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

Liu, Zhi -Hua; Hao, Naijia; Shinde, Somnath; Pu, Yunqiao Joseph; Kang, Xiaofeng; Ragauskas, Arthur J.; Yuan, Joshua S.

doi:10.1039/c8gc03290d

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

Journal Article · 15 November 2018 · Green Chemistry

DOI: https://doi.org/10.1039/c8gc03290d · OSTI ID:1489102

Liu, Zhi -Hua ^[1]; Hao, Naijia ^[2];

^[2];

^[3]; Kang, Xiaofeng ^[4];

^[5];

^[1]

Texas A & M Univ., College Station, TX (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Texas A & M Univ., College Station, TX (United States); Northwest Univ. (People's Republic of China)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-00OR22725; EE0006112; EE0007104; EE0008250

OSTI ID:: 1489102

Alternate ID(s):: OSTI ID: 1483017

Journal Information:: Green Chemistry, Vol. 21, Issue 2; ISSN 1463-9262

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 79 works

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