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文章编号： 1672-6987（2023）06-0038-10； DOI： 10.16351/j.1672-6987.2023.06.004
董文锦1， 邓理2， 宋晓明1， 陈夫山1*(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)
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。
关键词： 辅酶； 甲醛脱氢酶； NADH再生； 甲酸盐
中图分类号： Q 814.9文献标志码： A
引用格式： 董文锦， 邓理， 宋晓明， 等. 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［J］. 青岛科技大学学报(自然科学版), 2023, 44（6）： 38-47.
DONG Wenjin， DENG Li， SONG Xiaoming， et al. Feasibility study on production of methanol catalyzed by photocatalytic coenzyme regeneration system coupling with formaldehyde dehydrogenase［J］. Journal of Qingdao University of Science and Technology（Natural Science Edition), 2023， 44（6）： 38-47.
Feasibility Study on Production of Methanol Catalyzed by Photocatalytic
Coenzyme Regeneration System Coupling with Formaldehyde Dehydrogenase
DONG Wenjin1， DENG Li2， SONG Xiaoming1， CHEN Fushan1
(1. College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China;
2. Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China)
Abstract: 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 enzyme catalyzed in previous reports was most likely not using NADH as a reducing agent.
Key words: coenzyme; formaldehyde dehydrogenase; NADH regeneration; formate
收稿日期： 2023-04-09
基金项目： 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).
作者简介： 董文锦（1995-），女，博士研究生.*通信联系人.
