Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods

Namita Bansal, Aditya Bhalla, Sivakumar Pattathil, Sara L. Adelman, Michael G. Hahn, David B. Hodge, Eric L. Hegg

    Research output: Research - peer-reviewArticle

    • 1 Citations

    Abstract

    The responses of four diverse hardwoods (hybrid poplar, silver birch, hybrid aspen, and sugar maple) to alkaline hydrogen peroxide (AHP) pretreated at ambient temperature and pressure were analyzed to gain a deeper understanding of the cell wall properties that contribute to differences in enzymatic hydrolysis efficacy following alkaline-oxidative pretreatment. The enzymatic hydrolysis yields of these diverse hardwoods increased significantly with increasing the cell wall-associated, redox-active transition metal content. These increases in hydrolysis yields were directly correlated with improved delignification. Furthermore, we demonstrated that these improvements in hydrolysis yields could be achieved either through elevated levels of naturally-occurring metals, namely Cu, Fe, and Mn, or by the addition of a homogeneous transition metal catalyst (e.g. Cu 2,2′-bipyridine complexes) capable of penetrating into the cell wall matrix. Removal of naturally-occurring cell wall-associated transition metals by chelation resulted in substantial decreases in the hydrolysis yields following AHP pretreatment, while re-addition of metals in the form of Cu 2,2′-bipyridine complexes and to a limited extent Fe 2,2′-bipyridine complexes prior to pretreatment restored the improved hydrolysis yields. Glycome profiles showed improved extractability of xylan, xyloglucan, and pectin epitopes with increasing hydrolysis yields for the diverse hardwoods subjected to the alkaline-oxidative pretreatment, demonstrating that the strength of association between cell wall matrix polymers decreased as a consequence of improved delignification.

    LanguageEnglish (US)
    Pages1405-1415
    Number of pages11
    JournalGreen Chemistry
    Volume18
    Issue number5
    DOIs
    StatePublished - 2016

    Profile

    Hardwoods
    Transition metals
    Hydrolysis
    Cells
    transition element
    hydrolysis
    2,2'-Dipyridyl
    Delignification
    Enzymatic hydrolysis
    Hydrogen Peroxide
    Metals
    Hydrogen peroxide
    hydrogen peroxide
    matrix
    metal
    Xylans
    Chelation
    Polymer matrix
    Silver
    Sugars

    ASJC Scopus subject areas

    • Environmental Chemistry
    • Pollution

    Cite this

    Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods. / Bansal, Namita; Bhalla, Aditya; Pattathil, Sivakumar; Adelman, Sara L.; Hahn, Michael G.; Hodge, David B.; Hegg, Eric L.

    In: Green Chemistry, Vol. 18, No. 5, 2016, p. 1405-1415.

    Research output: Research - peer-reviewArticle

    Bansal, N, Bhalla, A, Pattathil, S, Adelman, SL, Hahn, MG, Hodge, DB & Hegg, EL 2016, 'Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods' Green Chemistry, vol 18, no. 5, pp. 1405-1415. DOI: 10.1039/c5gc01748c
    Bansal N, Bhalla A, Pattathil S, Adelman SL, Hahn MG, Hodge DB et al. Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods. Green Chemistry. 2016;18(5):1405-1415. Available from, DOI: 10.1039/c5gc01748c
    Bansal, Namita ; Bhalla, Aditya ; Pattathil, Sivakumar ; Adelman, Sara L. ; Hahn, Michael G. ; Hodge, David B. ; Hegg, Eric L./ Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods. In: Green Chemistry. 2016 ; Vol. 18, No. 5. pp. 1405-1415
    @article{6c38a42c687f486a9732bc2518238739,
    title = "Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods",
    abstract = "The responses of four diverse hardwoods (hybrid poplar, silver birch, hybrid aspen, and sugar maple) to alkaline hydrogen peroxide (AHP) pretreated at ambient temperature and pressure were analyzed to gain a deeper understanding of the cell wall properties that contribute to differences in enzymatic hydrolysis efficacy following alkaline-oxidative pretreatment. The enzymatic hydrolysis yields of these diverse hardwoods increased significantly with increasing the cell wall-associated, redox-active transition metal content. These increases in hydrolysis yields were directly correlated with improved delignification. Furthermore, we demonstrated that these improvements in hydrolysis yields could be achieved either through elevated levels of naturally-occurring metals, namely Cu, Fe, and Mn, or by the addition of a homogeneous transition metal catalyst (e.g. Cu 2,2′-bipyridine complexes) capable of penetrating into the cell wall matrix. Removal of naturally-occurring cell wall-associated transition metals by chelation resulted in substantial decreases in the hydrolysis yields following AHP pretreatment, while re-addition of metals in the form of Cu 2,2′-bipyridine complexes and to a limited extent Fe 2,2′-bipyridine complexes prior to pretreatment restored the improved hydrolysis yields. Glycome profiles showed improved extractability of xylan, xyloglucan, and pectin epitopes with increasing hydrolysis yields for the diverse hardwoods subjected to the alkaline-oxidative pretreatment, demonstrating that the strength of association between cell wall matrix polymers decreased as a consequence of improved delignification.",
    author = "Namita Bansal and Aditya Bhalla and Sivakumar Pattathil and Adelman, {Sara L.} and Hahn, {Michael G.} and Hodge, {David B.} and Hegg, {Eric L.}",
    year = "2016",
    doi = "10.1039/c5gc01748c",
    volume = "18",
    pages = "1405--1415",
    journal = "Green Chemistry",
    issn = "1463-9262",
    publisher = "Royal Society of Chemistry",
    number = "5",

    }

    TY - JOUR

    T1 - Cell wall-associated transition metals improve alkaline-oxidative pretreatment in diverse hardwoods

    AU - Bansal,Namita

    AU - Bhalla,Aditya

    AU - Pattathil,Sivakumar

    AU - Adelman,Sara L.

    AU - Hahn,Michael G.

    AU - Hodge,David B.

    AU - Hegg,Eric L.

    PY - 2016

    Y1 - 2016

    N2 - The responses of four diverse hardwoods (hybrid poplar, silver birch, hybrid aspen, and sugar maple) to alkaline hydrogen peroxide (AHP) pretreated at ambient temperature and pressure were analyzed to gain a deeper understanding of the cell wall properties that contribute to differences in enzymatic hydrolysis efficacy following alkaline-oxidative pretreatment. The enzymatic hydrolysis yields of these diverse hardwoods increased significantly with increasing the cell wall-associated, redox-active transition metal content. These increases in hydrolysis yields were directly correlated with improved delignification. Furthermore, we demonstrated that these improvements in hydrolysis yields could be achieved either through elevated levels of naturally-occurring metals, namely Cu, Fe, and Mn, or by the addition of a homogeneous transition metal catalyst (e.g. Cu 2,2′-bipyridine complexes) capable of penetrating into the cell wall matrix. Removal of naturally-occurring cell wall-associated transition metals by chelation resulted in substantial decreases in the hydrolysis yields following AHP pretreatment, while re-addition of metals in the form of Cu 2,2′-bipyridine complexes and to a limited extent Fe 2,2′-bipyridine complexes prior to pretreatment restored the improved hydrolysis yields. Glycome profiles showed improved extractability of xylan, xyloglucan, and pectin epitopes with increasing hydrolysis yields for the diverse hardwoods subjected to the alkaline-oxidative pretreatment, demonstrating that the strength of association between cell wall matrix polymers decreased as a consequence of improved delignification.

    AB - The responses of four diverse hardwoods (hybrid poplar, silver birch, hybrid aspen, and sugar maple) to alkaline hydrogen peroxide (AHP) pretreated at ambient temperature and pressure were analyzed to gain a deeper understanding of the cell wall properties that contribute to differences in enzymatic hydrolysis efficacy following alkaline-oxidative pretreatment. The enzymatic hydrolysis yields of these diverse hardwoods increased significantly with increasing the cell wall-associated, redox-active transition metal content. These increases in hydrolysis yields were directly correlated with improved delignification. Furthermore, we demonstrated that these improvements in hydrolysis yields could be achieved either through elevated levels of naturally-occurring metals, namely Cu, Fe, and Mn, or by the addition of a homogeneous transition metal catalyst (e.g. Cu 2,2′-bipyridine complexes) capable of penetrating into the cell wall matrix. Removal of naturally-occurring cell wall-associated transition metals by chelation resulted in substantial decreases in the hydrolysis yields following AHP pretreatment, while re-addition of metals in the form of Cu 2,2′-bipyridine complexes and to a limited extent Fe 2,2′-bipyridine complexes prior to pretreatment restored the improved hydrolysis yields. Glycome profiles showed improved extractability of xylan, xyloglucan, and pectin epitopes with increasing hydrolysis yields for the diverse hardwoods subjected to the alkaline-oxidative pretreatment, demonstrating that the strength of association between cell wall matrix polymers decreased as a consequence of improved delignification.

    UR - http://www.scopus.com/inward/record.url?scp=84959304247&partnerID=8YFLogxK

    UR - http://www.scopus.com/inward/citedby.url?scp=84959304247&partnerID=8YFLogxK

    U2 - 10.1039/c5gc01748c

    DO - 10.1039/c5gc01748c

    M3 - Article

    VL - 18

    SP - 1405

    EP - 1415

    JO - Green Chemistry

    T2 - Green Chemistry

    JF - Green Chemistry

    SN - 1463-9262

    IS - 5

    ER -