Self-assembly of synthetic cellulose during in-vitro enzymatic polymerization process as studied by a combined small-angle scattering method

Tanaka, Hirokazu*; Koizumi, Satoshi; Hashimoto, Takeji; Kurosaki, Kazuhiro*; Kobayashi, Shiro*

We have investigated the self-assembling process of cellulose artificially synthesized via enzymatic polymerization as one of general problems of non-equilibrium phenomenon and pattern formation. The chemical reaction and the self-assembling process were explored at real time and in-situ by a combined small-angle neutron scattering (SANS), small-angle X-ray scattering (SAXS), ultra-SANS and ultra-SAXS method, together with wide-angle X-ray diffraction and field-emission scanning electron microscopy. The results revealed for the first time the following pieces of new evidence: (1) The enzymes (cellulase) as a catalyst aggregate themselves into associations; (2) Cellulose molecules created at each active site of enzymes associate themselves around the enzyme associations into cellulose aggregates having surface fractal dimensions Ds, increasing from 2 to 2.3 with reaction time. (3) The fractal structure formed at the end of the reaction extends over a surprisingly wide length scale ranging from 30 nm to 30 m (3 orders of magnitude).