期刊论文详细信息
Biotechnology for Biofuels
The correlation between the enzymatic saccharification and the multidimensional structure of cellulose changed by different pretreatments
Ting Cui1  Jihong Li1  Zhipei Yan1  Menghui Yu1  Shizhong Li1 
[1] Beijing Engineering Research Centre of Biofuels, Tsinghua University, Beijing 100084, China
关键词: Specific surface area;    Lattice spacing;    Water contact angle;    Crystallinity;    Allomorph;    Crystalline cellulose;   
Others  :  1084509
DOI  :  10.1186/s13068-014-0134-6
 received in 2014-04-09, accepted in 2014-09-01,  发布年份 2014
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【 摘 要 】

Background

The bioconversion of cellulose into simple sugars or chemicals has attracted extensive attention in recent decades. The crystal allomorphs of cellulose are key factor affecting cellulose saccharification. However, due to the influence of lignin, hemicelluloses, and different characterization methods in the literature, the effect of cellulose allomorphs on cellulose saccharification is still unresolved. Thus, a systematic research on the effect of different cellulose allomorphs on enzymatic saccharification was required.

Results

Multiple approaches, including the use of ionic liquid (IL), ethylenediamine (EDA), glycerol, and sodium hydroxide, were used to pretreat α-cellulose in this work. The properties of the obtained cellulose (crystallinity, lattice spacing, specific surface area, and wettability) were characterized by X-ray diffraction, Brunauer, Emmett, and Teller (BET) specific surface area analysis, and water contact angle analysis, respectively. The distance of the lattice spacing of cellulose III was longer than that of other cellulose samples. The crystallinity and water contact angles of the cellulose samples were ranked in the following order: cellulose treated with IL < cellulose treated with NaOH < cellulose treated with EDA < cellulose without treatment < cellulose treated with glycerol. Cellulose treated with IL, with a crystallinity index value of 20%, was very close to amorphous cellulose. After 72 h hydrolysis, the cellulose conversion ratio ranged from 43% to 99%. Cellulose treated with IL exhibited the best hydrolysis profile, followed by cellulose treated with EDA.

Conclusion

Ionic liquid pretreatment significantly altered the ultrastructure and morphology of cellulose samples, making cellulose much easier for enzymes to digest due to its significantly high amorphous content. However, when the impact of amorphous content was not considered, the allomorph easiest for enzymes to digest was cellulose III, followed by cellulose II, cellulose Iα, and cellulose Iβ. When the cellulose crystallinity index was similar, the allomorph type was the dominant factor. The amorphous content had a strong positive influence on cellulose digestibility. Water contact angle was also an important factor in evaluating the enzymatic hydrolysis efficiency of cellulose except for cellulose III. A high wettability of cellulose enhanced the enzymatic hydrolysis when the crystal allomorph of all the cellulosic samples was the same.

【 授权许可】

   
2014 Cui et al.; licensee BioMed Central Ltd.

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【 参考文献 】
  • [1]PE Rez S, Mazeau K: Conformations, structures, and morphologies of celluloses. In Polysaccharides: Structural Diversity and Functional Versatility. 2nd edition. Edited by Dumitriu S. Marcel Dekker, New York; 2005:41-68.
  • [2]Himmel ME, Ding SY, Johnson DK, Adney WS, Nimlos MR, Brady JW, Foust TD: Biomass recalcitrance: engineering plants and enzymes for biofuels production. Science 2007, 315(5813):804-807.
  • [3]Salehi SMA, Karimi K, Behzad T, Poornejad N: Efficient conversion of rice straw to bioethanol using sodium carbonate pretreatment. Energ Fuel 2012, 26(12):7354-7361.
  • [4]Lou H, Zhu JY, Lan TQ, Lai H, Qiu X: pH-Induced lignin surface modification to reduce nonspecific cellulase binding and enhance enzymatic saccharification of lignocelluloses. ChemSusChem 2013, 6(5):919-927.
  • [5]Kim SB, Lee SJ, Lee JH, Jung YR, Thapa LP, Kim JS, Um Y, Park C, Kim SW: Pretreatment of rice straw with combined process using dilute sulfuric acid and aqueous ammonia. Biotechnol Biofuels 2013, 6(1):109. BioMed Central Full Text
  • [6]Xu N, Zhang W, Ren S, Liu F, Zhao C, Liao H, Xu Z, Huang J, Li Q, Tu Y, Yu B, Wang Y, Jiang J, Qin J, Peng L: Hemicelluloses negatively affect lignocellulose crystallinity for high biomass digestibility under NaOH and H2SO4 pretreatments in Miscanthus. Biotechnol Biofuels 2012, 5(1):58. BioMed Central Full Text
  • [7]Percival Zhang YH, Himmel ME, Mielenz JR: Outlook for cellulase improvement: Screening and selection strategies. Biotechnol Adv 2006, 24(5):452-481.
  • [8]Oh SY, Yoo DI, Shin Y, Kim HC, Kim HY, Chung YS, Park WH, Youk JH: Crystalline structure analysis of cellulose treated with sodium hydroxide and carbon dioxide by means of X-ray diffraction and FTIR spectroscopy. Carbohyd Res 2005, 340(15):2376-2391.
  • [9]Fan J, De Bruyn M, Budarin VL, Gronnow MJ, Shuttleworth PS, Breeden S, Macquarrie DJ, Clark JH: Direct microwave-assisted hydrothermal depolymerization of cellulose. J Am Chem Soc 2013, 135(32):11728-11731.
  • [10]Stauner T, Silva IB, El Seoud OA, Frollini E, Petri DFS: Cellulose loading and water sorption value as important parameters for the enzymatic hydrolysis of cellulose. Cellulose 2013, 20(3):1109-1119.
  • [11]Hall M, Bansal P, Lee JH, Realff MJ, Bommarius AS: Cellulose crystallinity - a key predictor of the enzymatic hydrolysis rate. FEBS J 2010, 277(6):1571-1582.
  • [12]Chundawat SPS, Bellesia G, Uppugundla N, Da Costa SL, Gao D, Cheh AM, Agarwal UP, Bianchetti CM, Phillips GN, Langan P, Balan V, Gnanakaran S, Dale BE: Restructuring the crystalline cellulose hydrogen bond network enhances its depolymerization rate. J Am Chem Soc 2011, 133(29):11163-11174.
  • [13]Igarashi K, Wada M, Samejima M: Activation of crystalline cellulose to cellulose IIII results in efficient hydrolysis by cellobiohydrolase. FEBS J 2007, 274(7):1785-1792.
  • [14]Cho HM, Gross AS, Chu J: Dissecting force interactions in cellulose deconstruction reveals the required solvent versatility for overcoming biomass recalcitrance. J Am Chem Soc 2011, 133(35):14033-14041.
  • [15]Mittal A, Katahira R, Himmel ME, Johnson DK: Effects of alkaline or liquid-ammonia treatment on crystalline cellulose: changes in crystalline structure and effects on enzymatic digestibility. Biotechnol Biofuels 2011, 4:41. BioMed Central Full Text
  • [16]Samayam IP, Hanson BL, Langan P, Schall CA: Ionic-liquid induced changes in cellulose structure associated with enhanced biomass hydrolysis. Biomacromolecules 2011, 12(8):3091-3098.
  • [17]Ciolacu D, Gorgieva S, Tampu D, Kokol V: Enzymatic hydrolysis of different allomorphic forms of microcrystalline cellulose. Cellulose 2011, 18(6):1527-1541.
  • [18]Nishiyama Y, Langan P, Chanzy H: Crystal structure and hydrogen-bonding system in cellulose Iβ from synchrotron x-ray and neutron fiber diffraction. J Am Chem Soc 2002, 124(31):9074-9082.
  • [19]Wada M, Heux L, Sugiyama J: Polymorphism of cellulose i family: reinvestigation of cellulose IV. Biomacromolecules 2004, 5(4):1385-1391.
  • [20]Zhang J, Wang Y, Zhang L, Zhang R, Liu G, Cheng G: Understanding changes in cellulose crystalline structure of lignocellulosic biomass during ionic liquid pretreatment by XRD. Bioresour Technol 2014, 151:402-405.
  • [21]Zhang J, Zhang B, Zhang J, Lin L, Liu S, Ouyang P: Effect of phosphoric acid pretreatment on enzymatic hydrolysis of microcrystalline cellulose. Biotechnol Adv 2010, 28(5):613-619.
  • [22]Li J, Li S, Fan C, Yan Z: The mechanism of poly(ethylene glycol) 4000 effect on enzymatic hydrolysis of lignocellulose. Colloids Surf B: Biointerfaces 2012, 89:203-210.
  • [23]Kataoka Y, Kondo T: FT-IR microscopic analysis of changing cellulose crystalline structure during wood cell wall formation. Macromolecules 1998, 31(3):760-764.
  • [24]Gao D, Chundawat SPS, Sethi A, Balan V, Gnanakaran S, Dale BE: Increased enzyme binding to substrate is not necessary for more efficient cellulose hydrolysis. Proc Natl Acad Sci 2013, 110(27):10922-10927.
  • [25]Russell JB, Muck RE, Weimer PJ: Quantitative analysis of cellulose degradation and growth of cellulolytic bacteria in the rumen. FEMS Microbiol Ecol 2009, 67(2):183-197.
  • [26]Mansfield S, Meder R: Cellulose hydrolysis - the role of monocomponent cellulases in crystalline cellulose degradation. Cellulose 2003, 10(2):159-169.
  • [27]Park S, Baker JO, Himmel ME, Parilla PA, Johnson DK: Cellulose crystallinity index: measurement techniques and their impact on interpreting cellulase performance. Biotechnol Biofuels 2010, 3:10. BioMed Central Full Text
  • [28]Wada M, Kwon GJ, Nishiyama Y: Structure and thermal behavior of a cellulose i -ethylenediamine complex. Biomacromolecules 2008, 9(10):2898-2904.
  • [29]Cheng G, Varanasi P, Li C, Liu H, Melnichenko YB, Simmons BA, Kent MS, Singh S: Transition of cellulose crystalline structure and surface morphology of biomass as a function of ionic liquid pretreatment and its relation to enzymatic hydrolysis. Biomacromolecules 2011, 12(4):933-941.
  • [30]Wada M, Heux L, Nishiyama Y, Langan P: The structure of the complex of cellulose I with ethylenediamine by X-ray crystallography and cross-polarization/magic angle spinning 13C nuclear magnetic resonance. Cellulose 2009, 16(6):943-957.
  • [31]Igarashi K, Uchihashi T, Koivula A, Wada M, Kimura S, Okamoto T, Penttila M, Ando T, Samejima M: Traffic jams reduce hydrolytic efficiency of cellulase on cellulose surface. Science 2011, 333(6047):1279-1282.
  • [32]Bertran MS, Dale BE: Determination of cellulose accessibility by differential scanning calorimetry. J Appl Polym Sci 1986, 32(3):4241-4253.
  • [33]Li C, Cheng G, Balan V, Kent MS, Ong M, Chundawat SPS, Sousa LD, Melnichenko YB, Dale BE, Simmons BA, Singh S: Influence of physico-chemical changes on enzymatic digestibility of ionic liquid and AFEX pretreated corn stover. Bioresource Technol 2011, 102(13):6928-6936.
  • [34]Silverstein RA, Chen Y, Sharma-Shivappa RR, Boyette MD, Osborne J: A comparison of chemical pretreatment methods for improving saccharification of cotton stalks. Bioresource Technol 2007, 98(16):3000-3011.
  • [35]Chen M, Zhao J, Xia L: Comparison of four different chemical pretreatments of corn stover for enhancing enzymatic digestibility. Biomass Bioenergy 2009, 33(10):1381-1385.
  • [36]Li C, Knierim B, Manisseri C, Arora R, Scheller HV, Auer M, Vogel KP, Simmons BA, Singh S: Comparison of dilute acid and ionic liquid pretreatment of switchgrass: Biomass recalcitrance, delignification and enzymatic saccharification. Bioresource Technol 2010, 101(13):4900-4906.
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