Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar

Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Ausführliche Beschreibung

Gespeichert in:

Autor*in:	Li, Zhenglun [verfasserIn] Bansal, Namita Azarpira, Ali Bhalla, Aditya Chen, Charles H Ralph, John Hegg, Eric L Hodge, David B

Format:	E-Artikel
Sprache:	Englisch

Erschienen:	2015

Schlagwörter:	Plant cell walls Pretreatment Catalytic oxidation Lignin Alkaline hydrogen peroxide (AHP) pretreatment NMR spectroscopy Electron microscopy

Anmerkung:	© Li et al. 2015

Übergeordnetes Werk:	Enthalten in: Biotechnology for biofuels - London : BioMed Central, 2008, 8(2015), 1 vom: 20. Aug.
Übergeordnetes Werk:	volume:8 ; year:2015 ; number:1 ; day:20 ; month:08

Links:	Volltext

DOI / URN:	10.1186/s13068-015-0300-5

Katalog-ID:	SPR030147220

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520			\|a Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization.
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allfields	10.1186/s13068-015-0300-5 doi (DE-627)SPR030147220 (SPR)s13068-015-0300-5-e DE-627 ger DE-627 rakwb eng Li, Zhenglun verfasserin aut Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar 2015 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Li et al. 2015 Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213 Bansal, Namita aut Azarpira, Ali aut Bhalla, Aditya aut Chen, Charles H aut Ralph, John aut Hegg, Eric L aut Hodge, David B aut Enthalten in Biotechnology for biofuels London : BioMed Central, 2008 8(2015), 1 vom: 20. Aug. (DE-627)563167882 (DE-600)2421351-2 1754-6834 nnns volume:8 year:2015 number:1 day:20 month:08 https://dx.doi.org/10.1186/s13068-015-0300-5 kostenfrei Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2003 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2027 GBV_ILN_2055 GBV_ILN_2108 GBV_ILN_2111 GBV_ILN_2119 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 8 2015 1 20 08
spelling	10.1186/s13068-015-0300-5 doi (DE-627)SPR030147220 (SPR)s13068-015-0300-5-e DE-627 ger DE-627 rakwb eng Li, Zhenglun verfasserin aut Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar 2015 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Li et al. 2015 Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213 Bansal, Namita aut Azarpira, Ali aut Bhalla, Aditya aut Chen, Charles H aut Ralph, John aut Hegg, Eric L aut Hodge, David B aut Enthalten in Biotechnology for biofuels London : BioMed Central, 2008 8(2015), 1 vom: 20. Aug. (DE-627)563167882 (DE-600)2421351-2 1754-6834 nnns volume:8 year:2015 number:1 day:20 month:08 https://dx.doi.org/10.1186/s13068-015-0300-5 kostenfrei Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2003 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2027 GBV_ILN_2055 GBV_ILN_2108 GBV_ILN_2111 GBV_ILN_2119 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 8 2015 1 20 08
allfields_unstemmed	10.1186/s13068-015-0300-5 doi (DE-627)SPR030147220 (SPR)s13068-015-0300-5-e DE-627 ger DE-627 rakwb eng Li, Zhenglun verfasserin aut Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar 2015 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Li et al. 2015 Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213 Bansal, Namita aut Azarpira, Ali aut Bhalla, Aditya aut Chen, Charles H aut Ralph, John aut Hegg, Eric L aut Hodge, David B aut Enthalten in Biotechnology for biofuels London : BioMed Central, 2008 8(2015), 1 vom: 20. Aug. (DE-627)563167882 (DE-600)2421351-2 1754-6834 nnns volume:8 year:2015 number:1 day:20 month:08 https://dx.doi.org/10.1186/s13068-015-0300-5 kostenfrei Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2003 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2027 GBV_ILN_2055 GBV_ILN_2108 GBV_ILN_2111 GBV_ILN_2119 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 8 2015 1 20 08
allfieldsGer	10.1186/s13068-015-0300-5 doi (DE-627)SPR030147220 (SPR)s13068-015-0300-5-e DE-627 ger DE-627 rakwb eng Li, Zhenglun verfasserin aut Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar 2015 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Li et al. 2015 Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213 Bansal, Namita aut Azarpira, Ali aut Bhalla, Aditya aut Chen, Charles H aut Ralph, John aut Hegg, Eric L aut Hodge, David B aut Enthalten in Biotechnology for biofuels London : BioMed Central, 2008 8(2015), 1 vom: 20. Aug. (DE-627)563167882 (DE-600)2421351-2 1754-6834 nnns volume:8 year:2015 number:1 day:20 month:08 https://dx.doi.org/10.1186/s13068-015-0300-5 kostenfrei Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2003 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2027 GBV_ILN_2055 GBV_ILN_2108 GBV_ILN_2111 GBV_ILN_2119 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 8 2015 1 20 08
allfieldsSound	10.1186/s13068-015-0300-5 doi (DE-627)SPR030147220 (SPR)s13068-015-0300-5-e DE-627 ger DE-627 rakwb eng Li, Zhenglun verfasserin aut Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar 2015 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Li et al. 2015 Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213 Bansal, Namita aut Azarpira, Ali aut Bhalla, Aditya aut Chen, Charles H aut Ralph, John aut Hegg, Eric L aut Hodge, David B aut Enthalten in Biotechnology for biofuels London : BioMed Central, 2008 8(2015), 1 vom: 20. Aug. (DE-627)563167882 (DE-600)2421351-2 1754-6834 nnns volume:8 year:2015 number:1 day:20 month:08 https://dx.doi.org/10.1186/s13068-015-0300-5 kostenfrei Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2003 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2027 GBV_ILN_2055 GBV_ILN_2108 GBV_ILN_2111 GBV_ILN_2119 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4335 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 8 2015 1 20 08
language	English
source	Enthalten in Biotechnology for biofuels 8(2015), 1 vom: 20. Aug. volume:8 year:2015 number:1 day:20 month:08
sourceStr	Enthalten in Biotechnology for biofuels 8(2015), 1 vom: 20. Aug. volume:8 year:2015 number:1 day:20 month:08
format_phy_str_mv	Article
institution	findex.gbv.de
topic_facet	Plant cell walls Pretreatment Catalytic oxidation Lignin Alkaline hydrogen peroxide (AHP) pretreatment NMR spectroscopy Electron microscopy
isfreeaccess_bool	true
container_title	Biotechnology for biofuels
authorswithroles_txt_mv	Li, Zhenglun @@aut@@ Bansal, Namita @@aut@@ Azarpira, Ali @@aut@@ Bhalla, Aditya @@aut@@ Chen, Charles H @@aut@@ Ralph, John @@aut@@ Hegg, Eric L @@aut@@ Hodge, David B @@aut@@
publishDateDaySort_date	2015-08-20T00:00:00Z
hierarchy_top_id	563167882
id	SPR030147220
language_de	englisch
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In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. 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author	Li, Zhenglun
spellingShingle	Li, Zhenglun misc Plant cell walls misc Pretreatment misc Catalytic oxidation misc Lignin misc Alkaline hydrogen peroxide (AHP) pretreatment misc NMR spectroscopy misc Electron microscopy Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar
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topic_title	Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar Plant cell walls (dpeaa)DE-He213 Pretreatment (dpeaa)DE-He213 Catalytic oxidation (dpeaa)DE-He213 Lignin (dpeaa)DE-He213 Alkaline hydrogen peroxide (AHP) pretreatment (dpeaa)DE-He213 NMR spectroscopy (dpeaa)DE-He213 Electron microscopy (dpeaa)DE-He213
topic	misc Plant cell walls misc Pretreatment misc Catalytic oxidation misc Lignin misc Alkaline hydrogen peroxide (AHP) pretreatment misc NMR spectroscopy misc Electron microscopy
topic_unstemmed	misc Plant cell walls misc Pretreatment misc Catalytic oxidation misc Lignin misc Alkaline hydrogen peroxide (AHP) pretreatment misc NMR spectroscopy misc Electron microscopy
topic_browse	misc Plant cell walls misc Pretreatment misc Catalytic oxidation misc Lignin misc Alkaline hydrogen peroxide (AHP) pretreatment misc NMR spectroscopy misc Electron microscopy
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title	Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar
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title_full	Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar
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author_browse	Li, Zhenglun Bansal, Namita Azarpira, Ali Bhalla, Aditya Chen, Charles H Ralph, John Hegg, Eric L Hodge, David B
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doi_str_mv	10.1186/s13068-015-0300-5
title_sort	chemical and structural changes associated with cu-catalyzed alkaline-oxidative delignification of hybrid poplar
title_auth	Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar
abstract	Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. © Li et al. 2015
abstractGer	Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. © Li et al. 2015
abstract_unstemmed	Background Alkaline hydrogen peroxide pretreatment catalyzed by Cu(II) 2,2′-bipyridine complexes has previously been determined to substantially improve the enzymatic hydrolysis of woody plants including hybrid poplar as a consequence of moderate delignification. In the present work, cell wall morphological and lignin structural changes were characterized for this pretreatment approach to gain insights into pretreatment outcomes and, specifically, to identify the extent and nature of lignin modification. Results Through TEM imaging, this catalytic oxidation process was shown to disrupt cell wall layers in hybrid poplar. Cu-containing nanoparticles, primarily in the Cu(I) oxidation state, co-localized with the disrupted regions, providing indirect evidence of catalytic activity whereby soluble Cu(II) complexes are reduced and precipitated during pretreatment. The concentration of alkali-soluble polymeric and oligomeric lignin was substantially higher for the Cu-catalyzed oxidative pretreatment. This alkali-soluble lignin content increased with time during the catalytic oxidation process, although the molecular weight distributions were unaltered. Yields of aromatic monomers (including phenolic acids and aldehydes) were found to be less than 0.2 % (wt/wt) on lignin. Oxidation of the benzylic alcohol in the lignin side-chain was evident in NMR spectra of the solubilized lignin, whereas minimal changes were observed for the pretreatment-insoluble lignin. Conclusions These results provide indirect evidence for catalytic activity within the cell wall. The low yields of lignin-derived aromatic monomers, together with the detailed characterization of the pretreatment-soluble and pretreatment-insoluble lignins, indicate that the majority of both lignin pools remained relatively unmodified. As such, the lignins resulting from this process retain features closely resembling native lignins and may, therefore, be amenable to subsequent valorization. © Li et al. 2015
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title_short	Chemical and structural changes associated with Cu-catalyzed alkaline-oxidative delignification of hybrid poplar
url	https://dx.doi.org/10.1186/s13068-015-0300-5
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author2	Bansal, Namita Azarpira, Ali Bhalla, Aditya Chen, Charles H Ralph, John Hegg, Eric L Hodge, David B
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