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Title: One-pot process for hydrodeoxygenation of lignin to alkanes using Ru-based bimetallic and bifunctional catalysts supported on zeolite Y

Abstract

Here, the synthesis of high-efficiency and low-cost catalysts for hydrodeoxygenation (HDO) of waste lignin to advanced biofuels is crucial for enhancing current biorefinery processes. Inexpensive transition metals, including Fe, Ni, Cu, and Zn, were severally co-loaded with Ru on HY zeolite to form bimetallic and bifunctional catalysts. These catalysts were subsequently tested for HDO conversion of softwood lignin and several lignin model compounds. Results indicated that the inexpensive earth-abundant metals could modulate the hydrogenolysis activity of Ru and decrease the yield of low-molecular-weight gaseous products. Among these catalysts, Ru-Cu/HY showed the best HDO performance, affording the highest selectivity to hydrocarbon products. The improved catalytic performance of Ru-Cu/HY was probably a result of the following three factors: (1) high total and strong acid sites, (2) good dispersion of metal species and limited segregation, and (3) high adsorption capacity for polar fractions, including hydroxyl groups and ether bonds. Moreover, all bifunctional catalysts proved to be superior over the combination catalysts of Ru/Al 2O 3 and HY zeolite.

Authors:
 [1];  [1];  [2];  [1];  [3];  [4];  [4];  [4];  [5];  [5];  [5]; ORCiD logo [1]
  1. Washington State Univ., Richland, WA (United States)
  2. Southwest Research Institute, San Antonio, TX (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Environmental Molecular Sciences Lab., Richland, WA (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1353424
Alternate Identifier(s):
OSTI ID: 1400822
Report Number(s):
NREL/JA-5100-68188
Journal ID: ISSN 1864-5631
Grant/Contract Number:
AC36-08GO28308; AC36-08G028308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 8; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bifunctional catalysts; bimetallic catalysts; biofuel; hydrodeoxygenation; lignin

Citation Formats

Wang, Hongliang, Ruan, Hao, Feng, Maoqi, Qin, Yuling, Job, Heather, Luo, Langli, Wang, Chongmin, Engelhard, Mark H., Kuhn, Erik, Chen, Xiaowen, Tucker, Melvin P., and Yang, Bin. One-pot process for hydrodeoxygenation of lignin to alkanes using Ru-based bimetallic and bifunctional catalysts supported on zeolite Y. United States: N. p., 2017. Web. doi:10.1002/cssc.201700160.
Wang, Hongliang, Ruan, Hao, Feng, Maoqi, Qin, Yuling, Job, Heather, Luo, Langli, Wang, Chongmin, Engelhard, Mark H., Kuhn, Erik, Chen, Xiaowen, Tucker, Melvin P., & Yang, Bin. One-pot process for hydrodeoxygenation of lignin to alkanes using Ru-based bimetallic and bifunctional catalysts supported on zeolite Y. United States. doi:10.1002/cssc.201700160.
Wang, Hongliang, Ruan, Hao, Feng, Maoqi, Qin, Yuling, Job, Heather, Luo, Langli, Wang, Chongmin, Engelhard, Mark H., Kuhn, Erik, Chen, Xiaowen, Tucker, Melvin P., and Yang, Bin. Wed . "One-pot process for hydrodeoxygenation of lignin to alkanes using Ru-based bimetallic and bifunctional catalysts supported on zeolite Y". United States. doi:10.1002/cssc.201700160. https://www.osti.gov/servlets/purl/1353424.
@article{osti_1353424,
title = {One-pot process for hydrodeoxygenation of lignin to alkanes using Ru-based bimetallic and bifunctional catalysts supported on zeolite Y},
author = {Wang, Hongliang and Ruan, Hao and Feng, Maoqi and Qin, Yuling and Job, Heather and Luo, Langli and Wang, Chongmin and Engelhard, Mark H. and Kuhn, Erik and Chen, Xiaowen and Tucker, Melvin P. and Yang, Bin},
abstractNote = {Here, the synthesis of high-efficiency and low-cost catalysts for hydrodeoxygenation (HDO) of waste lignin to advanced biofuels is crucial for enhancing current biorefinery processes. Inexpensive transition metals, including Fe, Ni, Cu, and Zn, were severally co-loaded with Ru on HY zeolite to form bimetallic and bifunctional catalysts. These catalysts were subsequently tested for HDO conversion of softwood lignin and several lignin model compounds. Results indicated that the inexpensive earth-abundant metals could modulate the hydrogenolysis activity of Ru and decrease the yield of low-molecular-weight gaseous products. Among these catalysts, Ru-Cu/HY showed the best HDO performance, affording the highest selectivity to hydrocarbon products. The improved catalytic performance of Ru-Cu/HY was probably a result of the following three factors: (1) high total and strong acid sites, (2) good dispersion of metal species and limited segregation, and (3) high adsorption capacity for polar fractions, including hydroxyl groups and ether bonds. Moreover, all bifunctional catalysts proved to be superior over the combination catalysts of Ru/Al2O3 and HY zeolite.},
doi = {10.1002/cssc.201700160},
journal = {ChemSusChem},
number = 8,
volume = 10,
place = {United States},
year = {Wed Feb 22 00:00:00 EST 2017},
month = {Wed Feb 22 00:00:00 EST 2017}
}

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  • The synthesis of high-efficiency and low-cost multifunctional catalysts for hydrodeoxygenation (HDO) of waste lignin into advanced biofuels is crucial for enhancing current biorefinery processes. Inexpensive transition metals, including Fe, Ni, Cu, Zn, were severally co-loaded with Ru on HY zeolite to form bimetallic and bifunctional catalysts. These catalysts were subsequently tested for HDO conversion of softwood lignin and several lignin model compounds. Results indicated that the inexpensive earth abundant metals could modulate the hydrogenolysis activity of Ru and decrease the yield of low molecular weight gaseous side-products. Among all the prepared catalysts, Ru-Cu/HY showed the best HDO performance, giving themore » highest selectivity to hydrocarbon products. The improved catalytic performance of Ru-Cu/HY was probably due to the following three factors: (1) high total and strong acid sites, (2) good dispersion of metal species and limited segregation, (3) high adsorption capacity for polar fractions, including hydroxyl groups and ether bonds. Moreover, all the bifunctional catalysts were proven to be superior over the combination catalysts of Ru/Al2O3 and HY zeolite, and this could be attributed to the “intimacy criterion”. The practical use of the designed catalysts would be promising in lignin valorization.« less
  • Flow reactor studies of the selective hydrogenation of acetylene in the presence of ethylene have been performed on Na+ exchanged {beta}-zeolite supported Pd, Ag and PdAg catalysts, as an extension of our previous batch reactor studies [W. Huang, J.R. McCormick, R.F. Lobo, J.G. Chen, J. Catal. 246 (2007) 40-51]. Results from flow reactor studies show that the PdAg/Na+-{beta}-zeolite bimetallic catalyst has lower activity than Pd/Na+-{beta}-zeolite monometallic catalyst, while Ag/Na+-{beta}-zeolite does not show any activity for acetylene hydrogenation. However, the selectivity for the PdAg bimetallic catalyst is much higher than that for either the Pd catalyst or Ag catalyst. The selectivitymore » to byproduct (ethane) is greatly inhibited on the PdAg bimetallic catalyst as well. The results from the current flow reactor studies confirmed the pervious results from batch reactor studies [W. Huang, J.R. McCormick, R.F. Lobo, J.G. Chen, J. Catal. 246 (2007) 40-51]. In addition, we used transmission electron microscope (TEM), extended X-ray absorption fine structure (EXAFS), and FTIR of CO adsorption to confirm the formation of Pd-Ag bimetallic alloy in the PdAg/Na+-{beta}-zeolite catalyst.« less
  • The laws of the transformations of methanol, the compounds CH/sub 3/X (where X = C1, Br, etc.), CH/sub 4/ + X (X = C1/sub 2/, Br/sub 2/, O/sub 2/, N/SUB x/ O/SUB y/), and CO + H/sub 2/ in the presence of catalytic systems based on type Y zeolites, erionite, mordenite, and silicarich zeolites (VKTs) are considered. A model of the centers catalytically active in hydrocarbon-forming reactions on zeolites is proposed on the basis of results of /sup 27/A1 and /sup 29/Si NMR.