PNNL

Abstract

: Hierarchically ordered mesocellular mesoporous silica materials (MMS) were synthesized using a single structure directing agent under neutral conditions for the first time. The mesocellular pores are synthesized without adding any pore expander, and the walls of cellular pores in MMS are composed of SBA-15 type mesopores. The small-angle X-ray scattering (SAXS) pattern of MMS revealed the presence of ordered pore structures with two different length scales. The current MMS possesses four different pore systems; complementary micro/mesopores, main 13 nm mesopores, 40 nm mesocellular spherical pores, and textural inter-particle macropores. Nanometer-scale enzyme reactors (NER) were developed in mesocellular mesoporous silica (MMS) via a ship-in-a-bottle approach, which employs adsorption of enzymes followed by cross-linking using glutaraldehyde (GA) treatment. The resulting NER show an impressive stability and activity with an extremely high loading of enzymes. For example, NER containing a-chymotrypsin (NER-CT) could hold 0.5 g CT in 1 g of silica, but the specific activity of NER-CT was 10.4 times higher than that of the adsorbed CT with a lower loading (0.07 g CT per 1 g of silica), which was further decreased by a continuous leaching of adsorbed CT. NER-CT showed excellent stability without any leaching, i.e. no activity decrease at all in a rigorously-shaking condition for two weeks (a half-life with 3.8 years), while the conventional adsorption method resulted in a half-life of 3.6 days in the same condition.