HKUST-1 catalyzed efficient in situ regeneration of NAD(+) for dehydrogenase mediated oxidation
HKUST-1 catalyzed efficient in situ regeneration of NAD(+) for dehydrogenase mediated oxidation
复制标题
HKUST-1 催化 NAD( ) 有效原位再生，用于脱氢酶介导的氧化
DOI：
10.1016/j.ces.2019.03.076
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发表时间：
2019
影响因子：
4.7
通讯作者：
Jiang Yanbin
中科院分区：
文献类型：
--
作者：
Xia Huan;Li Zhixian;Zhong Xue;Li Binghui;Jiang Yunpeng;Jiang Yanbin
几十年来，结合酶和化学反应来实现化学-酶协同过程提出了许多挑战。本研究将乙醇脱氢酶（ADH）通过anin - situapproach封装到金属-有机框架hust -1晶体中，构建了一个协同的化学和生物催化体系，其中ADH负责将苯甲醇转化为苯甲醛，hust -1负责氧化辅因子β-烟酰胺腺嘌呤二核苷酸（NAD+）的再生。发现HKUST-1是一种多功能催化剂，可在不同缓冲液中有效氧化NADH。与游离ADH相比，固定化ADH的Michaelis-Menten动力学参数增加了KM（约1.3倍），降低了Vmax（约4.7倍）。由于HKUST-1的保护，固定化酶对尿素和有机溶剂的抗性比游离酶强，6个循环后仍保持93%的活性。将固定化酶成功地应用于常温条件下苯甲醇转化为苯甲醛。由于HKUST-1的氧化辅因子再生，ADH@HKUST-1复合材料的苯甲醛产率达到28.5%，比单个生物催化的产率高约4.3倍。这种化学催化与生物催化相结合的概念可能为生物化学催化、生物传感器和药物传递等领域的应用提供一种新颖而通用的技术。
The combination of enzymatic and chemical reactions to achieve co-operative chemo-enzymatic processes has presented many challenges for decades. In this work, alcohol dehydrogenase (ADH) was encapsulated into metal-organic framework HKUST-1 crystals through anin situapproach to construct a synergistic chemo- and bio-catalysis system, where ADH was for the conversion of benzyl alcohol to benzaldehyde, and HKUST-1 was in charge for the regeneration of β-nicotinamide adenine dinucleotide (NAD+, the oxidized cofactor). It was found that HKUST-1 was a versatile catalyst for efficient oxidation of NADH in different buffers. The Michaelis-Menten kinetic parameters of immobilized ADH exhibited an increased KM(approximately 1.3-fold) and a decreased Vmax(approximately 4.7-fold) compared to free ADH. Due to the protection of HKUST-1, the immobilized enzyme showed a better resistance against urea and organic solvents compared with free enzyme, and still maintained 93% of its original activity after 6 cycles. The immobilized enzyme was successfully applied to the enzymatic transformation of benzyl alcohol to benzaldehyde in aqueous media at room temperature. Owing to the oxidized cofactor regeneration by HKUST-1, ADH@HKUST-1 composites achieved a benzaldehyde yield of 28.5%, which was approximately 4.3-fold higher than that of the individual bio-catalysis. This concept of combining chemo- and bio-catalysis may provide a novel and versatile technique for applications in biochemical catalysis, biosensors and drug delivery.