can be doped into the HCPs (Fe/HCPs), providing the Fe/HCPs with enhanced ORR properties (E1/2 = 0.850 V) in comparison with those of HCPs. As a result, we highlight the efficient structural engineering to transform ZIFs into advanced carbon nanostructures accomplishing morphological control and high electrocatalytic activity.},
doi = {10.1039/C6TA10609A},
journal = {Journal of Materials Chemistry. A},
number = 13,
volume = 5,
place = {United States},
year = {Tue Feb 21 00:00:00 EST 2017},
month = {Tue Feb 21 00:00:00 EST 2017}
}

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