Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining

de Assis, Tiago; Huang, Shixin; Driemeier, Carlos Eduardo; Donohoe, Bryon S.; Kim, Chaehoon; Kim, Seong H.; Gonzalez, Ronalds; Jameel, Hasan; Park, Sunkyu

doi:10.1186/s13068-018-1289-3

Title: Toward an understanding of the increase in enzymatic hydrolysis by mechanical refining

Journal Article · 24 October 2018 · Biotechnology for Biofuels

DOI: https://doi.org/10.1186/s13068-018-1289-3 · OSTI ID:1482793

de Assis, Tiago ^[1]; Huang, Shixin ^[2]; Driemeier, Carlos Eduardo ^[3]; Donohoe, Bryon S. ^[4]; Kim, Chaehoon ^[1]; Kim, Seong H. ^[2]; Gonzalez, Ronalds ^[1]; Jameel, Hasan ^[1];

^[1]

North Carolina State Univ., Raleigh, NC (United States)
Pennsylvania State Univ., University Park, PA (United States)
Brazilian Bioethanol Science and Technology Lab. (CTBE), Campinas, SP (Brazil)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Mechanical refining is a low-capital and well-established technology used in pulp and paper industry to improve fiber bonding for product strength. Refining can also be applied in a biorefinery context to overcome the recalcitrance of pretreated biomass by opening up the biomass structure and modifying substrate properties (e.g., morphology, particle size, porosity, crystallinity), which increases enzyme accessibility to substrate and improves carbohydrate conversion. Although several characterization methods have been used to identify the changes in substrate properties, there is no systematic approach to evaluate the extent of fiber cell wall disruption and what physical properties can explain the improvement in enzymatic digestibility when pretreated lignocellulosic biomass is mechanically refined. This is because the fiber cell wall is complex across multiple scales, including the molecular scale, nano- and meso-scale (microfibril), and microscale (tissue level). A combination of advanced characterization tools is used in this study to better understand the effect of mechanical refining on the meso-scale microfibril assembly and the relationship between those meso-scale modifications and enzymatic hydrolysis. Enzymatic conversion of autohydrolysis sugarcane bagasse was improved from 69.6 to 77.2% (11% relative increase) after applying mechanical refining and an increase in enzymatic digestibility is observed with an increase in refining intensity. Based on a combination of advanced characterizations employed in this study, it was found that the refining action caused fiber size reduction, internal delamination, and increase in pores and swellability. A higher level of delamination and higher increase in porosity, analyzed by TEM and DSC, were clearly demonstrated, which explain the faster digestibility rate during the first 72 h of enzymatic hydrolysis for disc-refined samples when compared to the PFI-refined samples. Additionally, an increased inter-fibrillar distance between cellulose microfibrils at the nano-meso-scale was also revealed by SFG analysis, while no evidence was found for a change in crystalline structure by XRD and solid-state NMR analysis.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1482793

Report Number(s):: NREL/JA-2700-72807

Journal Information:: Biotechnology for Biofuels, Journal Name: Biotechnology for Biofuels Journal Issue: 1 Vol. 11; ISSN 1754-6834

Publisher:: BioMed CentralCopyright Statement

Country of Publication:: United States

Language:: English

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Reduction of Enzyme Dosage by Oxygen Delignification and Mechanical Refining for Enzymatic Hydrolysis of Green Liquor-Pretreated Hardwood Koo, Bon-Wook; Treasure, Trevor H.; Jameel, Hasan Applied Biochemistry and Biotechnology, Vol. 165, Issue 3-4 https://doi.org/10.1007/s12010-011-9301-4	journal	June 2011
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Combined Deacetylation and PFI Refining Pretreatment of Corn Cob for the Improvement of a Two-Stage Enzymatic Hydrolysis Zhang, Yuedong; Mu, Xindong; Wang, Haisong Journal of Agricultural and Food Chemistry, Vol. 62, Issue 20 https://doi.org/10.1021/jf500189a	journal	May 2014
Probing crystal structure and mesoscale assembly of cellulose microfibrils in plant cell walls, tunicate tests, and bacterial films using vibrational Sum Frequency Generation (SFG) spectroscopy Lee, Christopher M.; Kafle, Kabindra; Park, Yong Bum Physical Chemistry Chemical Physics, Vol. 16, Issue 22 https://doi.org/10.1039/c4cp00515e	journal	January 2014
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Helically agitated mixing in dry dilute acid pretreatment enhances the bioconversion of corn stover into ethanol He, Yanqing; Zhang, Longping; Zhang, Jian Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-1	journal	January 2014
A highly efficient dilute alkali deacetylation and mechanical (disc) refining process for the conversion of renewable biomass to lower cost sugars Chen, Xiaowen; Shekiro, Joseph; Pschorn, Thomas Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-98	journal	January 2014
Optimization of Pilot Scale Mechanical Disk Refining for Improvements in Enzymatic Digestibility of Pretreated Hardwood Lignocellulosics Jones, Brandon W.; Venditti, Richard; Park, Sunkyu BioResources, Vol. 12, Issue 3 https://doi.org/10.15376/biores.12.3.4567-4593	journal	May 2017
Visualizing lignin coalescence and migration through maize cell walls following thermochemical pretreatment Donohoe, Bryon S.; Decker, Stephen R.; Tucker, Melvin P. Biotechnology and Bioengineering, Vol. 101, Issue 5 https://doi.org/10.1002/bit.21959	journal	December 2008
Mechanistic insights into the liquefaction stage of enzyme-mediated biomass deconstruction van der Zwan, Timo; Hu, Jinguang; Saddler, Jack N. Biotechnology and Bioengineering, Vol. 114, Issue 11 https://doi.org/10.1002/bit.26381	journal	August 2017
Measuring the crystallinity index of cellulose by solid state 13C nuclear magnetic resonance Park, Sunkyu; Johnson, David K.; Ishizawa, Claudia I. Cellulose, Vol. 16, Issue 4 https://doi.org/10.1007/s10570-009-9321-1	journal	June 2009
Dynamic vapor sorption and thermoporometry to probe water in celluloses Driemeier, Carlos; Mendes, Fernanda M.; Oliveira, Marcelo M. Cellulose, Vol. 19, Issue 4 https://doi.org/10.1007/s10570-012-9727-z	journal	May 2012
Cellulose co-crystallization and related phenomena occurring in hydrothermal treatment of sugarcane bagasse Driemeier, Carlos; Mendes, Fernanda M.; Santucci, Beatriz S. Cellulose, Vol. 22, Issue 4 https://doi.org/10.1007/s10570-015-0638-7	journal	April 2015
Reduction of Enzyme Dosage by Oxygen Delignification and Mechanical Refining for Enzymatic Hydrolysis of Green Liquor-Pretreated Hardwood Koo, Bon-Wook; Treasure, Trevor H.; Jameel, Hasan Applied Biochemistry and Biotechnology, Vol. 165, Issue 3-4 https://doi.org/10.1007/s12010-011-9301-4	journal	June 2011
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Synthetic multi-component enzyme mixtures for deconstruction of lignocellulosic biomass Banerjee, Goutami; Car, Suzana; Scott-Craig, John S. Bioresource Technology, Vol. 101, Issue 23, p. 9097-9105 https://doi.org/10.1016/j.biortech.2010.07.028	journal	December 2010
Comparison of different mechanical refining technologies on the enzymatic digestibility of low severity acid pretreated corn stover Chen, Xiaowen; Kuhn, Erik; Wang, Wei Bioresource Technology, Vol. 147 https://doi.org/10.1016/j.biortech.2013.07.109	journal	November 2013
Enhancement in enzymatic hydrolysis by mechanical refining for pretreated hardwood lignocellulosics Jones, Brandon W.; Venditti, Richard; Park, Sunkyu Bioresource Technology, Vol. 147 https://doi.org/10.1016/j.biortech.2013.08.030	journal	November 2013
Enzymatic hydrolysis of autohydrolyzed wheat straw followed by refining to produce fermentable sugars Ertas, Murat; Han, Qiang; Jameel, Hasan Bioresource Technology, Vol. 152 https://doi.org/10.1016/j.biortech.2013.11.026	journal	January 2014
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Production of fermentable sugars from sugarcane bagasse by enzymatic hydrolysis after autohydrolysis and mechanical refining Batalha, Larisse Aparecida Ribas; Han, Qiang; Jameel, Hasan Bioresource Technology, Vol. 180 https://doi.org/10.1016/j.biortech.2014.12.060	journal	March 2015
Use of mechanical refining to improve the production of low-cost sugars from lignocellulosic biomass Park, Junyeong; Jones, Brandon; Koo, Bonwook Bioresource Technology, Vol. 199 https://doi.org/10.1016/j.biortech.2015.08.059	journal	January 2016
Effects of fibrillation on the wood fibers’ enzymatic hydrolysis enhanced by mechanical refining Liu, Wei; Wang, Bing; Hou, Qingxi Bioresource Technology, Vol. 206 https://doi.org/10.1016/j.biortech.2016.01.074	journal	April 2016
Changes in pore size distribution during the drying of cellulose fibers as measured by differential scanning calorimetry Park, S.; Venditti, R.; Jameel, H. Carbohydrate Polymers, Vol. 66, Issue 1 https://doi.org/10.1016/j.carbpol.2006.02.026	journal	October 2006
Lignin contributions to the nanoscale porosity of raw and treated lignocelluloses as observed by calorimetric thermoporometry Driemeier, Carlos; Oliveira, Marcelo M.; Curvelo, Antônio A. S. Industrial Crops and Products, Vol. 82 https://doi.org/10.1016/j.indcrop.2015.11.084	journal	April 2016
Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope Lee, Christopher M.; Kafle, Kabindra; Huang, Shixin The Journal of Physical Chemistry B, Vol. 120, Issue 1 https://doi.org/10.1021/acs.jpcb.5b10290	journal	December 2015
Dependence of Sum Frequency Generation (SFG) Spectral Features on the Mesoscale Arrangement of SFG-Active Crystalline Domains Interspersed in SFG-Inactive Matrix: A Case Study with Cellulose in Uniaxially Aligned Control Samples and Alkali-Treated Secondary Cell Walls of Plants Makarem, Mohamadamin; Sawada, Daisuke; O’Neill, Hugh M. The Journal of Physical Chemistry C, Vol. 121, Issue 18 https://doi.org/10.1021/acs.jpcc.7b02770	journal	May 2017
Improving Sugar Yields and Reducing Enzyme Loadings in the Deacetylation and Mechanical Refining (DMR) Process through Multistage Disk and Szego Refining and Corresponding Techno-Economic Analysis Chen, Xiaowen; Wang, Wei; Ciesielski, Peter ACS Sustainable Chemistry & Engineering, Vol. 4, Issue 1 https://doi.org/10.1021/acssuschemeng.5b01242	journal	December 2015
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Combined Deacetylation and PFI Refining Pretreatment of Corn Cob for the Improvement of a Two-Stage Enzymatic Hydrolysis Zhang, Yuedong; Mu, Xindong; Wang, Haisong Journal of Agricultural and Food Chemistry, Vol. 62, Issue 20 https://doi.org/10.1021/jf500189a	journal	May 2014
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Probing crystal structure and mesoscale assembly of cellulose microfibrils in plant cell walls, tunicate tests, and bacterial films using vibrational Sum Frequency Generation (SFG) spectroscopy Lee, Christopher M.; Kafle, Kabindra; Park, Yong Bum Physical Chemistry Chemical Physics, Vol. 16, Issue 22 https://doi.org/10.1039/c4cp00515e	journal	January 2014
Monitoring Meso-Scale Ordering of Cellulose in Intact Plant Cell Walls Using Sum Frequency Generation Spectroscopy Park, Y. B.; Lee, C. M.; Koo, B. -W. PLANT PHYSIOLOGY, Vol. 163, Issue 2 https://doi.org/10.1104/pp.113.225235	journal	August 2013
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Cellulose crystallinity index: measurement techniques and their impact on interpreting cellulase performance Park, Sunkyu; Baker, John O.; Himmel, Michael E. Biotechnology for Biofuels, Vol. 3, Issue 1 https://doi.org/10.1186/1754-6834-3-10	journal	January 2010
Improved ethanol yield and reduced Minimum Ethanol Selling Price (MESP) by modifying low severity dilute acid pretreatment with deacetylation and mechanical refining: 1) Experimental Chen, Xiaowen; Tao, Ling; Shekiro, Joseph Biotechnology for Biofuels, Vol. 5, Issue 1 https://doi.org/10.1186/1754-6834-5-60	journal	January 2012
Helically agitated mixing in dry dilute acid pretreatment enhances the bioconversion of corn stover into ethanol He, Yanqing; Zhang, Longping; Zhang, Jian Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-1	journal	January 2014
A highly efficient dilute alkali deacetylation and mechanical (disc) refining process for the conversion of renewable biomass to lower cost sugars Chen, Xiaowen; Shekiro, Joseph; Pschorn, Thomas Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-98	journal	January 2014
Optimization of Pilot Scale Mechanical Disk Refining for Improvements in Enzymatic Digestibility of Pretreated Hardwood Lignocellulosics Jones, Brandon W.; Venditti, Richard; Park, Sunkyu BioResources, Vol. 12, Issue 3 https://doi.org/10.15376/biores.12.3.4567-4593	journal	May 2017
Process Design and Economics for Biochemical Conversion of Lignocellulosic Biomass to Ethanol: Dilute-Acid Pretreatment and Enzymatic Hydrolysis of Corn Stover Humbird, D.; Davis, R.; Tao, L. https://doi.org/10.2172/1013269	report	March 2011

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Fiber fractionation to understand the effect of mechanical refining on fiber structure and resulting enzymatic digestibility of biomass Corbett, Derek B.; Knoll, Charlie; Venditti, Richard Biotechnology and Bioengineering, Vol. 117, Issue 4 https://doi.org/10.1002/bit.27258	journal	January 2020
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