近日，由我组撰写的专题综述 “Towards Efficient Chemical Synthesis via Engineering Enzyme Catalysis in Biomimetic Nanoreactors” (Jia Liu, Qihua Yang, and Can Li, Chem. Commun., 2015, 51, 13731-13739.) 在Chemical Communications上发表，并被选为当期封面文章。
长期以来，研究者们对酶这种高催化活性、高选择性及反应条件温和的生物催化剂给予厚望，认为其有希望取代传统化学催化剂实现高效绿色催化转化。但是，如何在生物体外维持细胞内酶分子本征的优异催化性能是将生物催化剂应用于实际化工生产的一大挑战。针对这一难题，我组提出了“在载体纳米孔内模拟细胞内酶分子的微环境”的解决方案，并围绕这一构想从2003起开展了一系列研究工作，相关成果相继在Chem. Sci.、 Chem. Commun.、 Chem. Eur. J.、 Langmuir等杂志上发表。
本专题综述比较系统地总结了我组在构建高效生物催化剂方面的研究进展，并重点阐述了在载体纳米孔内模拟细胞内酶分子工作环境及工作模式的重要性。研究结果表明，以细胞内微环境为指导，通过特定有机物、聚合物对介孔氧化硅载体进行修饰，可从化学性质及物理性质两方面对纳米孔内酶分子的微环境进行优化，从而显著提高酶在生物体外的催化活性及稳定性。此外，将多种酶或酶与其他催化物种同时限域在纳米孔内催化串联反应，可对细胞内酶分子协同催化的工作方式实现有效模拟，从而进一步提高催化效率。该综述文章中提出的观点得到了国际同行的认可与肯定， 发表后被Faculty of 1000推荐为本领域具有特殊重要意义的论文（“of special significance in its field”）。
本工作得到了国家自然科学基金及中国科学院重点资助项目的支持。 （文/图 刘佳）
Towards Efficient Chemical Synthesis via Engineering Enzyme Catalysis in Biomimetic Nanoreactors
A feature article entitled “Towards Efficient Chemical Synthesis via Engineering Enzyme Catalysis in Biomimetic Nanoreactors” has been recently published online in the journal of Chemical Communications (Jia Liu, Qihua Yang, and Can Li, Chem. Commun., 2015, 51, 13731-13739), and featured on the outside front cover of the same issue.
Biocatalysis with immobilized enzymes as catalysts holds enormous promise in developing more efficient and sustainable process for the synthesis of various valuable chemicals. However, how to maintain the extraordinary catalytic performance of enzymes in cells under in vitro conditionis a key challenging issue seriously hampering the industrial-scale application of biocatalysts. To deal with this problem, a strategy focusing on mimicking the intracellular microenvironment of enzymes in support nanopores was put forward by our research group. Based on which, a series of research work has been carried out since 2003 and the corresponding outcomes have been published in the journals of Chem. Sci., Chem. Commun., Chem. Eur. J. and Langmuir, etc.
The recently published feature article has systematically summarized the research progress we have made in this area. A special emphasis was given to clarifying the importance of simulating the working environment and working patterns of intracellular enzymes in support nanopores. Research results have demonstrated that by modifying the mesoporous silica support with suitable organic moieties or polymers, it is possible to optimize the chemical as well as spatial microenvironment surrounding the enzyme molecules in nanopores in the light of the situation within intracellular environment. And this could be a useful approach to notably improve the catalytic activity and stability of biocatalysts in vitro. Besides that, confining multiple enzymes or enzyme and other catalytic entities inside nanopores is appealing for mimicking the ingenious array of multienzymatic systems in cells to catalyze cascade reactions with enhanced overall efficiency. The research concept underpinned in this feature article has soon received the attention of other researchers, and has been recommended in F1000Prime “as being of special significance in its field” by Faculty of 1000.
This work was supported by the National Natural Science Foundation of China and the Key Research Program of Chinese Academy of Sciences.
(By Jia Liu)
Newly published paper
The paper "Polystyrene sulphonic acid resins with enhanced acid strength via macromolecular self-assembly within confined nanospace "has been accepted by Nature Communications, doi:10.1038/ncomms4170.
The paper "Enzyme confined in silica-based nanocages for biocatalysis in a Pickering emulsion "has been accepted by Chem.Commun, DOI: 10.1039/c3cc45476b.
The paper "Mesoporous graphitic carbon nanodisks fabricated via catalytic carbonization of coordination polymers. "has been accepted by Chem.Commun, DOI: 10.1039/C2CC34234K.
The paper "Yolk-Shell Nanoreactor with Basic Core and Acidic Shell for Cascade Reactions."has been accepted by Angewandte Chemie International Edition, DOI: 10.1002/ange.201204829.
The paper "Oxygen evolution from water oxidation on molecular catalysts confined in the nanocages of mesoporous silicas. "has been published on Energy Environ.Sci. ASAP. DOI: 10.1039/C2EE22059H.
The paper "Promoted activity of Cr(Salen) in a nanoreactor for kinetic resolution of terminal epoxides."has been published on Chemical Science , DOI: 10.1039/C2SC20653F.
Professor Yang is awarded "China Young Women Scientists' Awards"
China Young Women Scientists' Award was jointly set up by the All-China Women's Federation, the China Association for Science and technology,the Chinese National Commission for UNESCO and L'Oreal (China) Ltd. The purpose of the award is to honor young women who have made important and innovative achievements in all fields of science, stimulate enthusiasm among the nation's young women scientists to contribute to the aim of building a well-off society in an all-round way, and encourage more women scientists to engage themselves in natural science research.
State Key Laboratory of Catalysis, SKLC
Dalian Institute of Chemical Physics,DICP
Chinese Academy Sciences, CAS
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