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Hedenström, Mattias
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Laera, A., Yekta, S. S., Hedenström, M., Buzier, R., Guibaud, G., Dario, M., . . . van Hullebusch, E. D. (2019). A simultaneous assessment of organic matter and trace elements bio-accessibility in substrate and digestate from an anaerobic digestion plant. Bioresource Technology, 288, Article ID 121587.
Open this publication in new window or tab >>A simultaneous assessment of organic matter and trace elements bio-accessibility in substrate and digestate from an anaerobic digestion plant
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2019 (English)In: Bioresource Technology, ISSN 0960-8524, E-ISSN 1873-2976, Vol. 288, article id 121587Article in journal (Refereed) Published
Abstract [en]

This study evaluates a simultaneous assessment of organic matter (OM) and trace elements (TE) bio-accessibility in substrate and digestate from a full-scale anaerobic digester by a sequential OM extraction method. Simultaneous release of TE was determined along with the extraction of different OM fractions and the effects of extracting reagents on characteristics of OM were evaluated by nuclear magnetic resonance (NMR) spectroscopy. The reagents used for sequential extraction of OM were not enough selective. However, proteins were particularly removed by 0.1 M NaOH, while 72% H2SO4 mainly extracted hemicellulose and cellulose. The OM fractionation allowed for simultaneous extraction of > 60% of total As, Cd, Co, Fe, Mn, Ni and Zn, while the extraction was limited for Al, Cr, Cu, Mo, and Pb. In substrate, > 50% of total As, Co, Mn and Ni and < 40% of total Fe, Zn and Mo were identified in bio-accessible fractions. In digestate, all elements demonstrated poor bio-accessibility except for As.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Sequential chemical extraction, Organic matter fractionation, Trace elements fractionation, NMR spectroscopy, Anaerobic co-digestion
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:umu:diva-161497 (URN)10.1016/j.biortech.2019.121587 (DOI)000472018100008 ()31200348 (PubMedID)
Available from: 2019-07-12 Created: 2019-07-12 Last updated: 2019-07-12Bibliographically approved
Michel, M., Visnes, T., Homan, E. J., Seashore-Ludlow, B., Hedenström, M., Wiita, E., . . . Helleday, T. (2019). Computational and Experimental Druggability Assessment of Human DNA Glycosylases. ACS OMEGA, 4(7), 11642-11656
Open this publication in new window or tab >>Computational and Experimental Druggability Assessment of Human DNA Glycosylases
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2019 (English)In: ACS OMEGA, ISSN 2470-1343, Vol. 4, no 7, p. 11642-11656Article in journal (Refereed) Published
Abstract [en]

Due to a polar or even charged binding interface, DNA-binding proteins are considered extraordinarily difficult targets for development of small-molecule ligands and only a handful of proteins have been targeted successfully to date. Recently, however, it has been shown that development of selective and efficient inhibitors of 8-oxoguanine DNA glycosylase is possible. Here, we describe the initial druggability assessment of DNA glycosylases in a computational setting and experimentally investigate several methods to target endonuclease VIII-like 1 (NEIL1) with small-molecule inhibitors. We find that DNA glycosylases exhibit good predicted druggability in both DNA-bound and -unbound states. Furthermore, we find catalytic sites to be highly flexible, allowing for a range of interactions and binding partners. One flexible catalytic site was rationalized for NEIL1 and further investigated experimentally using both a biochemical assay in the presence of DNA and a thermal shift assay in the absence of DNA.

National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:umu:diva-164548 (URN)10.1021/acsomega.9b00162 (DOI)000482176800036 ()31460271 (PubMedID)
Available from: 2019-10-23 Created: 2019-10-23 Last updated: 2019-10-23Bibliographically approved
Yekta, S. S., Hedenström, M., Svensson, B. H., Sundgren, I., Dario, M., Enrich-Prast, A., . . . Bjorn, A. (2019). Molecular characterization of particulate organic matter in full scale anaerobic digesters: An NMR spectroscopy study. Science of the Total Environment, 685, 1107-1115
Open this publication in new window or tab >>Molecular characterization of particulate organic matter in full scale anaerobic digesters: An NMR spectroscopy study
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2019 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 685, p. 1107-1115Article in journal (Refereed) Published
Abstract [en]

This study assesses the molecular characteristics of particulate organic matter (POM) in agricultural and food waste digesters and elucidates the molecular properties of the recalcitrant POM fraction, which remains in the digestate after AD process. Molecular properties of POM in influent (substrate) and effluent (digestate) of seven full-scale AD plants (three agricultural waste and four food waste digesters) were characterized and compared using solid-state (13)C( )cross-polarization magic angle spinning (CP-MAS) and solution-state H-1,C-13 heteronuclear single-quantum coherence (HSQC) nuclear magnetic resonance (NMR) spectroscopy. Comparison of the POM structural compositions of substrate and digestate from each AD plant revealed an enrichment of protein structures relative to the carbohydrates in most cases, implying a preferential degradation of the carbohydrates over proteins and/or increase of microbial biomass upon AD of agricultural and food wastes. Distinctive molecular structures of labile and recalcitrant fractions of POM, subjected to AD, were identified by comparing the NMR spectra of all substrate and digestate POM. Accordingly, the labile POM fraction in food and agricultural solid wastes is characterized by structural entities of lipids and starch-like carbohydrates, whereas recalcitrant POM structures resemble alkyl and aromatic subunits of amino acids, lignin, and polysaccharides with beta-glycosidic linkages. This information serves as a basis to further explore optimization approaches for improving AD of the underutilized POM and the fate of organic matter in digestate-amended arable lands. (C) 2018 The Authors. Published by Elsevier B.V.

Place, publisher, year, edition, pages
ELSEVIER, 2019
Keywords
Anaerobic digestion, Food waste, Agricultural waste, Organic matter, NMR, Digestate
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-162296 (URN)10.1016/j.scitotenv.2019.06.264 (DOI)000477951900102 ()31390701 (PubMedID)
Available from: 2019-08-27 Created: 2019-08-27 Last updated: 2019-08-27Bibliographically approved
Zhang, B., Sztojka, B., Escamez, S., Vanholme, R., Hedenström, M., Wang, Y., . . . Tuominen, H. (2019). PIRIN2 suppresses S-type lignin accumulation in a noncell-autonomous manner in Arabidopsis xylem elements. New Phytologist
Open this publication in new window or tab >>PIRIN2 suppresses S-type lignin accumulation in a noncell-autonomous manner in Arabidopsis xylem elements
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2019 (English)In: New Phytologist, ISSN 0028-646X, E-ISSN 1469-8137Article in journal (Refereed) Epub ahead of print
Abstract [en]
  • PIRIN (PRN) genes encode cupin domain‐containing proteins that function as transcriptional co‐regulators in humans but that are poorly described in plants. A previous study in xylogenic cell cultures of Zinnia elegans suggested a role for a PRN protein in lignification. This study aimed to identify the function of Arabidopsis (Arabidopsis thaliana) PRN proteins in lignification of xylem tissues.
  • Chemical composition of the secondary cell walls was analysed in Arabidopsis stems and/or hypocotyls by pyrolysis–gas chromatography/mass spectrometry, 2D‐nuclear magnetic resonance and phenolic profiling. Secondary cell walls of individual xylem elements were chemotyped by Fourier transform infrared and Raman microspectroscopy.
  • Arabidopsis PRN2 suppressed accumulation of S‐type lignin in Arabidopsis stems and hypocotyls. PRN2 promoter activity and PRN2:GFP fusion protein were localised specifically in cells next to the vessel elements, suggesting a role for PRN2 in noncell‐autonomous lignification of xylem vessels. Accordingly, PRN2 modulated lignin chemistry in the secondary cell walls of the neighbouring vessel elements.
  • These results indicate that PRN2 suppresses S‐type lignin accumulation in the neighbourhood of xylem vessels to bestow G‐type enriched lignin composition on the secondary cell walls of the vessel elements. Gene expression analyses suggested that PRN2 function is mediated by regulation of the expression of the lignin‐biosynthetic genes.
Place, publisher, year, edition, pages
New Phytologist Trust, 2019
Keywords
Arabidopsis, lignification, noncell-autonomy, PIRIN, xylem vessel element
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:umu:diva-165740 (URN)10.1111/nph.16271 (DOI)000495547800001 ()31625609 (PubMedID)
Funder
Swedish Research Council, 232-2011-1312Swedish Research Council Formas, 232-2011-1312Swedish Foundation for Strategic Research , RBP14-0011Vinnova, 201600504Knut and Alice Wallenberg Foundation, 20160341Bio4Energy
Available from: 2019-12-10 Created: 2019-12-10 Last updated: 2019-12-10
Semenchuk, P. R., Krab, E. J., Hedenström, M., Phillips, C. A., Ancin-Murguzur, F. J. & Cooper, E. J. (2019). Soil organic carbon depletion and degradation in surface soil after long-term non-growing season warming in High Arctic Svalbard. Science of the Total Environment, 646, 158-167
Open this publication in new window or tab >>Soil organic carbon depletion and degradation in surface soil after long-term non-growing season warming in High Arctic Svalbard
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2019 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 646, p. 158-167Article in journal (Refereed) Published
Abstract [en]

Arctic tundra active-layer soils are at risk of soil organic carbon (SOC) depletion and degradation upon global climate warming because they are in a stage of relatively early decomposition. Non-growing season (NGS) warming is particularly pronounced, and observed increases of CO2 emissions during experimentally warmed NGSs give concern for great SOC losses to the atmosphere. Here, we used snow fences in Arctic Spitsbergen dwarf shrub tundra to simulate 1.86 degrees C NGS warming for 9 consecutive years, while growing season temperatures remained unchanged. In the snow fence treatment, the 4-11 cm thick A-horizon had a 2% lower SOC concentration and a 0.48 kg Cm-2 smaller pool size than the controls, indicating SOC pool depletion. The snow fence treatment's A-horizon's alkyl/O-alkyl ratio was also significantly increased, indicating an advance of SOC degradation. The underlying 5 cm of B/C-horizon did not show these effects. Our results support the hypothesis that SOC depletion and degradation are connected to the long-term transience of observed ecosystem respiration (ER) increases upon soil warming. We suggest that the bulk of warming induced ER increases may originate from surface and not deep active layer or permafrost horizons. The observed losses of SOC might be significant for the ecosystem in question, but are in magnitude comparatively small relative to anthropogenic greenhouse gas enrichment of the atmosphere. We conclude that a positive feedback of carbon losses from surface soils of Arctic dwarf shrub tundra to anthropogenic forcing will be minor, but not negligible.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Snow fence, NMR, Carbon loss, Decomposition, Anthropogenic C emission feedback, Tundra
National Category
Environmental Sciences Soil Science
Identifiers
urn:nbn:se:umu:diva-166522 (URN)10.1016/j.scitotenv.2018.07.150 (DOI)000445164800017 ()30056226 (PubMedID)
Available from: 2019-12-17 Created: 2019-12-17 Last updated: 2019-12-17Bibliographically approved
Åkesson, K., Pettersson, S., Stahl, S., Surowiec, I., Hedenström, M., Eketjall, S., . . . Idborg, H. (2018). Kynurenine pathway is altered in patients with SLE and associated with severe fatigue. Lupus Science and Medicine, 5(1), Article ID e000254.
Open this publication in new window or tab >>Kynurenine pathway is altered in patients with SLE and associated with severe fatigue
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2018 (English)In: Lupus Science and Medicine, ISSN 2053-8790, E-ISSN 1625-9823, Vol. 5, no 1, article id e000254Article in journal (Refereed) Published
Abstract [en]

Objective: Fatigue has been reported as the most disturbing symptom in a majority of patients with SLE. Depression is common and often severe. Together these symptoms cause significant morbidity and affect patients with otherwise relatively mild disease. Tryptophan and its metabolites in the kynurenine pathway are known to be important in several psychiatric conditions, for example, depression, which are often also associated with fatigue. We therefore investigated the kynurenine pathway in patients with SLE and controls.

Methods: In a cross-sectional design plasma samples from 132 well-characterised patients with SLE and 30 age-matched and gender-matched population-based controls were analysed by liquid chromatography tandem mass spectrometry to measure the levels of tryptophan and its metabolites kynurenine and quinolinic acid. Fatigue was measured with Fatigue Severity Scale and depression with Hospital Anxiety and Depression Scale. SLE disease activity was assessed with Systemic Lupus Erythematosus Disease Activity Index (SLEDAI).

Results: The kynurenine/tryptophan ratio, as a measure of indoleamine 2,3-dioxygenase (IDO) activity, was increased in patients with SLE. Patients with active disease (SLEDAI >= 6) showed lower tryptophan levels compared with controls (54 mu M, SD=19 vs 62 mu M, SD=14, p=0.03), although patients with SLE overall did not differ compared with controls. Patients with SLE had higher levels of tryptophan metabolites kynurenine (966 nM, SD=530) and quinolinic acid (546 nM, SD=480) compared with controls (kynurenine: 712 nM, SD=230, p=0.0001; quinolinic acid: 380 nM, SD=150, p=0.001). Kynurenine, quinolinic acid and the kynurenine/tryptophan ratio correlated weakly with severe fatigue (r(s)=0.34, r(s)=0.28 and r(s)=0.24, respectively) but not with depression.

Conclusions: Metabolites in the kynurenine pathway are altered in patients with SLE compared with controls. Interestingly, fatigue correlated weakly with measures of enhanced tryptophan metabolism, while depression did not. Drugs targeting enzymes in the kynurenine pathway, for example, IDO inhibitors or niacin (B12) supplementation, which suppresses IDO activity, merit further investigation as treatments in SLE.

Place, publisher, year, edition, pages
BMJ Publishing Group Ltd, 2018
National Category
Rheumatology and Autoimmunity
Identifiers
urn:nbn:se:umu:diva-166400 (URN)10.1136/lupus-2017-000254 (DOI)000495994400006 ()29868176 (PubMedID)
Available from: 2019-12-17 Created: 2019-12-17 Last updated: 2019-12-17Bibliographically approved
Yekta, S. S., Hedenström, M., Stehr, J. E., Dario, M., Hertkorn, N. & Björn, A. (2018). Pretreatment of anaerobic digester samples by hydrochloric acid for solution-state H-1 and C-13 NMR spectroscopic characterization of organic matter. Chemosphere, 199, 201-209
Open this publication in new window or tab >>Pretreatment of anaerobic digester samples by hydrochloric acid for solution-state H-1 and C-13 NMR spectroscopic characterization of organic matter
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2018 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 199, p. 201-209Article in journal (Refereed) Published
Abstract [en]

Pretreatment of anaerobic digester samples by hydrochloric acid (HCl) resulted in removal of Fe-based mineral and coordination compounds, attenuating their interferences with solution-state nuclear magnetic resonance (NMR) spectroscopic characterization of the solid phase organic matter. Substrate (influent) and digestate (effluent) samples from two full-scale anaerobic digesters, designated CD (co-digester) and SSD (sewage sludge digester), were investigated. Pretreatment of CD samples with 0.2-2.0 mol l(-1) HCl and pretreatment of SSD samples with 1.0-3.0 mol l(-1) HCl removed 96-100% and 76-80% of total Fe, respectively. Pretreatment declined overall paramagnetic characteristics of digestate samples, manifested by 50% (CD) and 70% (SSD) decrease in electron paramagnetic resonance signal intensities. As a result, meaningful solution-state H-1,C-13 heteronuclear single quantum coherence and H-1 NMR spectra of DMSO-d(6) soluble organic matter could be acquired. Sample pretreatment with the lowest concentration of HCl resulted in alteration of C:N ratios in solid phase, likely due to removal of labile organic and inorganic C- and N-containing compounds, while elevating the HCl concentration did not further change the C:N ratios. Furthermore, sample pretreatment increased the solubility of carbohydrates and proteins in DMSO-d(6), enabling the detection of NMR resonances from certain structural units of carbohydrates (e.g. anomeric O2CH) and proteins (e.g. CH alpha in amino acids). Both attenuation of the paramagnetic matrix as well as art enhanced solubility of carbohydrate and protein fractions of the samples in DMSO-d(6) solvent contributed to an improved molecular characterization of anaerobic digester samples by solution-state NMR analysis. 

Place, publisher, year, edition, pages
Elsevier, 2018
Keywords
Anaerobic digestion, Organic matter characterization, Solution-state NMR, Sample pretreatment, HCI
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-148628 (URN)10.1016/j.chemosphere.2018.02.015 (DOI)000428973200025 ()29438947 (PubMedID)
Available from: 2018-06-26 Created: 2018-06-26 Last updated: 2018-06-26Bibliographically approved
Talyzin, A., Mercier, G., Klechikov, A., Hedenström, M., Johnels, D., Wei, D., . . . Moons, E. (2017). Brodie vs Hummers graphite oxides for preparation of multi-layered materials. Carbon, 115, 430-440
Open this publication in new window or tab >>Brodie vs Hummers graphite oxides for preparation of multi-layered materials
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2017 (English)In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 115, p. 430-440Article in journal (Refereed) Published
Abstract [en]

Graphite oxides synthesized by one and two step Brodie oxidation (BGO) and Hummers (HGO) methods were analyzed by a variety of characterization methods in order to evaluate the reasons behind the difference in their properties. It is found that the Brodie method results in a higher relative amount of hydroxyl groups and a more homogeneous overall distribution of functional groups over the planar surface of the graphene oxide flakes. The higher number of carbonyl and carboxyl groups in HGO, detected by several methods, including XPS, NMR and FTIR, unavoidably results in defects of the graphene "skeleton", holes and overall disruption of the carbon-carbon bond network, stronger deviation from planar flake shape and poor ordering of the graphene oxide layers. It is also suggested that functional groups in HGO are less homogeneously distributed over the flake surface, forming some nanometer-sized graphene areas. The presence of differently oxidized areas on the GO surface results in inhomogeneous solvation and hydration of HGO and effects of inter- and intra-stratification. The proposed interpretation of the data explains the higher mechanical strength of multi-layered BGO membranes/papers, which are also less affected by humidity changes, thus providing an example of a membrane property superior to that of HGO.

Place, publisher, year, edition, pages
Elsevier, 2017
Keywords
graphite, oxide
National Category
Condensed Matter Physics
Research subject
Physics
Identifiers
urn:nbn:se:umu:diva-130949 (URN)10.1016/j.carbon.2016.12.097 (DOI)000395601300045 ()
Available from: 2017-02-01 Created: 2017-02-01 Last updated: 2018-06-09Bibliographically approved
Gillgren, T., Hedenström, M. & Jönsson, L. J. (2017). Comparison of laccase-catalyzed cross-linking of organosolv lignin and lignosulfonates. International Journal of Biological Macromolecules, 105(1), 438-446
Open this publication in new window or tab >>Comparison of laccase-catalyzed cross-linking of organosolv lignin and lignosulfonates
2017 (English)In: International Journal of Biological Macromolecules, ISSN 0141-8130, E-ISSN 1879-0003, Vol. 105, no 1, p. 438-446Article in journal (Refereed) Published
Abstract [en]

Lignin, an underutilized by-product from chemical pulping of wood, can be modified enzymatically through oxidation by laccase. However, little is known about the molecular details surrounding the cross linking which is a result of the oxidation. To reduce this lack of knowledge, we used oxygen consumption rate data, phenolic content data and molecular weight data together with data from NMR and FTIR spectroscopy to.characterize laccase-catalyzed cross-linking of the industrial lignin preparations organosolv lignin and lignosulfonate. The organosolv lignin preparation had a M-n of 780 g/mol, a M-w of 5200 g/mol, and a phenolic content of 1.8 mmol/g. The lignosulfonate preparation had a M-n of 6000 g/mol, a M-w of 19800 g/mol, and a phenolic content of 1.1 mmol/g. Laccase-catalyzed oxidation of organosolv lignin was characterized by a relatively slow increase in molecular weight, decreased intensities for aromatic signals and p-hydroxycinnamyl groups, and increased intensity for beta-O-4' signals, whereas oxidation of lignosulfonates resulted in a very rapid increase in molecular weight, and strongly decreased intensities for aromatic signals. The data suggest that lignosulfonates cross-linked by couplings to the aromatic ring (e.g. 5-5' and 4-O-5'), whereas beta-O-4' coupling characterized cross-linking of organosolv lignin, probably involving cinnamyl alcohol end-groups. (C) 2017 Published by Elsevier B.V.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE BV, 2017
Keywords
Lignin, Lignosulfonate, Organosolv, Laccase, Polymerization, Cross-link
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:umu:diva-143011 (URN)10.1016/j.ijbiomac.2017.07.061 (DOI)000414882900049 ()28711620 (PubMedID)
Projects
Bio4Energy
Available from: 2017-12-14 Created: 2017-12-14 Last updated: 2019-08-30Bibliographically approved
Pawar, P.-A. M., Ratke, C., Balasubramanian, V. K., Chong, S.-L., Gandla, M. L., Adriasola, M., . . . Mellerowicz, E. J. (2017). Downregulation of RWA genes in hybrid aspen affects xylan acetylation and wood saccharification. New Phytologist, 214, 1491-1505
Open this publication in new window or tab >>Downregulation of RWA genes in hybrid aspen affects xylan acetylation and wood saccharification
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2017 (English)In: New Phytologist, ISSN 0028-646X, E-ISSN 1469-8137, Vol. 214, p. 1491-1505Article in journal (Refereed) Published
Abstract [en]

High acetylation of angiosperm wood hinders its conversion to sugars by glycoside hydrolases, subsequent ethanol fermentation and (hence) its use for biofuel production. We studied the REDUCED WALL ACETYLATION (RWA) gene family of the hardwood model Populus to evaluate its potential for improving saccharification. The family has two clades, AB and CD, containing two genes each. All four genes are expressed in developing wood but only RWA-A and -B are activated by master switches of the secondary cell wall PtNST1 and PtMYB21. Histochemical analysis of promoter:: GUS lines in hybrid aspen (Populus tremula x tremuloides) showed activation of RWA-A and -B promoters in the secondary wall formation zone, while RWA-C and -D promoter activity was diffuse. Ectopic downregulation of either clade reduced wood xylan and xyloglucan acetylation. Suppressing both clades simultaneously using the wood-specific promoter reduced wood acetylation by 25% and decreased acetylation at position 2 of Xylp in the dimethyl sulfoxide-extracted xylan. This did not affect plant growth but decreased xylose and increased glucose contents in the noncellulosic monosaccharide fraction, and increased glucose and xylose yields of wood enzymatic hydrolysis without pretreatment. Both RWA clades regulate wood xylan acetylation in aspen and are promising targets to improve wood saccharification.

Keywords
Cas1p, Populus, REDUCED CELL WALL ACETYLATION, saccharification, wood acetylation, xylan, xylan etylation, xylem
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-137061 (URN)10.1111/nph.14489 (DOI)000402412500011 ()
Projects
Bio4Energy
Available from: 2017-06-26 Created: 2017-06-26 Last updated: 2019-08-30Bibliographically approved
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