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Title: Catalytic valorization of hardwood for enhanced xylose-hydrolysate recovery and cellulose enzymatic efficiency via synergistic effect of Fe3+ and acetic acid

Abstract

Background: Poplars are considered suitable dedicated energy crops, with abundant cellulose and hemicellulose, and huge surplus biomass potential in China. Xylan, the major hemicellulosic component, contributes to the structural stability of wood and represents a tremendous quantity of biobased chemicals for fuel production. Monomeric xylose conversion to value-added chemicals such as furfural, xylitol, and xylonic acid could greatly improve the economics of pulp-paper industry and biorefinery. Acetic acid (HAc) is used as a friendly and recyclable selective catalyst amenable to xylan degradation and xylooligosaccharides production from lignocellulosic materials. However, HAc catalyst usually works much feebly at inert woods than agricultural straws. In this study, effects of different iron species in HAc media on poplar xylan degradation were systematically compared, and a preferable Fe3+-assisted HAc hydrolysis process was proposed for comparable xylose-hydrolysate recovery (XHR) and enzymatic saccharifcation of cellulose. Results: In presence of 6.5% HAc with 0.17–0.25 wt% Fe3+, xylose yield ranged between 72.5 and 73.9%. Additionally, pretreatment was effective in poplar delignification, with a lignin yield falling between 38.6 and 42.5%. Under similar conditions, saccharifcation efficiency varied between 60.3 and 65.9%. Starting with 100 g poplar biomass, a total amount of 12.7–12.8 g of xylose and 18.8–22.8 g of glucosemore » were harvested from liquid streams during the whole process of Fe3+-HAc hydrolysis coupled with enzymatic saccharification. Furthermore, the enhancement mechanism of Fe3+ coupled with HAc was investigated after proof-of-concept experiments. Beechwood xylan and xylose were treated under the same condition as poplar sawdust fractionation, giving understanding of the effect of catalysts on the hydrolysis pathway from wood xylan to xylose and furfural by Fe3+-HAc. Conclusions: The Fe3+-assisted HAc hydrolysis process was demonstrated as an effective approach to the wood xylose and other monosaccharides production. Synergistic effect of Lewis acid site and aqueous acetic acid provided a promising strategy for catalytic valorization of poplar biomass.« less

Authors:
 [1];  [2];  [1]; ORCiD logo [1]
  1. Nanjing Forestry Univ. (China). Key Lab. of Forestry Genetics & Biotechnology; Nanjing Forestry Univ. (China). Jiangsu Province Key Lab. of Green Biomass-based Fuels and Chemicals. Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources. College of Chemical Engineering
  2. Joint BioEnergy Institute (JBEI), Emeryville, CA (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States). Biomass Science and Conversion Technology
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER). Earth and Environmental Systems Science Division
OSTI Identifier:
1627006
Grant/Contract Number:  
NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Biotechnology for Biofuels
Additional Journal Information:
Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 1754-6834
Publisher:
BioMed Central
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 09 BIOMASS FUELS; Biotechnology & Applied Microbiology; Energy & Fuels; Poplar; Acetic acid catalysis; Fe3+-assisted hydrolysis; Xylose-hydrolysate recovery; Enzymatic saccharifcation of cellulose

Citation Formats

Huang, Kaixuan, Das, Lalitendu, Guo, Jianming, and Xu, Yong. Catalytic valorization of hardwood for enhanced xylose-hydrolysate recovery and cellulose enzymatic efficiency via synergistic effect of Fe3+ and acetic acid. United States: N. p., 2019. Web. doi:10.1186/s13068-019-1587-4.
Huang, Kaixuan, Das, Lalitendu, Guo, Jianming, & Xu, Yong. Catalytic valorization of hardwood for enhanced xylose-hydrolysate recovery and cellulose enzymatic efficiency via synergistic effect of Fe3+ and acetic acid. United States. https://doi.org/10.1186/s13068-019-1587-4
Huang, Kaixuan, Das, Lalitendu, Guo, Jianming, and Xu, Yong. Thu . "Catalytic valorization of hardwood for enhanced xylose-hydrolysate recovery and cellulose enzymatic efficiency via synergistic effect of Fe3+ and acetic acid". United States. https://doi.org/10.1186/s13068-019-1587-4. https://www.osti.gov/servlets/purl/1627006.
@article{osti_1627006,
title = {Catalytic valorization of hardwood for enhanced xylose-hydrolysate recovery and cellulose enzymatic efficiency via synergistic effect of Fe3+ and acetic acid},
author = {Huang, Kaixuan and Das, Lalitendu and Guo, Jianming and Xu, Yong},
abstractNote = {Background: Poplars are considered suitable dedicated energy crops, with abundant cellulose and hemicellulose, and huge surplus biomass potential in China. Xylan, the major hemicellulosic component, contributes to the structural stability of wood and represents a tremendous quantity of biobased chemicals for fuel production. Monomeric xylose conversion to value-added chemicals such as furfural, xylitol, and xylonic acid could greatly improve the economics of pulp-paper industry and biorefinery. Acetic acid (HAc) is used as a friendly and recyclable selective catalyst amenable to xylan degradation and xylooligosaccharides production from lignocellulosic materials. However, HAc catalyst usually works much feebly at inert woods than agricultural straws. In this study, effects of different iron species in HAc media on poplar xylan degradation were systematically compared, and a preferable Fe3+-assisted HAc hydrolysis process was proposed for comparable xylose-hydrolysate recovery (XHR) and enzymatic saccharifcation of cellulose. Results: In presence of 6.5% HAc with 0.17–0.25 wt% Fe3+, xylose yield ranged between 72.5 and 73.9%. Additionally, pretreatment was effective in poplar delignification, with a lignin yield falling between 38.6 and 42.5%. Under similar conditions, saccharifcation efficiency varied between 60.3 and 65.9%. Starting with 100 g poplar biomass, a total amount of 12.7–12.8 g of xylose and 18.8–22.8 g of glucose were harvested from liquid streams during the whole process of Fe3+-HAc hydrolysis coupled with enzymatic saccharification. Furthermore, the enhancement mechanism of Fe3+ coupled with HAc was investigated after proof-of-concept experiments. Beechwood xylan and xylose were treated under the same condition as poplar sawdust fractionation, giving understanding of the effect of catalysts on the hydrolysis pathway from wood xylan to xylose and furfural by Fe3+-HAc. Conclusions: The Fe3+-assisted HAc hydrolysis process was demonstrated as an effective approach to the wood xylose and other monosaccharides production. Synergistic effect of Lewis acid site and aqueous acetic acid provided a promising strategy for catalytic valorization of poplar biomass.},
doi = {10.1186/s13068-019-1587-4},
journal = {Biotechnology for Biofuels},
number = 1,
volume = 12,
place = {United States},
year = {Thu Oct 17 00:00:00 EDT 2019},
month = {Thu Oct 17 00:00:00 EDT 2019}
}

Works referenced in this record:

Low acid hydrothermal fractionation of Giant Miscanthus for production of xylose-rich hydrolysate and furfural
journal, October 2016


Oxidative conversion of glucose to gluconic acid by iron( iii ) chloride in water under mild conditions
journal, January 2016

  • Zhang, Hongdan; Li, Ning; Pan, Xuejun
  • Green Chemistry, Vol. 18, Issue 8
  • DOI: 10.1039/C5GC02614H

Iron-Catalyzed Furfural Production in Biobased Biphasic Systems: From Pure Sugars to Direct Use of Crude Xylose Effluents as Feedstock
journal, October 2011

  • vom Stein, Thorsten; Grande, Philipp M.; Leitner, Walter
  • ChemSusChem, Vol. 4, Issue 11
  • DOI: 10.1002/cssc.201100259

Sugar and ethanol production from woody biomass via supercritical water hydrolysis in a continuous pilot-scale system using acid catalyst
journal, December 2017


Xylan hydrolysis in Populus trichocarpa×P. deltoides and model substrates during hydrothermal pretreatment
journal, March 2015


Chemicals from biomass: technological versus environmental feasibility. A review
journal, November 2016

  • Fiorentino, Gabriella; Ripa, Maddalena; Ulgiati, Sergio
  • Biofuels, Bioproducts and Biorefining, Vol. 11, Issue 1
  • DOI: 10.1002/bbb.1729

Enhanced Furfural Yields from Xylose Dehydration in the γ-Valerolactone/Water Solvent System at Elevated Temperatures
journal, June 2018

  • Sener, Canan; Motagamwala, Ali Hussain; Alonso, David Martin
  • ChemSusChem, Vol. 11, Issue 14
  • DOI: 10.1002/cssc.201800730

Enhanced Xylooligosaccharides Yields and Enzymatic Hydrolyzability of Cellulose using Acetic Acid Catalysis of Poplar Sawdust
journal, September 2018


Energetics of Xylose Decomposition as Determined Using Quantum Mechanics Modeling
journal, October 2006

  • Nimlos, Mark R.; Qian, Xianghong; Davis, Mark
  • The Journal of Physical Chemistry A, Vol. 110, Issue 42
  • DOI: 10.1021/jp0626770

Furfural production from Eucalyptus wood using an Acidic Ionic Liquid
journal, August 2016


Seawater-based furfural production via corncob hydrolysis catalyzed by FeCl3 in acetic acid steam
journal, January 2013

  • Mao, Liaoyuan; Zhang, Lei; Gao, Ningbo
  • Green Chemistry, Vol. 15, Issue 3
  • DOI: 10.1039/c2gc36346a

β-Factor Based Separation Characteristics of Bio-derived Chemicals Present in Lignocellulosic Hydrolysates Using Vacuum Distillation
journal, December 2018


Fractionation of wheat straw by atmospheric acetic acid process
journal, July 2005


A study on the consecutive preparation of d-xylose and pure superfine silica from rice husk
journal, February 2010


Xylose and cellulose fractionation from corncob with three different strategies and separate fermentation of them to bioethanol
journal, September 2010


Conversion of xylose into furfural in a MOF-based mixed matrix membrane reactor
journal, December 2016


Biorefining: Heterogeneously Catalyzed Reactions of Carbohydrates for the Production of Furfural and Hydroxymethylfurfural
journal, July 2011


Highly efficient and selective CO 2 -adjunctive dehydration of xylose to furfural in aqueous media with THF
journal, January 2016

  • Morais, Ana Rita C.; Bogel-Lukasik, Rafal
  • Green Chemistry, Vol. 18, Issue 8
  • DOI: 10.1039/C5GC02863A

Acid-Catalyzed 2-Furaldehyde (Furfural) Decomposition Kinetics
journal, February 2000

  • Rose, Ian C.; Epstein, Norman; Watkinson, A. Paul
  • Industrial & Engineering Chemistry Research, Vol. 39, Issue 3
  • DOI: 10.1021/ie990550+

Effects and Mechanism of Metal Chloride Salts on Pretreatment and Enzymatic Digestibility of Corn Stover
journal, January 2013

  • Kamireddy, Srinivas R.; Li, Jinbao; Tucker, Melvin
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 5
  • DOI: 10.1021/ie3019609

Fungal treatment followed by FeCl3 treatment to enhance enzymatic hydrolysis of poplar wood for high sugar yields
journal, August 2013


Use of metal chlorides during waste wheat straw autohydrolysis to overcome the self-buffering effect
journal, November 2018


Generation of electricity from FeCl3 pretreatment of rice straw using a fuel cell system
journal, May 2013


Production of furfural from xylose, xylan and corncob in gamma-valerolactone using FeCl3·6H2O as catalyst
journal, January 2014


Corn stover pretreatment by inorganic salts and its effects on hemicellulose and cellulose degradation
journal, December 2009


Pretreatment of Japanese cedar by ionic liquid solutions in combination with acid and metal ion and its application to high solid loading
journal, August 2014

  • Ogura, Kazuma; Ninomiya, Kazuaki; Takahashi, Kenji
  • Biotechnology for Biofuels, Vol. 7, Issue 1
  • DOI: 10.1186/s13068-014-0120-z

Advanced Oxidation Processes for Organic Contaminant Destruction Based on the Fenton Reaction and Related Chemistry
journal, January 2006

  • Pignatello, Joseph J.; Oliveros, Esther; MacKay, Allison
  • Critical Reviews in Environmental Science and Technology, Vol. 36, Issue 1
  • DOI: 10.1080/10643380500326564

Comparative characterization of milled wood lignin from furfural residues and corncob
journal, November 2011


A study on catalytic hydrolysis of peat
journal, September 1996


The enhancement of xylose monomer and xylotriose degradation by inorganic salts in aqueous solutions at 180 °C
journal, November 2006


FeCl3 and acetic acid co-catalyzed hydrolysis of corncob for improving furfural production and lignin removal from residue
journal, November 2012


Removal of non-structural components from poplar whole-tree chips to enhance hydrolysis and fermentation performance
journal, August 2018


Chloride ions enhance furfural formation from d-xylose in dilute aqueous acidic solutions
journal, January 2010

  • Marcotullio, Gianluca; De Jong, Wiebren
  • Green Chemistry, Vol. 12, Issue 10
  • DOI: 10.1039/b927424c

Ferric chloride assisted plasma pretreatment of lignocellulose
journal, November 2017


Deposition of Lignin Droplets Produced During Dilute Acid Pretreatment of Maize Stems Retards Enzymatic Hydrolysis of Cellulose
journal, December 2007

  • Selig, M. J.; Viamajala, S.; Decker, S. R.
  • Biotechnology Progress, Vol. 23, Issue 6
  • DOI: 10.1021/bp0702018

Acid-catalyzed conversion of xylose, xylan and straw into furfural by microwave-assisted reaction
journal, August 2011


Synthesis of Furfural from Xylose, Xylan, and Biomass Using AlCl3⋅6 H2O in Biphasic Media via Xylose Isomerization to Xylulose
journal, February 2012


Hydrolysis of bamboo biomass by subcritical water treatment
journal, September 2015


Acid-Catalyzed Conversion of Sugars and Furfurals in an Ionic-Liquid Phase
journal, July 2009

  • Sievers, Carsten; Musin, Ildar; Marzialetti, Teresita
  • ChemSusChem, Vol. 2, Issue 7
  • DOI: 10.1002/cssc.200900092

Compositional Analysis of Lignocellulosic Feedstocks. 1. Review and Description of Methods
journal, August 2010

  • Sluiter, Justin B.; Ruiz, Raymond O.; Scarlata, Christopher J.
  • Journal of Agricultural and Food Chemistry, Vol. 58, Issue 16, p. 9043-9053
  • DOI: 10.1021/jf1008023

Enhanced Furfural Yields from Xylose Dehydration in the γ-Valerolactone/Water Solvent System at Elevated Temperatures
journal, July 2018

  • Sener, Canan; Motagamwala, Ali Hussain; Alonso, David Martin
  • ChemSusChem, Vol. 11, Issue 14
  • DOI: 10.1002/cssc.201801506