Chemico-biological conversion of carbon dioxide

The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of“peak shaving”and C-neutrality,contributing significantly to our collective efforts to combat climate change and its associated challenges.

Cell-free biocatalysis coupled with photo-catalysis and electro-catalysis: Efficient CO_(2)-to-chemical conversion

The increasing atmospheric carbon dioxide (CO_(2)) concentration has exposed a series of crises in the earth's ecological environment.How to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many researchers.Cell-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent years.In this review,the research progresses of photoenzyme catalysis,electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically summarized.We focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems,especially the materials used in the construction of the coupling system,and analyze and point out the characteristics and possible problems of different coupling methods.Finally,we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO_(2) fixation,suggesting possible strategies to improve the carbon sequestration capacity of such systems.

点击化学作为分子连接工具:机遇与挑战

2022年诺贝尔化学奖授予点击化学以及生物正交化学领域的三位科学家,显示了点击化学在当代合成领域的重要地位.点击化学本质是一类连接反应,旨在通过将不同单元分子高效地拼接在一起,最终得到具有特定结构与功能的分子.在传统有机化学中,碳碳键的合成通常具有较大难度,因为它们涉及较低的化学驱动力和较多的副反应.点击化学强调开发基于碳杂原子键的新型组合化学反应,并通过这些反应简单有效地获得多样性分子.点击化学的发展将科学家们从复杂、专业性强的有机合成中解放出来,使他们可以专注于分子功能的开发,一定程度拓宽了合成化学的应用范围.基于点击化学的优越性能,其在聚合物合成以及生物医学等领域表现出了非常广泛的应用前景.本文简要概述了几种涉及不同底物和催化剂类型的典型点击反应,并尝试解释这一领域背后的发展逻辑.此外,阐述了点击化学在现代科学,尤其是聚合物合成和生命科学等领域的应用,及其目前存在的局限性和未来可能的发展方向.点击反应的主要特征包括产率高、选择性好、副产物无害且易分离、反应条件简单、原料易得、符合原子经济性和应用范围广等.典型的点击化学包括亲核开环反应、环加成反应、保护基反应、碳碳多键加成反应和施陶丁格反应等,这些反应大多在点击化学概念提出之前就已被开发.通过改变反应条件,选择合适的底物和催化剂,这些反应可以更加满足点击标准.而随着点击化学在生命科学领域的应用,不依赖于催化剂的反应逐渐受到重视,因为他们更有希望在生物体内保持点击活性.环应力可以在无催化剂存在下有效改善反应动力学,针对底物分子应力的研究成为了点击化学领域的重点.此外,近年来光催化点击反应和解离反应也受到广泛关注,这些“智能”点击反应可以提供有效的时空控制、可逆的连接-释放过程,代表了点击化学新的突破.在应用方面,点击化学可以提供高原子经济性的分子合成方法,因而被广泛用于聚合物的合成,它也为聚合物的功能修饰提供了简便方法.然而在生命科学领域,无催化剂反应显然更有利于生理环境下的分子合成,这也体现了点击化学背后受应用驱动的发展逻辑.当然,不同应用场景也为点击反应提出了新要求.本文强调了生物相容性、可扩展性以及智能化会是点击化学未来发展面临的主要挑战,需要深入研究点击化学在复杂应用场景中的反应机制,引入计算机技术帮助提高可扩展性,以及开发光、磁等物理因素控制的反应类型.相信通过新理论、新技术的引入,点击化学领域将会取得更大的突破.

Physical stimuli-responsive cell-free protein synthesis

Cell-free protein synthesis has been developed as a critical platform in synthetic biology.Unlike the cell-based synthesis system,cell-free system activates transcriptional and translational mechanisms in vitro,and can control protein synthesis by artificially adding components or chemicals.However,the control method puts forward higher requirements in terms of accurate and non-toxic control,which cannot be achieved by chemical substances.For cell-free system,physical signal is a kind of ideal spatiotemporal control approach to replace chemical substances,realizing high accuracy with little side effect.Here we review the methods of using physical signals to control gene expression in cell-free systems,including studies based on light,temperature,electric field,and magnetic force.The transfer of these switches into cell-free system further expands the flexibility and controllability of the system,thus further expanding the application capability of cell-free systems.Finally,existing problems such as signal source and signal transmission are discussed,and future applications in pharmaceutical production,delivery and industrial production are further looked into.