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Title: 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:
ORCiD logo [1]; ORCiD logo [2];  [2];  [3]; ORCiD logo [2];  [4]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [6]
  1. Jiangnan Univ., Jiangsu (China); Univ. of Tennessee, Knoxville, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Jiangnan Univ., Jiangsu (China); Shanghai Jiao Tong Univ., Shanghai (China)
  4. Shanghai Jiao Tong Univ., Shanghai (China)
  5. Jiangnan Univ., Jiangsu (China)
  6. 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}
}

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