Sahlin Jenny, Wu Congyu, Buscemi Andrea, Schärer Claude, Nazemi Seyed Amirabbas, S K Rejaul, Herrera-Reinoza Nataly, Jung Thomas A, Shahgaldian Patrick
Institute of Chemistry and Bioanalytics, School of Life Science, University of Applied Sciences and Arts Northwestern Switzerland Hofackerstrasse 30 Muttenz CH-4132 Switzerland
Institute of Physics, University of Basel Klingelbergstrasse 82 Basel CH-4056 Switzerland.
Nanoscale Adv. 2023 Sep 1;5(18):5036-5044. doi: 10.1039/d3na00413a. eCollection 2023 Sep 12.
The major stumbling block in the implementation of oxidoreductase enzymes in continuous processes is their stark dependence on costly cofactors that are insoluble in organic solvents. We describe a chemical strategy that allows producing nanobiocatalysts, based on an oxidoreductase enzyme, that performs biocatalytic reactions in hydrophobic organic solvents without external cofactors. The chemical design relies on the use of a silica-based carrier nanoparticle, of which the porosity can be exploited to create an aqueous reservoir containing the cofactor. The nanoparticle core, possessing radial-centred pore channels, serves as a cofactor reservoir. It is further covered with a layer of reduced porosity. This layer serves as a support for the immobilisation of the selected enzyme yet allowing the diffusion of the cofactor from the nanoparticle core. The immobilised enzyme is, in turn, shielded by an organosilica layer of controlled thickness fully covering the enzyme. Such produced nanobiocatalysts are shown to catalyse the reduction of a series of relevant ketones into the corresponding secondary alcohols, also in a continuous flow fashion.
在连续过程中应用氧化还原酶的主要障碍是它们对昂贵且不溶于有机溶剂的辅因子的严重依赖。我们描述了一种化学策略，该策略能够制备基于氧化还原酶的纳米生物催化剂，其可在无外部辅因子的疏水性有机溶剂中进行生物催化反应。这种化学设计依赖于使用基于二氧化硅的载体纳米颗粒，其孔隙率可用于创建一个包含辅因子的水相储存库。具有径向中心孔道的纳米颗粒核心用作辅因子储存库。它进一步被一层孔隙率降低的层覆盖。这一层作为固定所选酶的支撑，同时允许辅因子从纳米颗粒核心扩散。反过来，固定化酶被一层厚度可控的有机硅层完全覆盖，从而得到保护。这种制备的纳米生物催化剂还能够以连续流动的方式催化一系列相关酮还原为相应的仲醇。
