Probing the early events associated with liquid ammonia pretreatment of native crystalline cellulose

Giovanni Bellesia, Shishir P.S. Chundawat, Paul Langan, Bruce E. Dale, S. Gnanakaran

Research output: Contribution to journalArticlepeer-review

32 Scopus citations

Abstract

Various chemicals are being explored for catalyzing efficient lignocellulose deconstruction. In particular, when liquid ammonia is used to convert the naturally occurring cellulose crystalline phase Iβ, to cellulose IIII, the rearrangement of the hydrogen bond network in cellulose IIII results in enhanced hydrolysis yields. We use molecular dynamics simulations to analyze the interaction between a cellulose Iβ fibril and ammonia. Our simulations reveal that early structural changes in the fibril are driven by the rapid formation of an extended hydrogen bond network between the solvent-exposed surface chains and ammonia that precedes ammonia penetration into the fibril. The emergence of this hydrogen bond network causes relative shifting of the cellulose layers within the fibril that in turn leads to the formation of channels orthogonal to the (100) and (-100) fibril surfaces. The channels allow ammonia molecules to penetrate into the cellulose fibril. These findings provide avenues for improving existing chemical pretreatments to make them more effective and economical.

Original languageEnglish
Pages (from-to)9782-9788
Number of pages7
JournalJournal of Physical Chemistry B
Volume115
Issue number32
DOIs
StatePublished - Aug 18 2011

Fingerprint

Dive into the research topics of 'Probing the early events associated with liquid ammonia pretreatment of native crystalline cellulose'. Together they form a unique fingerprint.

Cite this