Point by point analysis: how ionic liquid affects the enzymatic hydrolysis of native and modified cellulose
Abstract
New strategies are needed to efficiently convert non-food biomass to glucose as a platform chemical. One promising approach is to use ionic liquids to first dissolve lignocellulose. Yet, in the presence of such solvents, the enzymes that catalyze cellulose hydrolysis become compromised in their activity. However, this decreased cellulase activity has not been examined in detail. Thus, the aim of this study was to investigate how the ionic liquid precisely affects cellulase activity and stability with regard to different cellulose substrates. Hereby, four ionic liquids were screened to identify which one best minimized the loss of enzyme activity. Then, this best ionic liquid was tested on one insoluble and two soluble cellulose substrates. Subsequently, the relevant parameters of solution viscosity and ionic strength were evaluated with respect to enzyme activity and stability. Finally the residual ionic liquid concentration from the precipitation of α-cellulose was varied. The best ionic liquid was found to be 1,3-dimethylimidazolium dimethylphosphate with the highest retained activity of 30% on the α-cellulose substrate in the presence of 10% (v/v) ionic liquid. Most importantly, an increase in viscosity and ionic strength contributed to the decrease in enzyme activity which nonetheless retained their stability. The hydrolysis of precipitated α-cellulose from ionic liquid showed significant higher reaction rates but reduced sugar yields when residual ionic liquid was present. None the less, it should be possible to effectively produce glucose from precipitated cellulose without needing to wash off all residual ionic liquid when optimized cellulase mixtures are used.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
Hardwoods and softwoods may require prohibitive quantities of energy to grind to fine powders.
“In contrast, hardwoods and softwoods may require prohibitive quantities of energy to grind to fine powders.183,186”
From Deconstruction of lignocellulosic biomass with ionic liquids (2013) · cites this paper as [183]
The larger the ratio between initial and final particle size, the more mechanical energy is required for the size reduction, all other conditions being equal.
“However, the larger the ratio between initial and final particle size, the more mechanical energy is required for the size reduction, all other conditions being equal.183”
From Deconstruction of lignocellulosic biomass with ionic liquids (2013) · cites this paper as [183]
Cites
Use of Dinitrosalicylic Acid Reagent for Determination of Reducing Sugar
Miller, G. L. (1959) · Analytical Chemistry · doi:10.1021/ac60147a030 · Cited by 28,963 · see citing works
Cellulose: Fascinating Biopolymer and Sustainable Raw Material
Klemm, D., Heublein, B., Fink, H., & Bohn, A. (2005) · Angewandte Chemie International Edition · doi:10.1002/anie.200460587 · Cited by 7,551 · see citing works
Measurement of cellulase activities
Ghose, T. K. (1987) · Pure and Applied Chemistry · doi:10.1351/pac198759020257 · Cited by 6,256 · see citing works
Features of promising technologies for pretreatment of lignocellulosic biomass
MOSIER, N. (2005) · Bioresource Technology · doi:10.1016/j.biortech.2004.06.025 · Cited by 6,251 · see citing works
Microbial Cellulose Utilization: Fundamentals and Biotechnology
Lynd, L. R., Weimer, P. J., van Zyl, W. H., & Pretorius, I. S. (2002) · Microbiology and Molecular Biology Reviews · doi:10.1128/mmbr.66.3.506-577.2002 · Cited by 4,726 · see citing works
Zhang, Y. ‐. P., & Lynd, L. R. (2004) · Biotechnology and Bioengineering · doi:10.1002/bit.20282 · Cited by 1,891 · see citing works
van Rantwijk, F., & Sheldon, R. A. (2007) · Chemical Reviews · doi:10.1021/cr050946x · Cited by 1,561 · see citing works
Ionic Liquids and Their Interaction with Cellulose
Pinkert, A., Marsh, K. N., Pang, S., & Staiger, M. P. (2009) · Chemical Reviews · doi:10.1021/cr9001947 · Cited by 1,508 · see citing works
Klinke, H. B., Thomsen, A. B., & Ahring, B. K. (2004) · Applied Microbiology and Biotechnology · doi:10.1007/s00253-004-1642-2 · Cited by 1,485 · see citing works
Sun, N., Rahman, M., Qin, Y., Maxim, M. L., Rodríguez, H., & Rogers, R. D. (2009) · Green Chemistry · doi:10.1039/b822702k · Cited by 988 · see citing works
Dissolution of Wood in Ionic Liquids
Kilpeläinen, I., Xie, H., King, A. W. T., Granström, M., Heikkinen, S., & Argyropoulos, D. S. (2007) · Journal of Agricultural and Food Chemistry · doi:10.1021/jf071692e · Cited by 943 · see citing works
Lee, S. H., Doherty, T. V., Linhardt, R. J., & Dordick, J. S. (2008) · Biotechnology and Bioengineering · doi:10.1002/bit.22179 · Cited by 942 · see citing works
Cellulose dissolution with polar ionic liquids under mild conditions: required factors for anions
Fukaya, Y., Hayashi, K., Wada, M., & Ohno, H. (2008) · Green Chem. · doi:10.1039/b713289a · Cited by 775 · see citing works
High-throughput screening for ionic liquids dissolving (ligno-)cellulose
Zavrel, M., Bross, D., Funke, M., Büchs, J., & Spieß, A. C. (2009) · Bioresource Technology · doi:10.1016/j.biortech.2008.11.052 · Cited by 696 · see citing works
Ionic liquids: Green solvents for nonaqueous biocatalysis
Yang, Z., & Pan, W. (2005) · Enzyme and Microbial Technology · doi:10.1016/j.enzmictec.2005.02.014 · Cited by 673 · see citing works
Ionic Liquids as Reaction Medium in Cellulose Functionalization
Heinze, T. J., Schwikal, K., & Barthel, S. (2005) · Macromolecular Bioscience · doi:10.1002/mabi.200500039 · Cited by 589 · see citing works
Enhancement of cellulose saccharification kinetics using an ionic liquid pretreatment step
Dadi, A. P., Varanasi, S., & Schall, C. A. (2006) · Biotechnology and Bioengineering · doi:10.1002/bit.21047 · Cited by 574 · see citing works
Effect of hemicellulose and lignin removal on enzymatic hydrolysis of steam pretreated corn stover
Öhgren, K., Bura, R., Saddler, J. N., & Zacchi, G. (2006) · Bioresource Technology · doi:10.1016/j.biortech.2006.09.003 · Cited by 570 · see citing works
Wyman, C. E., Dale, B. E., Elander, R. T., Holtzapple, M. T., Ladisch, M. R., & Lee, Y. Y. (2005) · Bioresource Technology · doi:10.1016/j.biortech.2005.01.018 · Cited by 532 · see citing works
‘Cradle-to-grave’ assessment of existing lignocellulose pretreatment technologies
Sousa, L. D. C., Chundawat, S. P. S., Balan, V., & Dale, B. E. (2009) · Current Opinion in Biotechnology · doi:10.1016/j.copbio.2009.05.003 · Cited by 497 · see citing works
Regenerating cellulose from ionic liquids for an accelerated enzymatic hydrolysis
Zhao, H., Jones, C. L., Baker, G. A., Xia, S., Olubajo, O., & Person, V. N. (2009) · Journal of Biotechnology · doi:10.1016/j.jbiotec.2008.08.009 · Cited by 492 · see citing works
Synergism of Cellulases from Trichoderma reesei in the Degradation of Cellulose
Henrissat, B., Driguez, H., Viet, C., et al. (1985) · Nature Biotechnology · doi:10.1038/nbt0885-722 · Cited by 481 · see citing works
Pan, X., Gilkes, N. R., Kadla, J. F., Pye, K., Saka, S., Gregg, D. J., Ehara, K., Xie, D., Lam, D., & Saddler, J. N. (2006) · Biotechnology and Bioengineering · doi:10.1002/bit.20905 · Cited by 457 · see citing works
Tan, S. S. Y., MacFarlane, D. R., Upfal, J., Edye, L. A., Doherty, W. O. S., Patti, A. F., Pringle, J. M., & Scott, J. L. (2009) · Green Chemistry · doi:10.1039/b815310h · Cited by 429 · see citing works
Singh, S., Simmons, B. A., & Vogel, K. P. (2009) · Biotechnology and Bioengineering · doi:10.1002/bit.22386 · Cited by 380 · see citing works
Li, Q., He, Y.-C., Xian, M., Jun, G., Xu, X., Yang, J., & Li, L. (2009) · Bioresource Technology · doi:10.1016/j.biortech.2009.02.040 · Cited by 362 · see citing works
Pretreatment and fractionation of corn stover by ammonia recycle percolation process
Kim, T. H., & Lee, Y. Y. (2005) · Bioresource Technology · doi:10.1016/j.biortech.2005.01.015 · Cited by 329 · see citing works
Enzymatic hydrolysis of cellulose: An overview
Walker, L. P., & Wilson, D. B. (1991) · Bioresource Technology · doi:10.1016/0960-8524(91)90095-2 · Cited by 320 · see citing works
Dissolution of Candida antarctica lipase B in ionic liquids: effects on structure and activity
Lau, R. M., Sorgedrager, M. J., Carrea, G., van Rantwijk, F., Secundo, F., & Sheldon, R. A. (2004) · Green Chemistry · doi:10.1039/b405693k · Cited by 317 · see citing works
Ionic Liquids: The Neglected Issues
Scammells, P. J., Scott, J. L., & Singer, R. D. (2005) · Australian Journal of Chemistry · doi:10.1071/ch04272 · Cited by 278 · see citing works
Solvents applied in the field of cellulose chemistry: a mini review
Heinze, T. J., & Koschella, A. (2005) · Polímeros · doi:10.1590/s0104-14282005000200005 · Cited by 259 · see citing works
A simple test for inactivation of an enzyme during assay
Selwyn, M. J. (1965) · Biochimica et Biophysica Acta (BBA) - Enzymology and Biological Oxidation · doi:10.1016/s0926-6593(65)80190-4 · Cited by 256 · see citing works
Nidetzky, B., Steiner, W., Hayn, M., et al. (1994) · Biochemical Journal · doi:10.1042/bj2980705 · Cited by 239 · see citing works
Ionic liquid tolerant hyperthermophilic cellulases for biomass pretreatment and hydrolysis
Datta, S., Holmes, B. M., Park, J. I., Chen, Z., Dibble, D., Hadi, M. Z., Blanch, H. W., Simmons, B. A., & Sapra, R. (2010) · Green Chemistry · doi:10.1039/b916564a · Cited by 229 · see citing works
Stabilization of α‐chymotrypsin by ionic liquids in transesterification reactions
Lozano, P., Puente, T. D. D., Guégan, J., et al. (2001) · Biotechnology and Bioengineering · doi:10.1002/bit.10089 · Cited by 229 · see citing works
Rinaldi, R., Meine, N., vom Stein, J., Palkovits, R., & Schüth, F. (2010) · ChemSusChem · doi:10.1002/cssc.200900281 · Cited by 201 · see citing works
The influence of major structural features of cellulose on rate of enzymatic hydrolysis
Fan, L. T., Lee, Y., & Beardmore, D. R. (1981) · Biotechnology and Bioengineering · doi:10.1002/bit.260230215 · Cited by 199 · see citing works
Removal of Fermentation Inhibitors Formed during Pretreatment of Biomass by Polymeric Adsorbents
Weil, J. R., Dien, B. S., Bothast, R. J., et al. (2002) · Industrial & Engineering Chemistry Research · doi:10.1021/ie0201056 · Cited by 198 · see citing works
Influence of water on the dissolution of cellulose in selected ionic liquids
Mazza, M., Catana, D.-A., Vaca‐García, C., & Cecutti, C. (2008) · Cellulose · doi:10.1007/s10570-008-9257-x · Cited by 184 · see citing works
Factors Affecting Wood Dissolution and Regeneration of Ionic Liquids
Li, B., Asikkala, J., Filpponen, I., & Argyropoulos, D. S. (2010) · Industrial & Engineering Chemistry Research · doi:10.1021/ie901560p · Cited by 172 · see citing works
Väljamäe, P., Sild, V., Pettersson, G., et al. (1998) · European Journal of Biochemistry · doi:10.1046/j.1432-1327.1998.2530469.x · Cited by 163 · see citing works
Potthast, A., Rosenau, T., Buchner, R., et al. (2002) · Cellulose · doi:10.1023/a:1015811712657 · Cited by 150 · see citing works
Is log P a Convenient Criterion to Guide the Choice of Solvents for Biphasic Enzymatic Reactions?
Filho, M. V., Stillger, T., Müller, M., et al. (2003) · Angewandte Chemie International Edition · doi:10.1002/anie.200351089 · Cited by 133 · see citing works
Pottkämper, J., Barthen, P., Ilmberger, N., Schwaneberg, U., Schenk, A., Schulte, M. M., Ignatíev, N., & Streit, W. R. (2009) · Green Chemistry · doi:10.1039/b820157a · Cited by 129 · see citing works
Characterization and Properties of Cellulases Purified from Trichoderma Reesei Strain L27
Shoemaker, S. P., Watt, K. W. K., Tsitovsky, G., et al. (1983) · Nature Biotechnology · doi:10.1038/nbt1083-687 · Cited by 128 · see citing works
Pretreatment of corn fiber by pressure cooking in water
Weil, J. R., Sarikaya, A., Rau, S.-L., Goetz, J., Ladisch, C. M., Brewer, M., Hendrickson, R., & Ladisch, M. R. (1998) · Applied Biochemistry and Biotechnology · doi:10.1007/bf02788829 · Cited by 114 · see citing works
Xylanase contribution to the efficiency of cellulose enzymatic hydrolysis of barley straw
García-Aparicio, M. P., Ballesteros, M., Manzanares, P., Ballesteros, I., González, A., & Negro, M. J. (2007) · Applied Biochemistry and Biotechnology · doi:10.1007/s12010-007-9064-0 · Cited by 109 · see citing works
Shen, Y., Zhang, Y., Ma, T., Bao, X., Du, F., Zhuang, G., & Qu, Y. (2007) · Bioresource Technology · doi:10.1016/j.biortech.2007.09.046 · Cited by 98 · see citing works
Wood liquefaction by ionic liquids
Honglu, X., & Tiejun, S. (2006) · Holzforschung · doi:10.1515/hf.2006.084 · Cited by 91 · see citing works
Synergistic cellulose hydrolysis can be described in terms of fractal‐like kinetics
Väljamäe, P., Kipper, K., Pettersson, G., et al. (2003) · Biotechnology and Bioengineering · doi:10.1002/bit.10775 · Cited by 91 · see citing works
Adverse effect of chloride impurities on lipase-catalyzed transesterifications in ionic liquids
Lee, S. H., Ha, S. H., Lee, S. B., & Koo, Y. (2006) · Biotechnology Letters · doi:10.1007/s10529-006-9095-6 · Cited by 76 · see citing works
Acidolysis of Wood in Ionic Liquids
Li, B., Filpponen, I., & Argyropoulos, D. S. (2010) · Industrial & Engineering Chemistry Research · doi:10.1021/ie1000983 · Cited by 73 · see citing works
Cellulose hydrolysis by immobilized Trichoderma reesei cellulase
Jones, P. O., & Vasudevan, P. T. (2009) · Biotechnology Letters · doi:10.1007/s10529-009-0119-x · Cited by 60 · see citing works
Jäger, G., Wu, Z., Garschhammer, K., et al. (2010) · Biotechnology for Biofuels · doi:10.1186/1754-6834-3-18 · Cited by 58 · see citing works
Self-citationAdsul, M. G., Terwadkar, A. P., Varma, A. J., et al. (2009) · BioResources · doi:10.15376/biores.4.4.1670-1681 · Cited by 57 · see citing works
Ionic Liquids as Performance Additives for Electroenzymatic Syntheses
Kohlmann, C., Greiner, L., Leitner, W., et al. (2009) · Chemistry - A European Journal · doi:10.1002/chem.200901046 · Cited by 37 · see citing works
Ellouz, S. C., Durand, H., & Tiraby, G. (1987) · Journal of Chromatography A · doi:10.1016/s0021-9673(01)94068-3 · Cited by 28 · see citing works
A test for measuring the effects of enzyme inactivation
Schnell, S. D., & Hanson, S. M. (2006) · Biophysical Chemistry · doi:10.1016/j.bpc.2006.08.010 · Cited by 22 · see citing works
Park, S., Viklund, F., Hult, K., et al. (2003) · ACS symposium series · doi:10.1021/bk-2003-0856.ch019 · Cited by 20 · see citing works
Exo- and endo-glucanolytic activity of cellulases purified from Trichoderma reesei
Gama, M., Vilanova, M., & Mota, M. (1998) · Biotechnology Techniques · doi:10.1023/a:1008808803109 · Cited by 13 · see citing works
Comparison of three commercial cellulases for production of glucose from acid-treated hardwood
Beck, M. J., Johnson, R. D., & Baker, C. S. (1990) · Applied Biochemistry and Biotechnology · doi:10.1007/bf02920264 · Cited by 10 · see citing works
Flagged first, then by citations
Cited by
Sorted by citations
Deconstruction of lignocellulosic biomass with ionic liquids
Brandt, A., Gräsvik, J., Hallett, J. P., & Welton, T. (2013) · Green Chemistry · doi:10.1039/c2gc36364j · Cited by 1,557 · see citing works
Ionic liquids for biofuel production: Opportunities and challenges
Liu, C.-Z., Wang, F., Stiles, A. R., & Guo, C. (2012) · Applied Energy · doi:10.1016/j.apenergy.2011.11.031 · Cited by 236 · see citing works
Lu, H., Yadav, V., Bilal, M., & Iqbal, H. M. N. (2022) · Chemosphere · doi:10.1016/j.chemosphere.2021.132574 · Cited by 96 · see citing works
Sathitsuksanoh, N., Zhu, Z., & Zhang, Y.-H. P. (2012) · Cellulose · doi:10.1007/s10570-012-9719-z · Cited by 63 · see citing works
- Authors
- Engel, P., Mladenov, R., Wulfhorst, H., Jäger, G., & Spiess, A. C.
- Affiliations
- RWTH Aachen University (DE)
- Corresponding author
- Spiess, Antje C.
- Venue
- Green Chemistry
- Publisher
- Royal Society of Chemistry (RSC)
- Published
- 2010
- Volume
- 12
- Issue
- 11
- Pages
- 1959
- ISSN
- 1463-9262 (ISSN-L)
- 1463-9270
- OpenAlex
- W2074255689
- Cited by
- 137
- References
- 61
- Citations by year
- 2026: 1 · 2025: 2 · 2024: 3 · 2023: 3 · 2022: 5 · 2021: 8 · 2020: 2 · 2019: 15 · 2018: 10 · 2017: 12 · 2016: 11 · 2015: 11 · 2014: 18 · 2013: 13 · 2012: 14
- FWCI
- 6.80
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Green Chemistry (publishedVersion)
- RWTH Publications (RWTH Aachen) (submittedVersion)
- Funders
- Deutsche Forschungsgemeinschaft
- Topics
- Physical Sciences › Engineering › Biomedical Engineering › Biofuel production and bioconversion
- Physical Sciences › Chemical Engineering › Catalysis › Ionic liquids properties and applications
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Enzyme Catalysis and Immobilization
- Keywords
- ionic liquids, enzymatic hydrolysis, cellulase activity, alpha-cellulose, solution viscosity, ionic strength, glucose production, non-food biomass, sugar yield
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
