Overcoming the phase separation within high-entropy metal carbide by poly(ionic liquid)s
Abstract
High-entropy crystalline materials are attracting more attention. In principle, high-entropy metal carbides (HMCs) that contain five or more metal ions, possess more negative free energy value during catalysis. But its preparation is challenging because of the immiscibility of multi metal cations in a single carbide solid solution. Here, a rational strategy for preparing HMC is proposed via a coordination-assisted crystallization process in the presence of Br-based poly(ionic liquids). Through this method, Mo0.2W0.2V0.2Cr0.2Nb0.2C nanoparticles, with a single cubic phase structure, incorporated on porous carbon, are obtained (HMC@NC). By combination of well dispersed small particle size (~4 nm), high surface area (~270 m2 g–1), and high-entropy phase, HMC@NC can function as a promising catalyst for the dehydrogenation of ethylbenzene. Here, unexpected activity (EB conv.: 73%) and thermal stability (>100 h on steam) at 450 °C are observed. Such a facile synthetic strategy may inspire the fabrication of other types of HMCs for more specific tasks.
- Authors:
-
- Jiangnan Univ., Jiangsu (China); Univ. of Tennessee, Knoxville, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States)
- Jiangnan Univ., Jiangsu (China); Shanghai Jiao Tong Univ., Shanghai (China)
- Shanghai Jiao Tong Univ., Shanghai (China)
- Jiangnan Univ., Jiangsu (China)
- Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1808159
- Alternate Identifier(s):
- OSTI ID: 1771225
- Grant/Contract Number:
- AC05-00OR22725; 21776174
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemComm
- Additional Journal Information:
- Journal Volume: 57; Journal Issue: 30; Journal ID: ISSN 1359-7345
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; high entropy; metal carbides; porous carbon; poly(ionic liquids); mesoporous carbon
Citation Formats
Leng, Yan, Zhang, Zihao, Chen, Hao, Du, Shengyu, Liu, Jixing, Nie, Shiyang, Dong, Yuming, Zhang, Pengfei, and Dai, Sheng. Overcoming the phase separation within high-entropy metal carbide by poly(ionic liquid)s. United States: N. p., 2021.
Web. doi:10.1039/d1cc00497b.
Leng, Yan, Zhang, Zihao, Chen, Hao, Du, Shengyu, Liu, Jixing, Nie, Shiyang, Dong, Yuming, Zhang, Pengfei, & Dai, Sheng. Overcoming the phase separation within high-entropy metal carbide by poly(ionic liquid)s. United States. https://doi.org/10.1039/d1cc00497b
Leng, Yan, Zhang, Zihao, Chen, Hao, Du, Shengyu, Liu, Jixing, Nie, Shiyang, Dong, Yuming, Zhang, Pengfei, and Dai, Sheng. Fri .
"Overcoming the phase separation within high-entropy metal carbide by poly(ionic liquid)s". United States. https://doi.org/10.1039/d1cc00497b. https://www.osti.gov/servlets/purl/1808159.
@article{osti_1808159,
title = {Overcoming the phase separation within high-entropy metal carbide by poly(ionic liquid)s},
author = {Leng, Yan and Zhang, Zihao and Chen, Hao and Du, Shengyu and Liu, Jixing and Nie, Shiyang and Dong, Yuming and Zhang, Pengfei and Dai, Sheng},
abstractNote = {High-entropy crystalline materials are attracting more attention. In principle, high-entropy metal carbides (HMCs) that contain five or more metal ions, possess more negative free energy value during catalysis. But its preparation is challenging because of the immiscibility of multi metal cations in a single carbide solid solution. Here, a rational strategy for preparing HMC is proposed via a coordination-assisted crystallization process in the presence of Br-based poly(ionic liquids). Through this method, Mo0.2W0.2V0.2Cr0.2Nb0.2C nanoparticles, with a single cubic phase structure, incorporated on porous carbon, are obtained (HMC@NC). By combination of well dispersed small particle size (~4 nm), high surface area (~270 m2 g–1), and high-entropy phase, HMC@NC can function as a promising catalyst for the dehydrogenation of ethylbenzene. Here, unexpected activity (EB conv.: 73%) and thermal stability (>100 h on steam) at 450 °C are observed. Such a facile synthetic strategy may inspire the fabrication of other types of HMCs for more specific tasks.},
doi = {10.1039/d1cc00497b},
journal = {ChemComm},
number = 30,
volume = 57,
place = {United States},
year = {Fri Mar 05 00:00:00 EST 2021},
month = {Fri Mar 05 00:00:00 EST 2021}
}
Works referenced in this record:
Mechanochemical-Assisted Synthesis of High-Entropy Metal Nitride via a Soft Urea Strategy
journal, April 2018
- Jin, Tian; Sang, Xiahan; Unocic, Raymond R.
- Advanced Materials, Vol. 30, Issue 23
Catalytic behavior of manganese oxides for oxidative dehydrogenation of ethylbenzene with carbon dioxide
journal, December 2017
- Ren, Kai; Song, Jian; Song, Yong-Hong
- Journal of CO2 Utilization, Vol. 22
Robust Fe 3 Mo 3 C Supported IrMn Clusters as Highly Efficient Bifunctional Air Electrode for Metal-Air Battery
journal, August 2017
- Cui, Zhiming; Li, Yutao; Fu, Gengtao
- Advanced Materials, Vol. 29, Issue 40
Insights into the Oxidative Dehydrogenation of Ethylbenzene with CO 2 Catalyzed by the Ordered Mesoporous V 2 O 5 –Ce 0.5 Zr 0.5 O 2 –Al 2 O 3
journal, November 2019
- Wang, Huan; Zhu, Wei; Yang, Guo-Qing
- Industrial & Engineering Chemistry Research, Vol. 58, Issue 47
Design of house centipede-like MoC–Mo2C nanorods grafted with N-doped carbon nanotubes as bifunctional catalysts for high-performance Li–O2 batteries
journal, March 2020
- Oh, Yeon Jong; Kim, Jung Hyun; Lee, Jun Yeob
- Chemical Engineering Journal, Vol. 384
Carbon dioxide utilization as a soft oxidant and promoter in catalysis
journal, January 2012
- Ansari, Mohd Bismillah; Park, Sang-Eon
- Energy & Environmental Science, Vol. 5, Issue 11
Carbothermal shock synthesis of high-entropy-alloy nanoparticles
journal, March 2018
- Yao, Yonggang; Huang, Zhennan; Xie, Pengfei
- Science, Vol. 359, Issue 6383
Ionic liquids and their solid-state analogues as materials for energy generation and storage
journal, January 2016
- MacFarlane, Douglas R.; Forsyth, Maria; Howlett, Patrick C.
- Nature Reviews Materials, Vol. 1, Issue 2
Sustainable carbon materials
journal, January 2015
- Titirici, Maria-Magdalena; White, Robin J.; Brun, Nicolas
- Chemical Society Reviews, Vol. 44, Issue 1, p. 250-290
Ionic Liquids—New “Solutions” for Transition Metal Catalysis
journal, November 2000
- Wasserscheid, Peter; Keim, Wilhelm
- Angewandte Chemie, Vol. 39, Issue 21
Prussian Blue Iron–Cobalt Mesocrystals as a Template for the Growth of Fe/Co Carbide (Cementite) and Fe/Co Nanocrystals
journal, September 2019
- Hardy, David A.; Nguyen, Edward T.; Parrish, Sara E.
- Chemistry of Materials, Vol. 31, Issue 19
Highly Dispersed Copper over β-Mo 2 C as an Efficient and Stable Catalyst for the Reverse Water Gas Shift (RWGS) Reaction
journal, December 2016
- Zhang, Xiao; Zhu, Xiaobing; Lin, Lili
- ACS Catalysis, Vol. 7, Issue 1
Frontiers in poly(ionic liquid)s: syntheses and applications
journal, January 2017
- Qian, Wenjing; Texter, John; Yan, Feng
- Chemical Society Reviews, Vol. 46, Issue 4
Understanding the active-site nature of vanadia-based catalysts for oxidative dehydrogenation of ethylbenzene with CO2 via atomic layer deposited VOx on γ-Al2O3
journal, December 2019
- Yang, Guo-Qing; Wang, Huan; Gong, Ting
- Journal of Catalysis, Vol. 380
High-entropy high-hardness metal carbides discovered by entropy descriptors
journal, November 2018
- Sarker, Pranab; Harrington, Tyler; Toher, Cormac
- Nature Communications, Vol. 9, Issue 1
Room temperature lithium superionic conductivity in high entropy oxides
journal, January 2016
- Bérardan, D.; Franger, S.; Meena, A. K.
- Journal of Materials Chemistry A, Vol. 4, Issue 24
Role Of CO 2 As a Soft Oxidant For Dehydrogenation of Ethylbenzene to Styrene over a High-Surface-Area Ceria Catalyst
journal, October 2015
- Zhang, Li; Wu, Zili; Nelson, Nicholas C.
- ACS Catalysis, Vol. 5, Issue 11
Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts
journal, May 2016
- Hunt, S. T.; Milina, M.; Alba-Rubio, A. C.
- Science, Vol. 352, Issue 6288
Single-Phase Mixed Transition Metal Carbonate Encapsulated by Graphene: Facile Synthesis and Improved Lithium Storage Properties
journal, January 2018
- Zhang, Rui; Huang, Xiaoxiao; Wang, Dong
- Advanced Functional Materials, Vol. 28, Issue 10
Mixtures of ionic liquids
journal, January 2012
- Niedermeyer, Heiko; Hallett, Jason P.; Villar-Garcia, Ignacio J.
- Chemical Society Reviews, Vol. 41, Issue 23
High-Entropy Perovskite Fluorides: A New Platform for Oxygen Evolution Catalysis
journal, February 2020
- Wang, Tao; Chen, Hao; Yang, Zhenzhen
- Journal of the American Chemical Society, Vol. 142, Issue 10
Ionic Liquids for the Convenient Synthesis of Functional Nanoparticles and Other Inorganic Nanostructures
journal, September 2004
- Antonietti, Markus; Kuang, Daibin; Smarsly, Bernd
- Angewandte Chemie International Edition, Vol. 43, Issue 38, p. 4988-4992
Metal-organic frameworks and their derived materials for electrochemical energy storage and conversion: Promises and challenges
journal, December 2017
- Wu, Hao Bin; Lou, Xiong Wen (David)
- Science Advances, Vol. 3, Issue 12
Synthesis of Ti3AuC2, Ti3Au2C2 and Ti3IrC2 by noble metal substitution reaction in Ti3SiC2 for high-temperature-stable Ohmic contacts to SiC
journal, May 2017
- Fashandi, Hossein; Dahlqvist, Martin; Lu, Jun
- Nature Materials, Vol. 16, Issue 8
High entropy oxides for reversible energy storage
journal, August 2018
- Sarkar, Abhishek; Velasco, Leonardo; Wang, Di
- Nature Communications, Vol. 9, Issue 1
Influence of chemical disorder on energy dissipation and defect evolution in concentrated solid solution alloys
journal, October 2015
- Zhang, Yanwen; Stocks, G. Malcolm; Jin, Ke
- Nature Communications, Vol. 6, Issue 1
Mechanochemical Synthesis of High Entropy Oxide Materials under Ambient Conditions: Dispersion of Catalysts via Entropy Maximization
journal, May 2019
- Chen, Hao; Lin, Wenwen; Zhang, Zihao
- ACS Materials Letters, Vol. 1, Issue 1
Characterization of Imidazolium Chloride Ionic Liquids Plus Trivalent Chromium Chloride for Chromium Electroplating
journal, April 2015
- Sun, Liyuan; Brennecke, Joan F.
- Industrial & Engineering Chemistry Research, Vol. 54, Issue 17
Application of Ionic Liquids to Energy Storage and Conversion Materials and Devices
journal, January 2017
- Watanabe, Masayoshi; Thomas, Morgan L.; Zhang, Shiguo
- Chemical Reviews, Vol. 117, Issue 10
High-Entropy Metal Diborides: A New Class of High-Entropy Materials and a New Type of Ultrahigh Temperature Ceramics
journal, November 2016
- Gild, Joshua; Zhang, Yuanyao; Harrington, Tyler
- Scientific Reports, Vol. 6, Issue 1
Fe‐Doped Ni 3 C Nanodots in N‐Doped Carbon Nanosheets for Efficient Hydrogen‐Evolution and Oxygen‐Evolution Electrocatalysis
journal, September 2017
- Fan, Haosen; Yu, Hong; Zhang, Yufei
- Angewandte Chemie, Vol. 129, Issue 41
Poly(ionic liquid)s: Polymers expanding classical property profiles
journal, March 2011
- Yuan, Jiayin; Antonietti, Markus
- Polymer, Vol. 52, Issue 7
Metal-Containing Poly(ionic liquid) Membranes for Antibacterial Applications
journal, April 2017
- Zheng, Zhiqiang; Guo, Jiangna; Mao, Hailei
- ACS Biomaterials Science & Engineering, Vol. 3, Issue 6
Poly(ionic liquid)s: An update
journal, July 2013
- Yuan, Jiayin; Mecerreyes, David; Antonietti, Markus
- Progress in Polymer Science, Vol. 38, Issue 7
High‐Entropy Oxides: Fundamental Aspects and Electrochemical Properties
journal, March 2019
- Sarkar, Abhishek; Wang, Qingsong; Schiele, Alexander
- Advanced Materials, Vol. 31, Issue 26