Investigation of accessibility and reactivity of cellulose pretreated by ionic liquid at high loading

Endo, Takatsugu; Aung, Ei Mon; Fujii, Shunsuke; Hosomi, Shota; Kimizu, Mitsugu; Ninomiya, Kazuaki; Takahashi, Kenji

doi:10.1016/j.carbpol.2017.08.105

Cited by 31 publications

(15 citation statements)

References 65 publications

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“…6,7 Later, Endo et al have discovered that the use of high concentrations in the IL was advantageous for the cellulose pretreatment process because it did only reduced process cost but also increased hydrolytic efficiency. 8 In this paper, we demonstrate that the choice of anion species results in the unique structuring of cellulose/IL mixtures at high concentration. We employed three different ILs composed of the same cation such as 1-methyl-3propylimidazolium cation ([C 3 mim] + ) paired with [OAc] − , dimethylphospate ([DMP] − ), and chloride (Figure 1).…”

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confidence: 73%

“…These sheets are stacked on each other and are intercalated by the cation layer. In addition, high concentrations affect the cellulose/IL structure at various spatial scales; specifically, high concentrations produce liquid crystallinity, a nanolevel aggregated structure, and even moldability. , Later, Endo et al have discovered that the use of high concentrations in the IL was advantageous for the cellulose pretreatment process because it did only reduced process cost but also increased hydrolytic efficiency …”

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confidence: 99%

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Self-Assembly and Complexation of Cellulose/Ionic Liquid at High Cellulose Concentration: Anion Dependence

Endo

Yoshida

Kimura

2020

Crystal Growth & Design

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We investigated the state of cellulose that was dissolved in ionic liquid (IL) consisting of 1-methyl-3-propylimdiazolium cation ([C 3 mim] + ) paired with acetate ([OAc] − ), dimethylphospate ([DMP] − ), or chloride (Cl − ) anions using wide-angle X-ray scattering (WAXS), particularly focusing on the high cellulose concentration region (10−80 mol %). The anion species considerably altered the WAXS pattern of the cellulose/IL mixtures. [C 3 mim][OAc] deconstructed cellulose crystal structure up to the 40 mol % cellulose concentration. Similar to the previously reported cellulose/1-ethyl-3-methylimidazolium acetate system ([C 2 mim][OAc]), the mixtures of cellulose/[C 3 mim]-[OAc] at 25−60 mol % induced a low angle peak, which corresponds to the self-assembly of the system. For [C 3 mim]-[DMP] and [C 3 mim]Cl mixtures, sharp Bragg peaks were observed, which demonstrated the formation of the complex crystal of cellulose/IL. The presence of moisture eventually deconstructed these crystal structures; while for [C 3 mim]Cl, an intermediate complex crystal containing H 2 O molecules emerged. This work contributes to understanding the cellulose state dissolved in IL at high concentrations and to the development of crystal engineering on this most abundant and recalcitrant biopolymer.

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confidence: 73%

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confidence: 99%

Self-Assembly and Complexation of Cellulose/Ionic Liquid at High Cellulose Concentration: Anion Dependence

Endo

Yoshida

Kimura

2020

Crystal Growth & Design

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“…e.g., an increased substrate SSA improves cellulose adsorption and make enzymatic process more effective [ 31 , 32 ]. Assuming that MB forms a monolayer of adsorbed molecules on the surface of sorbent particles, the SSA can be calculated using Equation (2):

where

is the specific surface area (m 2 /g),

is the maximum mass of adsorbed MB in the monolayer (g/g),

is the surface area occupied by one MB molecule (m 2 /molecule) (typically assumed to be 130 Å 2 per molecule),

is Avogrado’s number (6.02 × 10 23 molecule/mol) and

is the MB molar mass (355.89 g/mol) [ 33 , 34 , 35 ].

was estimated from the Langmuir isotherm model.…”

Section: Methodsmentioning

confidence: 99%

Alkalization of Kraft Pulps from Pine and Eucalyptus and Its Effect on Enzymatic Saccharification and Viscosity Control of Cellulose

Carrillo-Varela¹,

Vidal

Vidaurre

et al. 2022

Polymers

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Bleached kraft pulps from eucalyptus and pine were subjected to cold caustic extraction (CCE) with NaOH (5, 10, 17.5, and 35%) for hemicelluloses removal and to increase cellulose accessibility. The effect of these changes was evaluated in enzymatic saccharification with the multicomponent Cellic CTec3 enzyme cocktail, and in viscosity reduction of pulps with the monocomponent Trichoderma reesei endoglucanase (EG). After CCE with 10% NaOH (CCE10) and 17.5% NaOH (CCE17.5), hemicellulose content lower than 1% was achieved in eucalyptus and pine pulps, respectively. At these concentrations, cellulose I started to be converted into cellulose II. NaOH concentrations higher than 17.5% decreased the intrinsic viscosity (from 730 to 420 mL/g in eucalyptus and from 510 to 410 mL/g in pine). Cellulose crystallinity was reduced from 60% to 44% in eucalyptus and from 71% to 44% in pine, as the NaOH concentration increased. Enzymatic multicomponent saccharification showed higher glucose yields in all CCE-treated eucalyptus samples (up to 93%) while only CCE17.5 and CCE35 pine pulps achieved 90% after 40 h of incubation. Untreated bleached pulps of both species presented saccharification yields lower than 70%. When monocomponent EG was used to treat the same pulps, depending on enzyme charge and incubation time, a wide range of intrinsic viscosity reduction was obtained (up to 74%). Results showed that eucalyptus pulps are more accessible and easier to hydrolyze by enzymes than pine pulps and that the conversion of cellulose I to cellulose II hydrate only has the effect of increasing saccharification of CCE pine samples. Viscosity reduction of CCE pulps and EG treated pulps were obtained in a wide range indicating that pulps presented characteristics suitable for cellulose derivatives production.

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“…Efficient conversion of cellulose to its constituent monomer, glucose, or other small molecules is the gateway to production of cost-effective second-generation biofuels and biochemicals [2,3]. Unfortunately, cellulose is resistant to depolymerization [4], and converting it into soluble products requires energy-intensive pretreatments [5][6][7][8][9][10], harsh conditions [11][12][13][14][15][16], excess enzymes [17][18][19], or expensive solvents [20,21] that contribute disproportionately to biofuel production costs [2,22].…”

Section: Introductionmentioning

confidence: 99%

A New Method for Solid Acid Catalyst Evaluation for Cellulose Hydrolysis

Tyufekchiev

Finzel

Zhang

et al. 2021

Sustainable Chemistry

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A systematic and structure-agnostic method for identifying heterogeneous activity of solid acids for catalyzing cellulose hydrolysis is presented. The basis of the method is preparation of a supernatant liquid by exposing the solid acid to reaction conditions and subsequent use of the supernatant liquid as a cellulose hydrolysis catalyst to determine the effects of in situ generated homogeneous acid species. The method was applied to representative solid acid catalysts, including polymer-based, carbonaceous, inorganic, and bifunctional materials. In all cases, supernatant liquids produced from these catalysts exhibited catalytic activity for cellulose hydrolysis. Direct comparison of the activity of the solid acid catalysts and their supernatants could not provide unambiguous detection of heterogeneous catalysis. A reaction pathway kinetic model was used to evaluate potential false-negative interpretation of the supernatant liquid test and to differentiate heterogeneous from homogeneous effects on cellulose hydrolysis. Lastly, differences in the supernatant liquids obtained in the presence and absence of cellulose were evaluated to understand possibility of false-positive interpretation, using structural evidence from the used catalysts to gain a fresh understanding of reactant–catalyst interactions. While many solid acid catalysts have been proposed for cellulose hydrolysis, to our knowledge, this is the first effort to attempt to differentiate the effects of heterogeneous and homogeneous activities. The resulting supernatant liquid method should be used in all future attempts to design and develop solid acids for cellulose hydrolysis.

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Investigation of accessibility and reactivity of cellulose pretreated by ionic liquid at high loading

Cited by 31 publications

References 65 publications

Self-Assembly and Complexation of Cellulose/Ionic Liquid at High Cellulose Concentration: Anion Dependence

Self-Assembly and Complexation of Cellulose/Ionic Liquid at High Cellulose Concentration: Anion Dependence

Alkalization of Kraft Pulps from Pine and Eucalyptus and Its Effect on Enzymatic Saccharification and Viscosity Control of Cellulose

A New Method for Solid Acid Catalyst Evaluation for Cellulose Hydrolysis

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