Abstract
In this work, we present a new coarse-grained (CG) model that captures the directional hydrogen bonding interactions that drive cellulose chains to assemble into ordered aggregates. This CG model balances the incorporation of chemical details at the monomer level needed to represent directional interactions and the coarse-graining needed to capture large length scales and time scales associated with macromolecular assembly. We validate this CG model by first comparing the cellulose single-chain structure in the CG molecular dynamics (MD) simulations with that in atomistic MD simulations. We also compare the hydrogen bonding pattern, interchain distance, and interchain orientation seen in assembled cellulose chains observed in CG MD simulations with those seen in experimental crystal structures of cellulose. Upon validation, we present the aggregation behavior of cellulose chains with "silenced"hydrogen bonding site interactions to mimic cellulose chains that are chemically modified at the donor and acceptor hydrogen bonding sites (e.g., methylcellulose). We expect this type of CG model to be useful in predicting the morphology of cellulose chains in solution under a wide range of solution conditions and chemical modifications.
| Original language | English |
|---|---|
| Pages (from-to) | 4599-4614 |
| Number of pages | 16 |
| Journal | Journal of Chemical Theory and Computation |
| Volume | 16 |
| Issue number | 7 |
| DOIs | |
| State | Published - Jul 14 2020 |
| Externally published | Yes |
Funding
The authors acknowledge financial support from the U.S. Department of Energy, Office of Science, Grant DE-SC0017753. The computational work in this article was supported by the Farber Higher-Performance Supercomputing Center at the University of Delaware. The authors also thank D. Intriago for input during the early stages of this model development.