Department of Chemistry, Emory University Atlanta, Georgia 30322, United States.
Department of Biological Chemistry, University of Michigan, Ann Arbor, Michigan 48109-0606, United States.
J Phys Chem Lett. 2022 Jun 23;13(24):5553-5556. doi: 10.1021/acs.jpclett.2c01412. Epub 2022 Jun 13.
The solar conversion of CO to low carbon fuels has been heralded as a potential solution to combat the rise in greenhouse gas emissions. Here we report the first light-driven activation of [NiFe] CODH II from for the reduction of CO to CO. To accomplish this, a hybrid photosystem composed of CODH II and CdSe/CdS dot-in-rod nanocrystals was developed. By incorporating a low-potential redox mediator to assist electron transfer, quantum yields up to 19% and turnover frequencies of 9 s were achieved. These results represent a new standard in efficient CO reduction by an enzyme-based photocatalytic systems. Furthermore, successful photoactivation of CODH II allows for future exploration into the enzyme's not fully understood mechanism.
将 CO 转化为低碳燃料的太阳能转换被认为是解决温室气体排放上升的一种潜在方法。在这里，我们报告了首例光驱动的[NiFe] CODH II 的激活，用于将 CO 还原为 CO。为了实现这一目标，开发了一种由 CODH II 和 CdSe/CdS 点-线纳米晶体组成的混合光系统。通过引入一种低电位氧化还原介体来辅助电子转移，实现了高达 19%的量子产率和 9 s 的周转率。这些结果代表了基于酶的光催化系统高效 CO 还原的新标准。此外，CODH II 的成功光激活允许对酶的不完全理解的机制进行进一步探索。
