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Fig. 1 Composition of lignocellulosic biomass and the structural roles of cellulose, hemicellulose, and lignin. 46

Fig. 2 Monolignol structure and positions indicated by blue numbers and letters.

so  woods and hardwoods, respectively. As this is the most common linkage, many deligni  cation processes target this speci  c linkage. For so  woods, the 5 – 5 linkage is also impor- tant, and has an abundance of 18 – 25% per 100 C 9 units, while this linkage occurs only around 3 – 9% in hardwoods. 52 In the process of isolating technical lignins, both the labile aryl-alkyl and b -O-4 bonds are most prone to cleavage. 53 This results in technical lignins having more condensed and variable structures than native lignin, and a wide variety in molecular weight ( M w ). Mass average values ( M w ) of 1000 – 15000 gmol − 1 for soda lignin, 1500 – 25000gmol − 1 forKra  lignin, and 1000 – 150 000 g mol − 1 for lignosulfonates have been reported, depending on botanical origin and process conditions. 54 Native lignin is a virtually in  nite macromer that is both randomly- and poly-branched. 55 The bonds between the lignin and surrounding hemicellulose and cellulose found in LCC have recently been reviewed. 56 All so  wood lignin, and 47 – 66% of hardwood lignin, is reportedly bound covalently to carbohy- drates, and mainly to hemicellulose. The most common types of linkages found in LCCs are benzyl ether-, benzyl ester-, ferulate ester-, phenyl glycosidic- and diferulate ester bonds. 57 Note that due to the high degree of variability in inter-unit and LCC

radical cross-coupling reactions which results in the complex, and varied, lignin network. The ratios of the three monolignols in lignin from di ff erent sources can vary quite signi  cantly, hardwood lignins contain G- (25 – 50%) and S-units (50 – 70%), so  wood lignins contain mostly G-units (80 – 90%), while grass lignin contains mixtures of S- (25 – 50%), G- (25 – 50%) and H- units (10 – 25%). 49 The monolignol composition (H : G : S ratio) can also vary between tissue types in the same organism, which has been illustrated in the cork oak, Quercus suber . Lignin from the xylem (1 : 45 : 55) and phloem (1 : 58 : 41) di ff er less in composition than the two compared to the phellem (cork-part, 2 : 85 : 13). These di ff erences a ff ect the occurrence of speci  c interunit linkages, where an increase in S-units lead to an increase in alkyl – aryl ether ( b -O-4) bonds: 68% in cork, 71% in phloem, 77% in xylem. 50 The di ff erence in abundance of the three monolignols lead tomany di ff erent types of interunit linkages in lignin, speci  - cally between angiosperm (hardwood and grass) and gymno- sperm(so  wood) lignin. 51 The most common interunit linkage is the b -O-4alkyl – aryl ether bond (Fig. 3), which occurs between 45 – 50% or 60 – 62% of phenyl propylene unit (C 9 units) in

RSCAdv. , 2023, 13 , 12529 – 12553 | 12531

© 2023 The Author(s). Published by the Royal Society of Chemistry

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