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Title: Hierarchically Structured CeO2 Catalyst Particles From Nanocellulose/Alginate Templates for Upgrading of Fast Pyrolysis Vapors

Abstract

Hierarchically structured porous materials often exhibit advantageous functionality for many applications including catalysts, adsorbents, and filtration systems. In this study, we report a facile approach to achieve hierarchically structured, porous cerium oxide (CeO2) catalyst particles using a templating method based on nanocellulose, a class of renewable, plant-derived nanomaterials. We demonstrate the catalyst performance benefits provided by this templating method in the context of Catalytic Fast Pyrolysis (CFP) which is a promising conversion technology to produce renewable fuel and chemical products from biomass and other types of organic waste. We show that variations in the porous structures imparted by this templating method may be achieved by modifying the content of cellulose nanofibrils, cellulose nanocrystals, and alginate in the templating suspensions. Nitrogen physisorption reveals that nearly 10-fold increases in surface area can be achieved using this method with respect to commercially available cerium oxide powder. Multiscale electron microscopy further verifies that bio-derived templating can alter the morphology of the catalyst nanostructure and tune the distribution of meso- and macro-porosity within the catalyst particles while maintaining CeO2 crystal structure. CFP experiments demonstrate that the templated catalysts display substantially higher activity on a gravimetric basis than their non-templated counterpart, and that variations in themore » catalyst architecture can impact the distribution of upgraded pyrolysis products. Finally, we demonstrate that the templating method described here may be extended to other materials derived from metal chlorides to achieve 3-dimensional networks of hierarchical porosity.« less

Authors:
; ; ; ; ;
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
OSTI Identifier:
1572417
Alternate Identifier(s):
OSTI ID: 1574198
Report Number(s):
NREL/JA-2700-75394
Journal ID: ISSN 2296-2646; 730
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Published Article
Journal Name:
Frontiers in Chemistry
Additional Journal Information:
Journal Name: Frontiers in Chemistry Journal Volume: 7; Journal ID: ISSN 2296-2646
Publisher:
Frontiers Media SA
Country of Publication:
Switzerland
Language:
English
Subject:
09 BIOMASS FUELS; nanocellulose; catalysis; fast pyrolysis; hierarchical structure; templated synthesis; CCTPL

Citation Formats

Moyer, Kathleen, Conklin, Davis R., Mukarakate, Calvin, Vardon, Derek R., Nimlos, Mark R., and Ciesielski, Peter N. Hierarchically Structured CeO2 Catalyst Particles From Nanocellulose/Alginate Templates for Upgrading of Fast Pyrolysis Vapors. Switzerland: N. p., 2019. Web. doi:10.3389/fchem.2019.00730.
Moyer, Kathleen, Conklin, Davis R., Mukarakate, Calvin, Vardon, Derek R., Nimlos, Mark R., & Ciesielski, Peter N. Hierarchically Structured CeO2 Catalyst Particles From Nanocellulose/Alginate Templates for Upgrading of Fast Pyrolysis Vapors. Switzerland. https://doi.org/10.3389/fchem.2019.00730
Moyer, Kathleen, Conklin, Davis R., Mukarakate, Calvin, Vardon, Derek R., Nimlos, Mark R., and Ciesielski, Peter N. 2019. "Hierarchically Structured CeO2 Catalyst Particles From Nanocellulose/Alginate Templates for Upgrading of Fast Pyrolysis Vapors". Switzerland. https://doi.org/10.3389/fchem.2019.00730.
@article{osti_1572417,
title = {Hierarchically Structured CeO2 Catalyst Particles From Nanocellulose/Alginate Templates for Upgrading of Fast Pyrolysis Vapors},
author = {Moyer, Kathleen and Conklin, Davis R. and Mukarakate, Calvin and Vardon, Derek R. and Nimlos, Mark R. and Ciesielski, Peter N.},
abstractNote = {Hierarchically structured porous materials often exhibit advantageous functionality for many applications including catalysts, adsorbents, and filtration systems. In this study, we report a facile approach to achieve hierarchically structured, porous cerium oxide (CeO2) catalyst particles using a templating method based on nanocellulose, a class of renewable, plant-derived nanomaterials. We demonstrate the catalyst performance benefits provided by this templating method in the context of Catalytic Fast Pyrolysis (CFP) which is a promising conversion technology to produce renewable fuel and chemical products from biomass and other types of organic waste. We show that variations in the porous structures imparted by this templating method may be achieved by modifying the content of cellulose nanofibrils, cellulose nanocrystals, and alginate in the templating suspensions. Nitrogen physisorption reveals that nearly 10-fold increases in surface area can be achieved using this method with respect to commercially available cerium oxide powder. Multiscale electron microscopy further verifies that bio-derived templating can alter the morphology of the catalyst nanostructure and tune the distribution of meso- and macro-porosity within the catalyst particles while maintaining CeO2 crystal structure. CFP experiments demonstrate that the templated catalysts display substantially higher activity on a gravimetric basis than their non-templated counterpart, and that variations in the catalyst architecture can impact the distribution of upgraded pyrolysis products. Finally, we demonstrate that the templating method described here may be extended to other materials derived from metal chlorides to achieve 3-dimensional networks of hierarchical porosity.},
doi = {10.3389/fchem.2019.00730},
url = {https://www.osti.gov/biblio/1572417}, journal = {Frontiers in Chemistry},
issn = {2296-2646},
number = ,
volume = 7,
place = {Switzerland},
year = {Wed Oct 30 00:00:00 EDT 2019},
month = {Wed Oct 30 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.3389/fchem.2019.00730

Citation Metrics:
Cited by: 5 works
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Works referenced in this record:

Stabilization of furanics to cyclic ketone building blocks in the vapor phase
journal, October 2019


Correction To Wood-Derived Materials for Green Electronics, Biological Devices, and Energy Applications
journal, September 2016


Ultrahigh intercalation pseudocapacitance of mesoporous orthorhombic niobium pentoxide from a novel cellulose nanocrystal template
journal, January 2015


Hierarchically porous materials: synthesis strategies and structure design
journal, January 2017


A critical review of the current knowledge regarding the biological impact of nanocellulose
journal, December 2016


A Sustainable Template for Mesoporous Zeolite Synthesis
journal, February 2014


Hierarchical zeolites: Synthesis and catalytic properties
journal, March 2018


Properties and Reactivity of Nanostructured CeO 2 Powders:  Comparison among Two Synthesis Procedures
journal, December 2005


Photocatalytic Antifouling Graphene Oxide-Mediated Hierarchical Filtration Membranes with Potential Applications on Water Purification
journal, September 2014


Chemistry challenges to enable a sustainable bioeconomy
journal, September 2017


Condensation reactions of propanal over CexZr1−xO2 mixed oxide catalysts
journal, September 2010


Surfactant-assisted synthesis of CeO2 nanoparticles and their application in wastewater treatment
journal, January 2012


Biological Chitin-MOF Composites with Hierarchical Pore Systems for Air-Filtration Applications
journal, August 2015


Key advances in the chemical modification of nanocelluloses
journal, January 2014


Inorganic Hollow Nanotube Aerogels by Atomic Layer Deposition onto Native Nanocellulose Templates
journal, February 2011


A Perspective on Catalytic Strategies for Deoxygenation in Biomass Pyrolysis
journal, August 2016


Ordered Mesoporous CeO 2 Synthesized by Nanocasting from Cubic Ia3d Mesoporous MCM-48 Silica: Formation, Characterization and Photocatalytic Activity
journal, October 2008


Catalytic Upgrading of Biomass Fast Pyrolysis Vapors with Nano Metal Oxides: An Analytical Py-GC/MS Study
journal, November 2010


Synthesis and Characterization of Cerium Oxide Nanoparticles by Hydroxide Mediated Approach
journal, December 2012


Modeling HCCI combustion of biofuels: A review
journal, April 2012


Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors
journal, May 2017


Synthesis of mesoporous silica by sol–gel mineralisation of cellulose nanorod nematic suspensions
journal, February 2003


Chiral Nematic Mesoporous Carbon Derived From Nanocrystalline Cellulose
journal, September 2011


Advancing catalytic fast pyrolysis through integrated multiscale modeling and experimentation: Challenges, progress, and perspectives
journal, April 2018

  • Ciesielski, Peter N.; Pecha, M. Brennan; Bharadwaj, Vivek S.
  • Wiley Interdisciplinary Reviews: Energy and Environment, Vol. 7, Issue 4
  • https://doi.org/10.1002/wene.297

Real-time monitoring of the deactivation of HZSM-5 during upgrading of pine pyrolysis vapors
journal, January 2014


Molybdenum incorporated mesoporous silica catalyst for production of biofuels and value-added chemicals via catalytic fast pyrolysis
journal, January 2015


From Hydrocolloids to High Specific Surface Area Porous Supports for Catalysis
journal, September 2005


Catalytic conversion of biomass pyrolysis vapors into hydrocarbon fuel precursors
journal, January 2015


Role of Biopolymers in the Deactivation of ZSM-5 during Catalytic Fast Pyrolysis of Biomass
journal, June 2018


Preparation methods of alginate nanoparticles
journal, July 2014


Template synthesis of porous titania using cellulose nanocrystals
journal, May 2007


Ceria Catalysts at Nanoscale: How Do Crystal Shapes Shape Catalysis?
journal, June 2017


Ketonization of Carboxylic Acids: Mechanisms, Catalysts, and Implications for Biomass Conversion
journal, October 2013


Review of Hydrogels and Aerogels Containing Nanocellulose
journal, April 2017


Cellulose Nanofibril Hydrogel Tubes as Sacrificial Templates for Freestanding Tubular Cell Constructs
journal, February 2016


Production of nanocrystalline cellulose from lignocellulosic biomass: Technology and applications
journal, April 2013


Ceria-Based Solid Catalysts for Organic Chemistry
journal, May 2010


Free-standing mesoporous silica films with tunable chiral nematic structures
journal, November 2010


Cellulose Nanocrystals: Chemistry, Self-Assembly, and Applications
journal, June 2010


Heat and Mass Transfer Effects in a Furnace-Based Micropyrolyzer
journal, August 2016


Chiral Nematic Mesoporous Carbon Derived From Nanocrystalline Cellulose
journal, September 2011


Works referencing / citing this record:

Chiral Nematic Mesoporous Carbon Derived From Nanocrystalline Cellulose
journal, September 2011


Biological Chitin-MOF Composites with Hierarchical Pore Systems for Air-Filtration Applications
journal, August 2015


Ceria-Based Solid Catalysts for Organic Chemistry
journal, May 2010


A Perspective on Catalytic Strategies for Deoxygenation in Biomass Pyrolysis
journal, August 2016


Heat and Mass Transfer Effects in a Furnace-Based Micropyrolyzer
journal, August 2016


Advancing catalytic fast pyrolysis through integrated multiscale modeling and experimentation: Challenges, progress, and perspectives
journal, April 2018

  • Ciesielski, Peter N.; Pecha, M. Brennan; Bharadwaj, Vivek S.
  • Wiley Interdisciplinary Reviews: Energy and Environment, Vol. 7, Issue 4
  • https://doi.org/10.1002/wene.297

Condensation reactions of propanal over CexZr1−xO2 mixed oxide catalysts
journal, September 2010


Stabilization of furanics to cyclic ketone building blocks in the vapor phase
journal, October 2019


Production of nanocrystalline cellulose from lignocellulosic biomass: Technology and applications
journal, April 2013


Preparation methods of alginate nanoparticles
journal, July 2014


Ultrahigh intercalation pseudocapacitance of mesoporous orthorhombic niobium pentoxide from a novel cellulose nanocrystal template
journal, January 2015


Template synthesis of porous titania using cellulose nanocrystals
journal, May 2007


Hierarchical zeolites: Synthesis and catalytic properties
journal, March 2018


Modeling HCCI combustion of biofuels: A review
journal, April 2012


Cellulose Nanofibril Hydrogel Tubes as Sacrificial Templates for Freestanding Tubular Cell Constructs
journal, February 2016


Review of Hydrogels and Aerogels Containing Nanocellulose
journal, April 2017


Correction To Wood-Derived Materials for Green Electronics, Biological Devices, and Energy Applications
journal, September 2016


Ceria Catalysts at Nanoscale: How Do Crystal Shapes Shape Catalysis?
journal, June 2017


Deactivation of Multilayered MFI Nanosheet Zeolite during Upgrading of Biomass Pyrolysis Vapors
journal, May 2017


Role of Biopolymers in the Deactivation of ZSM-5 during Catalytic Fast Pyrolysis of Biomass
journal, June 2018


Photocatalytic Antifouling Graphene Oxide-Mediated Hierarchical Filtration Membranes with Potential Applications on Water Purification
journal, September 2014


From Hydrocolloids to High Specific Surface Area Porous Supports for Catalysis
journal, September 2005


Properties and Reactivity of Nanostructured CeO 2 Powders:  Comparison among Two Synthesis Procedures
journal, December 2005


Cellulose Nanocrystals: Chemistry, Self-Assembly, and Applications
journal, June 2010


Ketonization of Carboxylic Acids: Mechanisms, Catalysts, and Implications for Biomass Conversion
journal, October 2013


A Sustainable Template for Mesoporous Zeolite Synthesis
journal, February 2014


Ordered Mesoporous CeO 2 Synthesized by Nanocasting from Cubic Ia3d Mesoporous MCM-48 Silica: Formation, Characterization and Photocatalytic Activity
journal, October 2008


Inorganic Hollow Nanotube Aerogels by Atomic Layer Deposition onto Native Nanocellulose Templates
journal, February 2011


Free-standing mesoporous silica films with tunable chiral nematic structures
journal, November 2010


Chemistry challenges to enable a sustainable bioeconomy
journal, September 2017


Synthesis of mesoporous silica by sol–gel mineralisation of cellulose nanorod nematic suspensions
journal, February 2003


Surfactant-assisted synthesis of CeO2 nanoparticles and their application in wastewater treatment
journal, January 2012


A critical review of the current knowledge regarding the biological impact of nanocellulose
journal, December 2016


Catalytic Upgrading of Biomass Fast Pyrolysis Vapors with Nano Metal Oxides: An Analytical Py-GC/MS Study
journal, November 2010


Synthesis and Characterization of Cerium Oxide Nanoparticles by Hydroxide Mediated Approach
journal, December 2012