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Title: Scalable continuous flow synthesis of ZnO nanorod arrays in 3-D ceramic honeycomb substrates for low-temperature desulfurization

Scalable and cost-effective synthesis and assembly of technologically important nanostructures in three-dimensional (3D) substrates hold keys to bridge the demonstrated nanotechnologies in academia with industrially relevant scalable manufacturing. In this paper, using ZnO nanorod arrays as an example, a hydrothermal-based continuous flow synthesis (CFS) method is successfully used to integrate the nano-arrays in multi-channeled monolithic cordierite. Compared to the batch process, CFS enhances the average growth rate of nano-arrays by 125%, with the average length increasing from 2 μm to 4.5 μm within the same growth time of 4 hours. The precursor utilization efficiency of CFS is enhanced by 9 times compared to that of batch process by preserving the majority of precursors in recyclable solution. Computational fluid dynamic simulation suggests a steady-state solution flow and mass transport inside the channels of honeycomb substrates, giving rise to steady and consecutive growth of ZnO nano-arrays with an average length of 10 μm in 12 h. The monolithic ZnO nano-array-integrated cordierite obtained through CFS shows enhanced low-temperature (200 °C) desulfurization capacity and recyclability in comparison to ZnO powder wash-coated cordierite. This can be attributed to exposed ZnO {101¯0} planes, better dispersion and stronger interactions between sorbent and reactant in the ZnO nanorodmore » arrays, as well as the sintering-resistance of nano-array configurations during sulfidation–regeneration cycles. Finally, with the demonstrated scalable synthesis and desulfurization performance of ZnO nano-arrays, a promising, industrially relevant integration strategy is provided to fabricate metal oxide nano-array-based monolithic devices for various environmental and energy applications.« less
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1] ;  [2] ; ORCiD logo [3] ; ORCiD logo [1]
  1. Univ. of Connecticut, Storrs, CT (United States). Dept. of Materials Science and Engineering. Inst. of Materials Science
  2. Univ. of Connecticut, Storrs, CT (United States). Dept. of Mechanical Engineering
  3. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry
  4. Univ. of Connecticut, Storrs, CT (United States). Dept. of Mechanical Engineering; Tsinghua Univ., Beijing (China). Center for Combustion Energy
Publication Date:
Grant/Contract Number:
EE0006854; CBET-1344792
Type:
Accepted Manuscript
Journal Name:
CrystEngComm
Additional Journal Information:
Journal Volume: 19; Journal Issue: 34; Journal ID: ISSN 1466-8033
Publisher:
Royal Society of Chemistry
Research Org:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; continuous flow synthesis; ZnO nano-array; monolithic devices; scalable nanomanufacturing; desulfurization
OSTI Identifier:
1430254

Wang, Sibo, Wu, Yunchao, Miao, Ran, Zhang, Mingwan, Lu, Xingxu, Zhang, Bo, Kinstler, Alexander, Ren, Zhuyin, Guo, Yanbing, Lu, Tianfeng, Suib, Steven L., and Gao, Pu-Xian. Scalable continuous flow synthesis of ZnO nanorod arrays in 3-D ceramic honeycomb substrates for low-temperature desulfurization. United States: N. p., Web. doi:10.1039/c7ce00921f.
Wang, Sibo, Wu, Yunchao, Miao, Ran, Zhang, Mingwan, Lu, Xingxu, Zhang, Bo, Kinstler, Alexander, Ren, Zhuyin, Guo, Yanbing, Lu, Tianfeng, Suib, Steven L., & Gao, Pu-Xian. Scalable continuous flow synthesis of ZnO nanorod arrays in 3-D ceramic honeycomb substrates for low-temperature desulfurization. United States. doi:10.1039/c7ce00921f.
Wang, Sibo, Wu, Yunchao, Miao, Ran, Zhang, Mingwan, Lu, Xingxu, Zhang, Bo, Kinstler, Alexander, Ren, Zhuyin, Guo, Yanbing, Lu, Tianfeng, Suib, Steven L., and Gao, Pu-Xian. 2017. "Scalable continuous flow synthesis of ZnO nanorod arrays in 3-D ceramic honeycomb substrates for low-temperature desulfurization". United States. doi:10.1039/c7ce00921f. https://www.osti.gov/servlets/purl/1430254.
@article{osti_1430254,
title = {Scalable continuous flow synthesis of ZnO nanorod arrays in 3-D ceramic honeycomb substrates for low-temperature desulfurization},
author = {Wang, Sibo and Wu, Yunchao and Miao, Ran and Zhang, Mingwan and Lu, Xingxu and Zhang, Bo and Kinstler, Alexander and Ren, Zhuyin and Guo, Yanbing and Lu, Tianfeng and Suib, Steven L. and Gao, Pu-Xian},
abstractNote = {Scalable and cost-effective synthesis and assembly of technologically important nanostructures in three-dimensional (3D) substrates hold keys to bridge the demonstrated nanotechnologies in academia with industrially relevant scalable manufacturing. In this paper, using ZnO nanorod arrays as an example, a hydrothermal-based continuous flow synthesis (CFS) method is successfully used to integrate the nano-arrays in multi-channeled monolithic cordierite. Compared to the batch process, CFS enhances the average growth rate of nano-arrays by 125%, with the average length increasing from 2 μm to 4.5 μm within the same growth time of 4 hours. The precursor utilization efficiency of CFS is enhanced by 9 times compared to that of batch process by preserving the majority of precursors in recyclable solution. Computational fluid dynamic simulation suggests a steady-state solution flow and mass transport inside the channels of honeycomb substrates, giving rise to steady and consecutive growth of ZnO nano-arrays with an average length of 10 μm in 12 h. The monolithic ZnO nano-array-integrated cordierite obtained through CFS shows enhanced low-temperature (200 °C) desulfurization capacity and recyclability in comparison to ZnO powder wash-coated cordierite. This can be attributed to exposed ZnO {101¯0} planes, better dispersion and stronger interactions between sorbent and reactant in the ZnO nanorod arrays, as well as the sintering-resistance of nano-array configurations during sulfidation–regeneration cycles. Finally, with the demonstrated scalable synthesis and desulfurization performance of ZnO nano-arrays, a promising, industrially relevant integration strategy is provided to fabricate metal oxide nano-array-based monolithic devices for various environmental and energy applications.},
doi = {10.1039/c7ce00921f},
journal = {CrystEngComm},
number = 34,
volume = 19,
place = {United States},
year = {2017},
month = {7}
}

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