Isolation and modification of nano-scale cellulose from organosolv-treated birch through the synergistic activity of LPMO and endoglucanases

Muraleedharan, Madhu Nair; Karnaouri, Anthi; Piatkova, Mariia; Ruiz-Caldas, Maria-Ximena; Μάτσακας, Λεωνίδας; Liu, Bing; Christakopoulos, Paul; Mathew, Aji P.

doi:10.1016/j.ijbiomac.2021.04.136

Cited by 17 publications

(20 citation statements)

References 46 publications

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“…Here we have optimized a chemo-enzymatic method, based on the unique activity of C1-oxidising LPMOs, to activate cellulose surfaces for further functionalisation. Our study builds upon significant efforts on the kinetic and mechanistic characterisation of LPMOs, 51 recent examples of the use of cellulolytic LPMOs for nanocellulose production, [59][60][61][62][63][64][65] and the development of LPMO assays based on surface carboxylation. 66,92,93 In particular, seminal work by Hsieh and colleagues specifically demonstrated the potential of a chitinolytic LPMO for the chemo-enzymatic functionalisation of insoluble chitin.…”

Section: Discussionmentioning

confidence: 99%

“…52–58 On the other hand, recent research has demonstrated that the ability of LPMOs to disrupt fibre structure under controlled conditions can be used to generate oxidised nanofibrils for materials applications. 59–65 These latter studies exemplify the use of LPMOs to modify the bulk properties of cellulosic materials. However, the potential of LPMOs to surgically introduce carboxylic acid groups on the cellulose surface for subsequent chemical functionalization is relatively unexplored.…”

Section: Introductionmentioning

confidence: 95%

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Oxidative enzyme activation of cellulose substrates for surface modification

Solhi

et al. 2022

Green Chem.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 95%

Oxidative enzyme activation of cellulose substrates for surface modification

Solhi

et al. 2022

Green Chem.

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“…Among the numerous women working on this topic, Kristiina Oksman (Luleå University of Technology, Sweden), Aji Mathew (Stockholm University, Sweden), and Arantxa Eceiza (University of Basque Country, Spain) have achieved significant progresses on nanocellulose. These include: (i) the isolation of nanocellulose (nanofibers, nanocrystals, or whiskers) from different origins and sources such as microcrystalline cellulose from Norway spruce, kenaf fibers, beech pulp, and unbleached rice straw among others by using different isolation approaches, namely, chemical hydrolysis or physical or mechanical isolation methods such as refining, high-pressure homogenization and ultrafine grinder and their characterization [ 88 , 89 , 90 , 91 ]; (ii) the processing of functional materials such as nanocomposites with interesting mechanical properties [ 92 , 93 , 94 ], hydrogels, aerogels [ 95 ], and membranes for several applications [ 96 , 97 ]; and (iii) the cellulose-based material development for biomedical applications; for example, as scaffolds [ 83 , 98 , 99 ].…”

Section: Advances In Biopolymer Research: Examples From Well-known Bi...mentioning

confidence: 99%

Contributions of Women in Recent Research on Biopolymer Science

et al. 2022

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Nowadays, biopolymers are playing a fundamental role in our society because of the environmental issues and concerns associated with synthetic polymers. The aim of this Special Issue entitled ‘Women in Polymer Science and Technology: Biopolymers’ is highlighting the work designed and developed by women on biopolymer science and technology. In this context, this short review aims to provide an introduction to this Special Issue by highlighting some recent contributions of women around the world on the particular topic of biopolymer science and technology during the last 20 years. In the first place, it highlights a selection of important works performed on a number of well-studied natural polymers, namely, agar, chitin, chitosan, cellulose, and collagen. Secondly, it gives an insight into the discovery of new polysaccharides and enzymes that have a role in their synthesis and in their degradation. These contributions will be paving the way for the next generation of female and male scientists on this topic.

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“…In AA9, AA11, AA13 and AA14 LPMOs, the third amino acid is a tyrosine, while a phenylalanine is found in AA10 (90% conserved) and chitin-specific AA15 LPMOs (149,150,154). This structural coordination is recognized as a histidine-brace motif, which is conserved in all LPMOs to date (145,154,158,159). The histidine-brace motif has been shown to be key for the LPMO catalytic reaction.…”

Section: Conserved Mono-copper Active Site and Unique "Histidine-brac...mentioning

confidence: 99%

“…In addition to lignocellulose degradation, LPMOs have been used to assist the production of functional materials and compounds. Several studies have investigated the LPMO-assisted production of nanocellulose (152)(153)(154)(155)(156)(157)(158)(159)(160)(161), which is a valuable material used as emulsion stabilizer and gas barrier, also even in food industry (162-165).…”

Section: Lpmo-assisted Nanocellulose Productionmentioning

confidence: 99%

High resolution product profiling of lytic polysaccharide monooxygenases

Sun¹

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Biorefinery of non-food lignocellulosic plant biomass to be valorized as biofuels, biochemicals and biomaterials is considered as a sustainable alternative for fossil resource-based production. In biorefinery, a key step is enzymatic degradation of plant cell wall polysaccharides into (fermentable) monomeric building blocks, which is typically driven by (hemi-)cellulases and essential lytic polysaccharide monooxygenases (LPMOs). Although some LPMOs have already been incorporated into industrial enzyme cocktails, only a limited number of LPMOs have been biochemically characterized. Therefore, this PhD thesis aimed to further shed light on the mode-ofaction, regioselectivity, substrate cleavage profiles and specificity of AA9 LPMOs from the fungi Myceliophthora thermophila C1 (MtLPMOs) and Neurospora crassa (NcLPMOs).We demonstrated that AA9 LPMOs show distinct cleavage profiles towards different types of cellulose; from bacterial cellulose mainly oxidized DP2-4 products were generated, while from the regenerated amorphous cellulose larger oxidized products prevailed. We developed a new method, making use of NaBD4-reduction in combination with hydrophilic interaction chromatography-mass spectrometric analysis, for separation and identification of LPMO-generated non-, C1-and C4-oxidized oligosaccharides. We found that oxidized (and reduced) oligosaccharides differ in their mass spectrometric fragmentation behaviors and patterns. Using this developed methodology, we discovered a series of novel double, C4 and C6, oxidized cellooligosaccharides. Again using this methodology, we identified and distinguished for the first time (isomeric) LPMO-oxidized xylogluco-oligosaccharides, and characterized two distinct oxidative xyloglucan degradation profiles. These xyloglucan substitution tolerant and intolerant cleavage profiles were correlated to specific active site segment configurations of AA9 LPMOs. Additionally, the active site segment configuration predicted for two (other) MtLPMOs, confirmed the aforementioned correlation with their xyloglucan substitution (in)tolerant cleavage profiles. Lastly, we studied two novel AA16 copper-dependent oxidoreductases, which were predicted to function as LPMOs. We showed their inactivity towards carbohydrate substrates, hence, disproved them being LPMOs, but we discovered that these AA16s can boost AA9 MtLPMOs to oxidatively degrade cellulose. Table of contents Chapter 1 General introduction Chapter 2 Oxidized product profiles of AA9 lytic polysaccharide monooxygenases depend on the type of cellulose Chapter 3 Mass spectrometric fragmentation patterns discriminate C1-and C4-oxidized cellooligosaccharides from their non-oxidized and reduced forms Chapter 4 Regioselectivity Substrate specificity MtLPMO9A 1 M. thermophila C1 No C1/C4 Cellulose (RAC), xylan associated to cellulose, xyloglucan 10 , mixed β-(1→3, 1→4)-linked glucan 10 MtLPMO9B 2 M. thermophila C1 CBM1 C1 Cellulose (RAC) MtLPMO9C 3 M. thermophila C1 No C4 Cellulose (RAC), xyloglucan 10 , mixed β-(1→3, 1→4)-linked glucan 10 ...

show abstract

Isolation and modification of nano-scale cellulose from organosolv-treated birch through the synergistic activity of LPMO and endoglucanases

Cited by 17 publications

References 46 publications

Oxidative enzyme activation of cellulose substrates for surface modification

Oxidative enzyme activation of cellulose substrates for surface modification

Contributions of Women in Recent Research on Biopolymer Science

High resolution product profiling of lytic polysaccharide monooxygenases

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