State Key Laboratory of Food Nutrition and Safety, Laboratory of Industrial Fermentation Microbiology, Ministry of Education, Tianjin University of Science and Technology, No 29, 13th, Avenue, Tianjin Economic and Technological Development Area (TEDA), Tianjin 300457, China.
School of Life Science and Food Engineering, Huaiyin Institute of Technology, Huaian 223003, China.
Int J Biol Macromol. 2020 Jul 15;155:110-118. doi: 10.1016/j.ijbiomac.2020.03.177. Epub 2020 Mar 24.
Multienzymatic conversion of carbon dioxide (CO) into chemicals has been extensively studied. However, regeneration and reuse of co-factor are still the main problems for the efficient conversion of CO. In this study, a nanoscale multienzyme reactor was constructed by encapsulating simultaneously carbonic anhydrase (CA), formate dehydrogenase (FateDH), co-factor (NADH), and glutamate dehydrogenases (GDH) into ZIF-8. In the multienzyme reactors, cationic polyelectrolyte (polyethyleneimine, PEI) was doped in the ZIF-8 by dissolving it in the precursors of ZIF-8. Co-factor (NADH) was anchored in ZIF-8 by ion exchange between PEI (positive charge) and co-factor (negative charge), and regenerated through GDH embedded in the ZIF-8, thus keeping high activity of FateDH. Activity recovery of FateDH in the multienzyme reactors reached 50%. Furthermore, the dissolution of CO in the reaction solution was increased significantly by the combination of CA and ZIF-8. As a result, the nanoscale multienzyme reactor exhibited superior capacity for conversion of CO to formate. Compared with free multienzyme system, formate yield was increased 4.6-fold by using the nanoscale multienzyme reactor. Furthermore, the nanoscale multienzyme reactor still retained 50% of its original productivity after 8 cycles, indicating excellent reusability.
二氧化碳(CO)的多酶转化已得到广泛研究。然而,辅因子的再生和再利用仍然是 CO 高效转化的主要问题。在这项研究中,通过将碳酸酐酶(CA)、甲酸脱氢酶(FateDH)、辅因子(NADH)和谷氨酸脱氢酶(GDH)同时包封到 ZIF-8 中,构建了纳米级多酶反应器。在多酶反应器中,通过将其溶解在 ZIF-8 的前体中,将阳离子聚合物(聚乙烯亚胺,PEI)掺杂到 ZIF-8 中。辅因子(NADH)通过 PEI(正电荷)与辅因子(负电荷)之间的离子交换锚定在 ZIF-8 中,并通过嵌入 ZIF-8 中的 GDH 再生,从而保持 FateDH 的高活性。多酶反应器中 FateDH 的活性恢复达到 50%。此外,CA 和 ZIF-8 的结合显著增加了反应溶液中 CO 的溶解。结果,纳米级多酶反应器表现出将 CO 转化为甲酸盐的卓越能力。与游离多酶体系相比,使用纳米级多酶反应器将甲酸盐的产率提高了 4.6 倍。此外,纳米级多酶反应器在 8 个循环后仍保留其原始生产力的 50%,表明其具有出色的可重复使用性。