High-throughput continuous flow synthesis of nickel nanoparticles for the catalytic hydrodeoxygenation of guaiacol
Abstract
The translation of batch chemistries to high-throughput continuous flow methods dresses scaling, automation, and reproducibility concerns associated with the implementation of colloidally prepared nanoparticle (NP) catalysts for industrial catalytic processes. Nickel NPs were synthesized by the high-temperature amine reduction of a Ni2+ precursor using a continuous millifluidic (mF) flow method, achieving yields greater than 60%. The resulting Ni NP catalysts were compared against catalysts prepared in a batch reaction under conditions analogous to the continuous flow conditions with respect to total reaction volume, time, and temperature and by traditional incipient wetness (IW) impregnation for the hydrodeoxygenation (HDO) of guaiacol under ex situ catalytic fast pyrolysis conditions. Compared to the IW method, the colloidally prepared NPs displayed increased morphological control and narrowed size distributions, and the NPs prepared by both methods showed similar size, shape, and crystallinity. The Ni NP catalyst synthesized by the continuous flow method exhibited similar H-adsorption site densities, site-time yields, and selectivities towards deoxygenated products as compared to the analogous batch reaction, and outperformed the IW catalyst with respect to higher selectivity to lower oxygen content products and a 6.9-fold slower deactivation rate. These results demonstrate the utility of synthesizing colloidal Ni NP catalysts using continuous flowmore »
- Authors:
-
[1];
- Univ. of Southern California, Los Angeles, CA (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office (BETO)
- OSTI Identifier:
- 1339239
- Report Number(s):
- NREL/JA-5100-66750
Journal ID: ISSN 2168-0485
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Sustainable Chemistry & Engineering
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; ex-situ catalytic fast pyrolysis; hydrodeoxygenation; lignin model compound; microreactor; millifluidics; nickel nanoparticles
Citation Formats
Roberts, Emily J., Habas, Susan E., Wang, Lu, Ruddy, Daniel A., White, Erick A., Baddour, Frederick G., Griffin, Michael B., Schaidle, Joshua A., Malmstadt, Noah, and Brutchey, Richard L. High-throughput continuous flow synthesis of nickel nanoparticles for the catalytic hydrodeoxygenation of guaiacol. United States: N. p., 2016.
Web. doi:10.1021/acssuschemeng.6b02009.
Roberts, Emily J., Habas, Susan E., Wang, Lu, Ruddy, Daniel A., White, Erick A., Baddour, Frederick G., Griffin, Michael B., Schaidle, Joshua A., Malmstadt, Noah, & Brutchey, Richard L. High-throughput continuous flow synthesis of nickel nanoparticles for the catalytic hydrodeoxygenation of guaiacol. United States. https://doi.org/10.1021/acssuschemeng.6b02009
Roberts, Emily J., Habas, Susan E., Wang, Lu, Ruddy, Daniel A., White, Erick A., Baddour, Frederick G., Griffin, Michael B., Schaidle, Joshua A., Malmstadt, Noah, and Brutchey, Richard L. Mon .
"High-throughput continuous flow synthesis of nickel nanoparticles for the catalytic hydrodeoxygenation of guaiacol". United States. https://doi.org/10.1021/acssuschemeng.6b02009. https://www.osti.gov/servlets/purl/1339239.
@article{osti_1339239,
title = {High-throughput continuous flow synthesis of nickel nanoparticles for the catalytic hydrodeoxygenation of guaiacol},
author = {Roberts, Emily J. and Habas, Susan E. and Wang, Lu and Ruddy, Daniel A. and White, Erick A. and Baddour, Frederick G. and Griffin, Michael B. and Schaidle, Joshua A. and Malmstadt, Noah and Brutchey, Richard L.},
abstractNote = {The translation of batch chemistries to high-throughput continuous flow methods dresses scaling, automation, and reproducibility concerns associated with the implementation of colloidally prepared nanoparticle (NP) catalysts for industrial catalytic processes. Nickel NPs were synthesized by the high-temperature amine reduction of a Ni2+ precursor using a continuous millifluidic (mF) flow method, achieving yields greater than 60%. The resulting Ni NP catalysts were compared against catalysts prepared in a batch reaction under conditions analogous to the continuous flow conditions with respect to total reaction volume, time, and temperature and by traditional incipient wetness (IW) impregnation for the hydrodeoxygenation (HDO) of guaiacol under ex situ catalytic fast pyrolysis conditions. Compared to the IW method, the colloidally prepared NPs displayed increased morphological control and narrowed size distributions, and the NPs prepared by both methods showed similar size, shape, and crystallinity. The Ni NP catalyst synthesized by the continuous flow method exhibited similar H-adsorption site densities, site-time yields, and selectivities towards deoxygenated products as compared to the analogous batch reaction, and outperformed the IW catalyst with respect to higher selectivity to lower oxygen content products and a 6.9-fold slower deactivation rate. These results demonstrate the utility of synthesizing colloidal Ni NP catalysts using continuous flow methods while maintaining the catalytic properties displayed by the batch equivalent. Finally, this methodology can be extended to other catalytically relevant base metals for the high-throughput synthesis of metal NPs for the catalytic production of biofuels.},
doi = {10.1021/acssuschemeng.6b02009},
journal = {ACS Sustainable Chemistry & Engineering},
number = 1,
volume = 5,
place = {United States},
year = {Mon Nov 07 00:00:00 EST 2016},
month = {Mon Nov 07 00:00:00 EST 2016}
}
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