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Title: Methyl Ketone Condensation over Tailored Metal Oxides

Abstract

Methyl ketones represent promising oxygenate intermediates that can be derived from lignocellulosic biomass via numerous conversion routes and subsequently coupled to produce precursors for renewable diesel and aviation fuels. Basic metal oxides are known to promote ketone coupling via condensation reactions, with magnesium oxide (MgO) providing an ideal catalytic system for evaluating the reaction mechanism and role of water on observed activity. Recent studies demonstrate that the MgO(111) surface facet can be promoted to enhance activity for base catalyzed reactions; however, to our knowledge, there is a dearth of information regarding the impact of MgO(111) faceting and surface termination under reaction conditions for ketone coupling. Therefore, this talk will discuss our recent investigation into the catalytic coupling of methyl ketones over MgO(100) and MgO(111) catalysts. Results will be presented that address the synthesis and detailed characterization of MgO(111) nanosheets, as well as their activity and selectivity for ketone coupling when compared to MgO(100). The impact of water on MgO surface termination will be discussed, as well as a proposed reaction mechanism for ketone condensation over clean and hydroxyl terminated surfaces for both facets. Findings will include outcomes from experimental studies, computational modeling, and advanced surface characterization by neutron scattering. Collectively,more » this work provides further insight into the role of tailored metal oxide catalysts for this important class of biomass conversion chemistry.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [2];  [1];  [1];  [3];  [3];  [3];  [4];  [2]
  1. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  2. Argonne National Laboratory
  3. Oak Ridge National Laboratory
  4. Colorado School of Mines, Golden Colorado
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
OSTI Identifier:
1569208
Report Number(s):
NREL/PR-5100-75017
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Conference
Resource Relation:
Conference: Presented at the ACS Fall National Meeting 2019, 26-27 August 2019, San Diego, California
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; biofuels; biomass; lignocellulosic biomass; methyl ketones; magnesium oxide; metal oxide catalyst; oxygenate intermediates; renewable diesel; aviation fuels

Citation Formats

Vardon, Derek R, Huo, Xiangchen, Vorotnikov, Vassili, Beckham, Gregg T, Zhou, Mingxia, Conklin, Davis, York, Allyson, Metz, Peter Metz, Li, Zhenglong, Page, Katharine L., Richards, Ryan, and Assary, Rajeez. Methyl Ketone Condensation over Tailored Metal Oxides. United States: N. p., 2019. Web.
Vardon, Derek R, Huo, Xiangchen, Vorotnikov, Vassili, Beckham, Gregg T, Zhou, Mingxia, Conklin, Davis, York, Allyson, Metz, Peter Metz, Li, Zhenglong, Page, Katharine L., Richards, Ryan, & Assary, Rajeez. Methyl Ketone Condensation over Tailored Metal Oxides. United States.
Vardon, Derek R, Huo, Xiangchen, Vorotnikov, Vassili, Beckham, Gregg T, Zhou, Mingxia, Conklin, Davis, York, Allyson, Metz, Peter Metz, Li, Zhenglong, Page, Katharine L., Richards, Ryan, and Assary, Rajeez. Fri . "Methyl Ketone Condensation over Tailored Metal Oxides". United States. https://www.osti.gov/servlets/purl/1569208.
@article{osti_1569208,
title = {Methyl Ketone Condensation over Tailored Metal Oxides},
author = {Vardon, Derek R and Huo, Xiangchen and Vorotnikov, Vassili and Beckham, Gregg T and Zhou, Mingxia and Conklin, Davis and York, Allyson and Metz, Peter Metz and Li, Zhenglong and Page, Katharine L. and Richards, Ryan and Assary, Rajeez},
abstractNote = {Methyl ketones represent promising oxygenate intermediates that can be derived from lignocellulosic biomass via numerous conversion routes and subsequently coupled to produce precursors for renewable diesel and aviation fuels. Basic metal oxides are known to promote ketone coupling via condensation reactions, with magnesium oxide (MgO) providing an ideal catalytic system for evaluating the reaction mechanism and role of water on observed activity. Recent studies demonstrate that the MgO(111) surface facet can be promoted to enhance activity for base catalyzed reactions; however, to our knowledge, there is a dearth of information regarding the impact of MgO(111) faceting and surface termination under reaction conditions for ketone coupling. Therefore, this talk will discuss our recent investigation into the catalytic coupling of methyl ketones over MgO(100) and MgO(111) catalysts. Results will be presented that address the synthesis and detailed characterization of MgO(111) nanosheets, as well as their activity and selectivity for ketone coupling when compared to MgO(100). The impact of water on MgO surface termination will be discussed, as well as a proposed reaction mechanism for ketone condensation over clean and hydroxyl terminated surfaces for both facets. Findings will include outcomes from experimental studies, computational modeling, and advanced surface characterization by neutron scattering. Collectively, this work provides further insight into the role of tailored metal oxide catalysts for this important class of biomass conversion chemistry.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {9}
}

Conference:
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