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Title: A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts

Abstract

Herein, we first put forward a smart strategy to in situ fabricate Ru nanoparticle (NP) inserted porous carbon nanofibers by one-pot conversion of Ru-functionalized metal organic framework fibers. Such fiber precursors are skillfully constructed by cooperative assembly of different proportional RuCl3 and Zn(Ac)2·2H2O along with trimesic acid (H3BTC) in the presence of N,N-dimethylformamide. The following high-temperature pyrolysis affords uniform and evenly dispersed Ru NPs (ca. 12-16 nm), which are firmly inserted into the hierarchically porous carbon nanofibers formed simultaneously. The resulting Ru-carbon nanofiber (Ru-CNF) catalysts prove to be active towards the liquid-phase hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL), a biomass-derived platform molecule with wide applications in the preparation of renewable chemicals and liquid transportation fuels. The optimal GVL yield of 96.0% is obtained, corresponding to a high activity of 9.23 molLAh–1gRu–1, 17 times of that using the commercial Ru/C catalyst. Moreover, the Ru-CNF catalyst is extremely stable, and can be cycled up to 7 times without significant loss of reactivity. Our strategy demonstrated here reveals new possibilities to make proficient metal catalysts, and provides a general way to fabricate metal-carbon nanofiber composites available for other applications.

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1389797
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Green Chemistry
Additional Journal Information:
Journal Volume: 18; Journal Issue: 12; Journal ID: ISSN 1463-9262
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Yang, Ying, Sun, Cheng-Jun, Brown, Dennis E., Zhang, Liqiang, Yang, Feng, Zhao, Hairui, Wang, Yue, Ma, Xiaohui, Zhang, Xin, and Ren, Yang. A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts. United States: N. p., 2016. Web. doi:10.1039/c5gc02802g.
Yang, Ying, Sun, Cheng-Jun, Brown, Dennis E., Zhang, Liqiang, Yang, Feng, Zhao, Hairui, Wang, Yue, Ma, Xiaohui, Zhang, Xin, & Ren, Yang. A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts. United States. doi:10.1039/c5gc02802g.
Yang, Ying, Sun, Cheng-Jun, Brown, Dennis E., Zhang, Liqiang, Yang, Feng, Zhao, Hairui, Wang, Yue, Ma, Xiaohui, Zhang, Xin, and Ren, Yang. Fri . "A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts". United States. doi:10.1039/c5gc02802g.
@article{osti_1389797,
title = {A smart strategy to fabricate Ru nanoparticle inserted porous carbon nanofibers as highly efficient levulinic acid hydrogenation catalysts},
author = {Yang, Ying and Sun, Cheng-Jun and Brown, Dennis E. and Zhang, Liqiang and Yang, Feng and Zhao, Hairui and Wang, Yue and Ma, Xiaohui and Zhang, Xin and Ren, Yang},
abstractNote = {Herein, we first put forward a smart strategy to in situ fabricate Ru nanoparticle (NP) inserted porous carbon nanofibers by one-pot conversion of Ru-functionalized metal organic framework fibers. Such fiber precursors are skillfully constructed by cooperative assembly of different proportional RuCl3 and Zn(Ac)2·2H2O along with trimesic acid (H3BTC) in the presence of N,N-dimethylformamide. The following high-temperature pyrolysis affords uniform and evenly dispersed Ru NPs (ca. 12-16 nm), which are firmly inserted into the hierarchically porous carbon nanofibers formed simultaneously. The resulting Ru-carbon nanofiber (Ru-CNF) catalysts prove to be active towards the liquid-phase hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL), a biomass-derived platform molecule with wide applications in the preparation of renewable chemicals and liquid transportation fuels. The optimal GVL yield of 96.0% is obtained, corresponding to a high activity of 9.23 molLAh–1gRu–1, 17 times of that using the commercial Ru/C catalyst. Moreover, the Ru-CNF catalyst is extremely stable, and can be cycled up to 7 times without significant loss of reactivity. Our strategy demonstrated here reveals new possibilities to make proficient metal catalysts, and provides a general way to fabricate metal-carbon nanofiber composites available for other applications.},
doi = {10.1039/c5gc02802g},
journal = {Green Chemistry},
issn = {1463-9262},
number = 12,
volume = 18,
place = {United States},
year = {2016},
month = {1}
}

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