当前位置: X-MOL 学术ACS Omega › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Oxazolidine Transient Bases as Molecular Platforms for Testing Dynamic CO2 Capture in Biochemical Systems
ACS Omega ( IF 4.1 ) Pub Date : 2018-03-09 00:00:00 , DOI: 10.1021/acsomega.7b02028
Lan Sheng , Qiaonan Chen , Chunyu Wang , Hongwei Chen 1 , Ting Zhang , Tianyou Qin , Minjie Li , Jinyan Zhang , Jing Ma 1 , Sean Xiao-An Zhang
Affiliation  

Understanding the dynamic processes of CO2 capture in biosystems is important because of the great effect CO2 has on the carbon cycle, human health, the global climate, and living environments. After years of multidisciplinary studies, researchers have gained only basic mechanistic knowledge about how enzymes or protein-aggregates capture and deliver CO2, a process involving reversible bonding of CO2 with basic amino acid residues. However, vital mechanistic details of how the activated basic residues within these enzymes or protein-aggregates are initially formed, a crucial step for CO2 capture, are still lacking. Herein, we designed specific molecules, i.e., oxazolidines, which are able to reversibly change their alkalinity via ultrafast isomerizations. Serving as so-called transient bases, these oxazolidines mimic the activated/deactivated states of enzymes or protein-aggregates responsible for dynamic CO2 capture/release. A detailed mechanism for CO2 capture, which involves dynamic covalent bonding and multimolecular cooperative interactions among functional groups that occur with the help of a polyhydroxyl environment, is demonstrated by UV−vis and multiple NMR spectroscopies as well as theoretical calculations. Using suitable oxazolidine transient bases, applications for visual CO2 detection under different detection limit requirements were also developed. Insights for further understanding the process of dynamic CO2 capture in biosystems are also discussed. This oxazolidine-inspired biomimetic CO2 capture serves as a platform for the future development of additional biomimicking systems, as well as offers unique perspectives for other complicated life processes.

中文翻译:

恶唑烷瞬态碱作为在生物化学系统中测试动态CO 2捕集的分子平台

了解CO 2在生物系统中捕获的动态过程非常重要,因为CO 2对碳循环,人类健康,全球气候和生活环境具有重大影响。经过多年的多学科研究,研究人员仅获得了有关酶或蛋白质聚集体如何捕获和传递CO 2的基本机械知识,该过程涉及将CO 2与碱性氨基酸残基可逆结合。但是,如何初步形成这些酶或蛋白质聚集体中活化的碱性残基的重要机理细节,这是CO 2的关键步骤捕获,仍然缺乏。在这里,我们设计了特定的分子,即恶唑烷,它们能够通过超快异构化可逆地改变其碱度。这些恶唑烷用作所谓的瞬时碱基,模仿负责动态CO 2捕获/释放的酶或蛋白质聚集体的活化/失活状态。UV-vis和多个NMR光谱以及理论计算证明了CO 2捕集的详细机制,其中涉及在多羟基环境的帮助下发生的动态共价键合和官能团之间的多分子协作相互作用。使用合适的恶唑烷瞬变碱,用于可视CO 2的应用还开发了不同检出限要求下的检出。还讨论了进一步了解生物系统中动态CO 2捕获过程的见解。该恶唑烷酮启发的仿生CO 2捕集装置为未来其他仿生系统的开发提供了平台,并为其他复杂的生命过程提供了独特的见解。
更新日期:2018-03-09
down
wechat
bug