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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 Lab., 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:
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 = {2017},
month = {2}
}

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Works referenced in this record:

MOF-Derived Hierarchically Porous Carbon with Exceptional Porosity and Hydrogen Storage Capacity
journal, December 2011

  • Yang, Seung Jae; Kim, Taehoon; Im, Ji Hyuk
  • Chemistry of Materials, Vol. 24, Issue 3
  • DOI: 10.1021/cm202554j

Carbonized Nanoscale Metal–Organic Frameworks as High Performance Electrocatalyst for Oxygen Reduction Reaction
journal, November 2014

  • Zhao, Shenlong; Yin, Huajie; Du, Lei
  • ACS Nano, Vol. 8, Issue 12
  • DOI: 10.1021/nn505582e

From Metal–Organic Framework to Nitrogen-Decorated Nanoporous Carbons: High CO 2 Uptake and Efficient Catalytic Oxygen Reduction
journal, May 2014

  • Aijaz, Arshad; Fujiwara, Naoko; Xu, Qiang
  • Journal of the American Chemical Society, Vol. 136, Issue 19
  • DOI: 10.1021/ja5003907

Dopamine as a Carbon Source: The Controlled Synthesis of Hollow Carbon Spheres and Yolk-Structured Carbon Nanocomposites
journal, June 2011

  • Liu, Rui; Mahurin, Shannon M.; Li, Chen
  • Angewandte Chemie International Edition, Vol. 50, Issue 30
  • DOI: 10.1002/anie.201102070

Beanpod-shaped Fe–C–N composite as promising ORR catalyst for fuel cells operated in neutral media
journal, January 2014

  • Yang, Zhi-Yu; Zhang, Yu-Xia; Jing, Lin
  • Journal of Materials Chemistry A, Vol. 2, Issue 8
  • DOI: 10.1039/c3ta13788k

N-doped mesoporous carbon spheres as the oxygen reduction reaction catalysts
journal, January 2014

  • Yang, Tianyu; Liu, Jian; Zhou, Ruifeng
  • J. Mater. Chem. A, Vol. 2, Issue 42
  • DOI: 10.1039/C4TA04301D

Composites of metal–organic frameworks and carbon-based materials: preparations, functionalities and applications
journal, January 2016

  • Liu, Xiao-Wei; Sun, Tian-Jun; Hu, Jiang-Liang
  • Journal of Materials Chemistry A, Vol. 4, Issue 10
  • DOI: 10.1039/C5TA09924B

Core-Shell Noble-Metal@Metal-Organic-Framework Nanoparticles with Highly Selective Sensing Property
journal, February 2013

  • He, Liangcan; Liu, Yong; Liu, Jingzhu
  • Angewandte Chemie International Edition, Vol. 52, Issue 13
  • DOI: 10.1002/anie.201209903

Porous nitrogen-doped hollow carbon spheres derived from polyaniline for high performance supercapacitors
journal, January 2014

  • Han, Jinpeng; Xu, Guiyin; Ding, Bing
  • J. Mater. Chem. A, Vol. 2, Issue 15
  • DOI: 10.1039/C3TA15271E

Ultrathin two-dimensional layered metal hydroxides: an emerging platform for advanced catalysis, energy conversion and storage
journal, January 2016

  • Yin, Huajie; Tang, Zhiyong
  • Chemical Society Reviews, Vol. 45, Issue 18
  • DOI: 10.1039/C6CS00343E

Development of MOF-Derived Carbon-Based Nanomaterials for Efficient Catalysis
journal, August 2016


Hollow Zn/Co ZIF Particles Derived from Core-Shell ZIF-67@ZIF-8 as Selective Catalyst for the Semi-Hydrogenation of Acetylene
journal, August 2015

  • Yang, Jian; Zhang, Fengjun; Lu, Haiyuan
  • Angewandte Chemie International Edition, Vol. 54, Issue 37
  • DOI: 10.1002/anie.201504242

A multiple coating route to hollow carbon spheres with foam-like shells and their applications in supercapacitor and confined catalysis
journal, January 2014

  • Fang, Xiaoliang; Zang, Jun; Wang, Xingli
  • Journal of Materials Chemistry A, Vol. 2, Issue 17
  • DOI: 10.1039/c3ta14881e

Metal–organic frameworks as potential drug carriers
journal, April 2010

  • Huxford, Rachel C.; Della Rocca, Joseph; Lin, Wenbin
  • Current Opinion in Chemical Biology, Vol. 14, Issue 2
  • DOI: 10.1016/j.cbpa.2009.12.012

Fe/Co/C–N nanocatalysts for oxygen reduction reaction synthesized by directly pyrolyzing Fe/Co-doped polyaniline
journal, September 2013


Porous Hollow Carbon@Sulfur Composites for High-Power Lithium-Sulfur Batteries
journal, May 2011

  • Jayaprakash, N.; Shen, J.; Moganty, Surya S.
  • Angewandte Chemie International Edition, Vol. 50, Issue 26, p. 5904-5908
  • DOI: 10.1002/anie.201100637

Optimized Synthesis of Fe/N/C Cathode Catalysts for PEM Fuel Cells: A Matter of Iron-Ligand Coordination Strength
journal, May 2013

  • Tian, Juan; Morozan, Adina; Sougrati, Moulay Tahar
  • Angewandte Chemie International Edition, Vol. 52, Issue 27
  • DOI: 10.1002/anie.201303025

Co@Co 3 O 4 Encapsulated in Carbon Nanotube-Grafted Nitrogen-Doped Carbon Polyhedra as an Advanced Bifunctional Oxygen Electrode
journal, February 2016

  • Aijaz, Arshad; Masa, Justus; Rösler, Christoph
  • Angewandte Chemie International Edition, Vol. 55, Issue 12
  • DOI: 10.1002/anie.201509382

Thermal Structural Transitions and Carbon Dioxide Adsorption Properties of Zeolitic Imidazolate Framework-7 (ZIF-7)
journal, May 2014

  • Cai, Wanxi; Lee, Taehee; Lee, Maro
  • Journal of the American Chemical Society, Vol. 136, Issue 22
  • DOI: 10.1021/ja5016298

Metal–organic frameworks and their derived nanostructures for electrochemical energy storage and conversion
journal, January 2015

  • Xia, Wei; Mahmood, Asif; Zou, Ruqiang
  • Energy & Environmental Science, Vol. 8, Issue 7
  • DOI: 10.1039/C5EE00762C

Hollow Spheres of Iron Carbide Nanoparticles Encased in Graphitic Layers as Oxygen Reduction Catalysts
journal, February 2014

  • Hu, Yang; Jensen, Jens Oluf; Zhang, Wei
  • Angewandte Chemie International Edition, Vol. 53, Issue 14
  • DOI: 10.1002/anie.201400358

From Bimetallic Metal-Organic Framework to Porous Carbon: High Surface Area and Multicomponent Active Dopants for Excellent Electrocatalysis
journal, July 2015

  • Chen, Yu-Zhen; Wang, Chengming; Wu, Zhen-Yu
  • Advanced Materials, Vol. 27, Issue 34
  • DOI: 10.1002/adma.201502315

Controlled synthesis of sustainable N-doped hollow core-mesoporous shell carbonaceous nanospheres from biomass
journal, September 2014


Uniform Hollow Carbon Shells: Nanostructured Graphitic Supports for Improved Oxygen-Reduction Catalysis
journal, August 2010

  • Schaefer, Zachary L.; Gross, Matthew L.; Hickner, Michael A.
  • Angewandte Chemie International Edition, Vol. 49, Issue 39
  • DOI: 10.1002/anie.201003213

Nanoengineering of Inorganic and Hybrid Hollow Spheres by Colloidal Templating
journal, November 1998


Insight into Structure-Dependent Self-Activation Mechanism in a Confined Nanospace of Core-Shell Nanocomposites
journal, December 2012


High Proton Conductivity by a Metal–Organic Framework Incorporating Zn 8 O Clusters with Aligned Imidazolium Groups Decorating the Channels
journal, November 2012

  • Sen, Susan; Nair, Nisanth N.; Yamada, Teppei
  • Journal of the American Chemical Society, Vol. 134, Issue 47
  • DOI: 10.1021/ja3076378

Evaluating metal–organic frameworks for natural gas storage
journal, January 2014

  • Mason, Jarad A.; Veenstra, Mike; Long, Jeffrey R.
  • Chemical Science, Vol. 5, Issue 1, p. 32-51
  • DOI: 10.1039/C3SC52633J

Nitrogen-Doped Carbon Nanocages as Efficient Metal-Free Electrocatalysts for Oxygen Reduction Reaction
journal, August 2012


Ultrathin metal–organic framework nanosheets for electrocatalytic oxygen evolution
journal, November 2016


Effect of Nitrogen Doping on Hydrogen Storage Capacity of Palladium Decorated Graphene
journal, May 2012

  • Parambhath, Vinayan Bhagavathi; Nagar, Rupali; Ramaprabhu, S.
  • Langmuir, Vol. 28, Issue 20
  • DOI: 10.1021/la301232r

Synthesis of Monodisperse Palladium Nanoclusters Using Metal-Organic Frameworks as Sacrificial Templates
journal, June 2016


Metal-Organic Framework as a Template for Porous Carbon Synthesis
journal, April 2008

  • Liu, Bo; Shioyama, Hiroshi; Akita, Tomoki
  • Journal of the American Chemical Society, Vol. 130, Issue 16
  • DOI: 10.1021/ja7106146

Selective nitrogen doping in graphene for oxygen reduction reactions
journal, January 2013

  • Yasuda, Satoshi; Yu, Li; Kim, Jeheon
  • Chemical Communications, Vol. 49, Issue 83
  • DOI: 10.1039/c3cc45641b

Hollow Co@C prepared from a Co-ZIF@microporous organic network: magnetic adsorbents for aromatic pollutants in water
journal, January 2015

  • Hong, Seokjo; Yoo, Jin; Park, Nojin
  • Chemical Communications, Vol. 51, Issue 100
  • DOI: 10.1039/C5CC06873H

From a metal–organic framework to hierarchical high surface-area hollow octahedral carbon cages
journal, January 2015

  • Aijaz, Arshad; Sun, Jian-Ke; Pachfule, Pradip
  • Chemical Communications, Vol. 51, Issue 73
  • DOI: 10.1039/C5CC04230E

Hierarchical hollow ZnO cubes constructed using self-sacrificial ZIF-8 frameworks and their enhanced benzene gas-sensing properties
journal, January 2015

  • Li, Wenhui; Wu, Xiaofeng; Liu, Haidi
  • New Journal of Chemistry, Vol. 39, Issue 9
  • DOI: 10.1039/C5NJ00549C

Molecular-based design and emerging applications of nanoporous carbon spheres
journal, July 2015

  • Liu, Jian; Wickramaratne, Nilantha P.; Qiao, Shi Zhang
  • Nature Materials, Vol. 14, Issue 8
  • DOI: 10.1038/nmat4317

Anion-Exchange Membrane Fuel Cells: Dual-Site Mechanism of Oxygen Reduction Reaction in Alkaline Media on Cobalt−Polypyrrole Electrocatalysts
journal, March 2010

  • Olson, Tim S.; Pylypenko, Svitlana; Atanassov, Plamen
  • The Journal of Physical Chemistry C, Vol. 114, Issue 11
  • DOI: 10.1021/jp910572g

Exceptional CO 2 capture in a hierarchically porous carbon with simultaneous high surface area and pore volume
journal, January 2014

  • Srinivas, Gadipelli; Krungleviciute, Vaiva; Guo, Zheng-Xiao
  • Energy Environ. Sci., Vol. 7, Issue 1
  • DOI: 10.1039/C3EE42918K

Well-defined carbon polyhedrons prepared from nano metal–organic frameworks for oxygen reduction
journal, January 2014

  • Xia, Wei; Zhu, Jinghan; Guo, Wenhan
  • J. Mater. Chem. A, Vol. 2, Issue 30
  • DOI: 10.1039/C4TA01656D

Metal–Organic Framework Materials as Chemical Sensors
journal, September 2011

  • Kreno, Lauren E.; Leong, Kirsty; Farha, Omar K.
  • Chemical Reviews, Vol. 112, Issue 2, p. 1105-1125
  • DOI: 10.1021/cr200324t

Thermal Conversion of Core–Shell Metal–Organic Frameworks: A New Method for Selectively Functionalized Nanoporous Hybrid Carbon
journal, January 2015

  • Tang, Jing; Salunkhe, Rahul R.; Liu, Jian
  • Journal of the American Chemical Society, Vol. 137, Issue 4
  • DOI: 10.1021/ja511539a

Nitrogen, Phosphorus, and Sulfur Co-Doped Hollow Carbon Shell as Superior Metal-Free Catalyst for Selective Oxidation of Aromatic Alkanes
journal, February 2016

  • Yang, Shuliang; Peng, Li; Huang, Peipei
  • Angewandte Chemie International Edition, Vol. 55, Issue 12
  • DOI: 10.1002/anie.201600455

Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells
journal, August 2011

  • Proietti, Eric; Jaouen, Frédéric; Lefèvre, Michel
  • Nature Communications, Vol. 2, Issue 1
  • DOI: 10.1038/ncomms1427

Tandem Catalysis by Palladium Nanoclusters Encapsulated in Metal–Organic Frameworks
journal, September 2014

  • Li, Xinle; Guo, Zhiyong; Xiao, Chaoxian
  • ACS Catalysis, Vol. 4, Issue 10
  • DOI: 10.1021/cs5006635

Tin-Nanoparticles Encapsulated in Elastic Hollow Carbon Spheres for High-Performance Anode Material in Lithium-Ion Batteries
journal, March 2008


Efficient Oxygen Electroreduction: Hierarchical Porous Fe–N-doped Hollow Carbon Nanoshells
journal, May 2015


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