光催化辅酶再生体系与甲醛脱氢酶耦合制备甲醇的可行性研究  

Feasibility Study on Production of Methanol Catalyzed by Photocatalytic Coenzyme Regeneration System Coupling with Formaldehyde Dehydrogenase

作　　者：董文锦 邓理 宋晓明[1] 陈夫山[1] DONG Wenjin;DENG Li;SONG Xiaoming;CHEN Fushan(College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao 266042,China;Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 730000,China)

机构地区：[1]青岛科技大学化工学院,山东青岛266042 [2]中国科学院兰州化学物理研究所,中国兰州730000

出　　处：《青岛科技大学学报（自然科学版）》2023年第6期38-47,共10页Journal of Qingdao University of Science and Technology:Natural Science Edition

基　　金：国家自然科学基金项目(22078167);山东省重大创新工程项目(2018CXGC1001);山东省教育厅青创团队项目(2019KJC008);青岛市西海岸重大创新工程项目(2019-27);山东省科技攻关项目(2019JZZY020213)。

摘　　要：为实现温和条件下甲醛或甲醇的制备,对光催化辅酶再生体系与甲醛脱氢酶(FaldDH)耦合进行了研究,提出了以甲酸歧化方式制备甲醛、甲醇的新方法。该方法将光催化NADH再生体系与甲醛脱氢酶、醇脱氢酶耦合,不过未检测到甲醛或甲醇。通过实验对结果进行验证,考察了FaldDH催化甲酸盐还原制备甲醛的反应的影响因素,并通过平衡反应、结合已有文献报道给出了合理的解释。结果表明:受热力学反应平衡限制,反应条件下生成的甲醛量低于Nash显色法定量甲醛的检测限,以往报道中酶催化生成的甲醛极有可能未利用NADH作为还原剂。In order to realize the synthesis of formaldehyde or methanol under mild conditions,the coupling of photocatalytic coenzyme regeneration system with formaldehyde dehydrogenase(FaldDH)was studied,and a new method for preparing formaldehyde and methanol by formic acid disproportionation was proposed.The photocatalytic NADH regeneration system was coupled with formaldehyde dehydrogenase and alcohol dehydrogenase,and no formaldehyde or methanol was detected.Through designed experiments,the influencing factors of enzymatic reaction were investigated.A reasonable explanation was given by the equilibrium reaction and the existing literature reports.The results show that limited by the equilibrium of the thermodynamic reaction,the amount of formaldehyde generated under the reaction conditions was lower than detection limit.The formaldehyde generated by the en-zyme catalyzed in previous reports was most likely not using NADH as a reducing agent.

关 键 词：辅酶 甲醛脱氢酶 NADH再生 甲酸盐 

分 类 号：Q814.9[生物学—生物工程]