NEUTRON AND SYNCHROTRON X-RAY FIBER DIFFRACTION STUDIES OF CELLULOSE POLYMORPHS.
Although the crystalline nature of cellulose has been one of most studied structural problems in polymer science there remain many open questions. Cellulose is a polymer formed by (1-4)-linked {beta}-D-glucosyl residues that are alternately rotated by 180o along the polymer axis to form flat ribbon-like chains. Each glucosyl unit bears three hydroxyl groups, one an hydroxymethyl group. It has been long recognized that these hydroxyl groups and their ability to bond via hydrogen bonding not only play a major role in directing how the crystal structure of cellulose forms but also in governing important physical properties of cellulose materials. Through the development of new techniques we have been able to prepare fiber samples of cellulose with exceptionally high order. The quality of these samples is allowing us to exploit the unique properties of synchrotron X-ray and neutron sources in order to collect diffraction data to near atomic resolution. Synchrotron X-rays are used to provide accurate crystallographic parameters for C and O atoms. However, because of the relatively weak scattering power of H atoms for X-rays, neutrons are used to determine H atom parameters. We have developed methods for replacing labile H atoms with D, without any loss in crystalline perfection. Deuterated fibers can diffract neutrons with intensities that are substantially different from the intensities diffracted from hydrogenated fibers. These differences, along with the phases calculated from the C and O positions determined in our X-ray studies, are used to calculate Fourier difference syntheses in which density associated with labile hydrogen atoms is imaged. The unprecedented high resolution of these data is revealing new information on cellulose structure and hydrogen bonding.
- Research Organization:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- USDOE
- OSTI ID:
- 975877
- Report Number(s):
- LA-UR-01-6470; TRN: US1006809
- Resource Relation:
- Conference: Submitted to: "Polymer Reprints," A publication of the American Chemical Society for 2002 Annual Meeting
- Country of Publication:
- United States
- Language:
- English
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