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Title: Rapid and near-complete dissolution of wood lignin at ≤80°C by a recyclable acid hydrotrope

Journal Article · · Science Advances
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [2]; ORCiD logo [8]; ORCiD logo [4]; ORCiD logo [9]
  1. Jinan Univ., (China). Key Lab. of Biomaterials of Guangdong Higher Education Inst., Dept. of Biomedical Engineering; US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.
  2. Aalto Univ., Espoo (Finland). School of Chemical Engineering, Dept. of Bioproducts and Biosystems
  3. US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.; South China Univ. of Technology (SCUT), Guangzhou (China). State Key Lab. of Pulp and Paper Engineering
  4. Univ. of Wisconsin, Madison, WI (United States). Dept. of Biological Systems Engineering
  5. US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.; Guangxi Univ. for Nationalities, Nanning (China). School of Chemistry and Chemical Engineering
  6. US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.; Nanjing Forestry Univ. (China). Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources
  7. US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.
  8. South China Univ. of Technology (SCUT), Guangzhou (China). State Key Lab. of Pulp and Paper Engineering
  9. US Dept. of Agriculture (USDA)., Madison, WI (United States), Forest Service, Forest Products Lab.; Univ. of Wisconsin, Madison, WI (United States). Dept. of Biological Systems Engineering

We report the discovery of the hydrotropic properties of a recyclable aromatic acid, p-toluenesulfonic acid (p-TsOH), for potentially low-cost and efficient fractionation of wood through rapid and near-complete dissolution of lignin. Approximately 90% of poplar wood (NE222) lignin can be dissolved at 80°C in 20 min. Equivalent delignification using known hydrotropes, such as aromatic salts, can be achieved only at 150°C or higher for more than 10 hours or at 150°C for 2 hours with alkaline pulping. p-TsOH fractionated wood into two fractions: (i) a primarily celluloserich water-insoluble solid fraction that can be used for the production of high-value building blocks, such as dissolving pulp fibers, lignocellulosic nanomaterials, and/or sugars through subsequent enzymatic hydrolysis; and (ii) a spent acid liquor stream containing mainly dissolved lignin that can be easily precipitated as lignin nanoparticles by diluting the spent acid liquor to below the minimal hydrotrope concentration. Our nuclear magnetic resonance analyses of the dissolved lignin revealed that p-TsOH can depolymerize lignin via ether bond cleavage and can separate carbohydrate-free lignin from the wood. p-TsOH has a relatively low water solubility, which can facilitate efficient recovery using commercially proven crystallization technology by cooling the concentrated spent acid solution to ambient temperatures to achieve environmental sustainability through recycling of p-TsOH.

Research Organization:
USDOE Bioenergy Research Centers (BRC) (United States). Great Lakes Bioenergy Research Center (GLBRC); Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER). Biological Systems Science Division; USDA; Chinese State Forestry Administration; Finnish Cultural Foundation; Chinese Scholarship Council (CSC)
Grant/Contract Number:
SC0018409; 2011-67009-20056
OSTI ID:
1625976
Journal Information:
Science Advances, Vol. 3, Issue 9; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 149 works
Citation information provided by
Web of Science

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A Highly Conductive Cationic Wood Membrane journal August 2019
High Purity and Low Molecular Weight Lignin Nano-Particles Extracted from Acid-Assisted MIBK Pretreatment journal February 2020
Integrating Benzenesulfonic Acid Pretreatment and Bio-Based Lignin-Shielding Agent for Robust Enzymatic Conversion of Cellulose in Bamboo journal January 2020
Multiple hydrogen bond coordination in three-constituent deep eutectic solvents enhances lignin fractionation from biomass journal January 2018
Characterization of Lignin Extracted from Willow by Deep Eutectic Solvent Treatments journal August 2018
Development of anti-photo and anti-thermal high internal phase emulsions stabilized by biomass lignin as a nutraceutical delivery system journal January 2019
Direct transformation of lignin into fluorescence-switchable graphene quantum dots and their application in ultrasensitive profiling of a physiological oxidant journal January 2019
Lignin Nanoparticle-Coated Celgard Separator for High-Performance Lithium–Sulfur Batteries journal November 2019
Valorization of Alkaline Peroxide Mechanical Pulp by Metal Chloride-Assisted Hydrotropic Pretreatment for Enzymatic Saccharification and Cellulose Nanofibrillation journal February 2019
Mechanistic insights into the lignin dissolution behaviors of a recyclable acid hydrotrope, deep eutectic solvent (DES), and ionic liquid (IL) journal January 2020
Closed cycle production of concentrated and dry redispersible colloidal lignin particles with a three solvent polarity exchange method journal January 2018
Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA) journal January 2019
Comparing a deep eutectic solvent (DES) to a hydrotrope for their ability to enhance the fractionation and enzymatic hydrolysis of willow and corn stover journal January 2019
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