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Title: Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA)

Sustainable biorefinery heavily depends on the generation of value-added products, particularly from lignin. Despite considerable efforts, the production of fungible lignin bioproducts is still hindered by the poor fractionation and low reactivity of lignin. To address these challenges, the sequential organosolv fragmentation approach (SOFA) using ethanol plus different-stage catalysts was explored to selectively dissolve lignin for producing multiple uniform lignin streams, and to tailor its chemistry and reactivity for fabricating lignin nanoparticles (LNPs) with desired quality features. In a biorefinery concept, the carbohydrate output is taken into consideration. SOFA significantly increased the glucose and xylose yields, suggesting an improved monomer-sugar release. The fractionated lignin was used to fabricate LNPs via self-assembly. Although these LNPs were derived from the same substrate, they exhibited different properties. The effective diameter almost followed the order of stage 1, stage 3, and stage 2 in each SOFA, and the smallest effective diameter was approximately 130 nm from SOFA using ethanol plus sulfuric acid. The polydispersity index and zeta potential were less than 0.08 and –50 mV, respectively, suggesting good uniformity and stability of the LNPs. Lignin characterization results suggested that SOFA using ethanol plus sulfuric acid produced high-molecular-weight lignin, decreased S/G ratio, and β-O-4 andmore » β–β linkage abundance, yet produced the condensed lignin and enhanced its hydrophobicity. More importantly, it exposed more phenolic OH groups and enhanced the stability of LNPs, likely due to the hydrogen bond networks. Together with enriched COOH groups, it promoted the formation of electrical double layers and increased the zeta potential of LNPs. In conclusion, by tailoring the lignin chemistry using SOFA to enhance the self-assembling process, high-quality LNPs of a spherical shape, small effective diameters, and good stability have been fabricated, which represents a sustainable means for upgrading the low-value lignin and thus contributes to the profitability of biorefineries.« less
Authors:
 [1] ;  [2] ; ORCiD logo [2] ; ORCiD logo [3] ;  [4] ; ORCiD logo [5] ; ORCiD logo [1]
  1. Texas A & M Univ., College Station, TX (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Texas A & M Univ., College Station, TX (United States); Northwest Univ. (People's Republic of China)
  5. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725; EE0006112; EE0007104; EE0008250
Type:
Accepted Manuscript
Journal Name:
Green Chemistry
Additional Journal Information:
Journal Name: Green Chemistry; Journal ID: ISSN 1463-9262
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1489102
Alternate Identifier(s):
OSTI ID: 1483017

Liu, Zhi -Hua, Hao, Naijia, Shinde, Somnath, Pu, Yunqiao Joseph, Kang, Xiaofeng, Ragauskas, Arthur J., and Yuan, Joshua S.. Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA). United States: N. p., Web. doi:10.1039/c8gc03290d.
Liu, Zhi -Hua, Hao, Naijia, Shinde, Somnath, Pu, Yunqiao Joseph, Kang, Xiaofeng, Ragauskas, Arthur J., & Yuan, Joshua S.. Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA). United States. doi:10.1039/c8gc03290d.
Liu, Zhi -Hua, Hao, Naijia, Shinde, Somnath, Pu, Yunqiao Joseph, Kang, Xiaofeng, Ragauskas, Arthur J., and Yuan, Joshua S.. 2018. "Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA)". United States. doi:10.1039/c8gc03290d.
@article{osti_1489102,
title = {Defining lignin nanoparticle properties through tailored lignin reactivity by sequential organosolv fragmentation approach (SOFA)},
author = {Liu, Zhi -Hua and Hao, Naijia and Shinde, Somnath and Pu, Yunqiao Joseph and Kang, Xiaofeng and Ragauskas, Arthur J. and Yuan, Joshua S.},
abstractNote = {Sustainable biorefinery heavily depends on the generation of value-added products, particularly from lignin. Despite considerable efforts, the production of fungible lignin bioproducts is still hindered by the poor fractionation and low reactivity of lignin. To address these challenges, the sequential organosolv fragmentation approach (SOFA) using ethanol plus different-stage catalysts was explored to selectively dissolve lignin for producing multiple uniform lignin streams, and to tailor its chemistry and reactivity for fabricating lignin nanoparticles (LNPs) with desired quality features. In a biorefinery concept, the carbohydrate output is taken into consideration. SOFA significantly increased the glucose and xylose yields, suggesting an improved monomer-sugar release. The fractionated lignin was used to fabricate LNPs via self-assembly. Although these LNPs were derived from the same substrate, they exhibited different properties. The effective diameter almost followed the order of stage 1, stage 3, and stage 2 in each SOFA, and the smallest effective diameter was approximately 130 nm from SOFA using ethanol plus sulfuric acid. The polydispersity index and zeta potential were less than 0.08 and –50 mV, respectively, suggesting good uniformity and stability of the LNPs. Lignin characterization results suggested that SOFA using ethanol plus sulfuric acid produced high-molecular-weight lignin, decreased S/G ratio, and β-O-4 and β–β linkage abundance, yet produced the condensed lignin and enhanced its hydrophobicity. More importantly, it exposed more phenolic OH groups and enhanced the stability of LNPs, likely due to the hydrogen bond networks. Together with enriched COOH groups, it promoted the formation of electrical double layers and increased the zeta potential of LNPs. In conclusion, by tailoring the lignin chemistry using SOFA to enhance the self-assembling process, high-quality LNPs of a spherical shape, small effective diameters, and good stability have been fabricated, which represents a sustainable means for upgrading the low-value lignin and thus contributes to the profitability of biorefineries.},
doi = {10.1039/c8gc03290d},
journal = {Green Chemistry},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {11}
}

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