Abstract
BackgroundSubstrate accessibility to catalysts has been a dominant theme in theories of biomass deconstruction. However, current methods of quantifying accessibility do not elucidate mechanisms for increased accessibility due to changes in microstructure following pretreatment.ResultsWe introduce methods for characterization of surface accessibility based on fine-scale microstructure of the plant cell wall as revealed by 3D electron tomography. These methods comprise a general framework, enabling analysis of image-based cell wall architecture using a flexible model of accessibility. We analyze corn stover cell walls, both native and after undergoing dilute acid pretreatment with and without a steam explosion process, as well as AFEX pretreatment.ConclusionImage-based measures provide useful information about how much pretreatments are able to increase biomass surface accessibility to a wide range of catalyst sizes. We find a strong dependence on probe size when measuring surface accessibility, with a substantial decrease in biomass surface accessibility to probe sizes above 5–10 nm radius compared to smaller probes.
Highlights
Substrate accessibility to catalysts has been a dominant theme in theories of biomass deconstruction
Substrate accessibility to catalysts has been a dominant theme in biomass deconstruction and several groups have concluded that enabling the accessibility of the biopolymers of plant cell walls remains the single most important challenge of biomass deconstruction [3,4,5,6]
Our results indicate that image-based surface accessibility provides a useful quantification of accessibility of biomass to catalyst
Summary
Substrate accessibility to catalysts has been a dominant theme in theories of biomass deconstruction. The most commonly used catalyst system for biomass deconstruction is the small, secreted enzymes from cellulolytic fungi, such as Trichoderma reesei [8] These enzymes range from 10–12 nm in their largest dimensions. Recent work has used solute exclusion to probe the changes in porosity caused by dilute acid pretreatment [17] Another commonly used technique is Simons’ stain, which employs two differently sized molecular stains in tandem to interrogate the range of accessibility created in pretreated materials [18]. An overview of these and more recent methods involving NMR and mercury intrusion has been reported by Meng and Ragauskas [19]
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