A Simple, Robust Biomimetic Charge Separation Protein Domain

智力价值这项研究涉及一种人造蛋白质的设计、合成和分析，这种蛋白质在短时间的光激发下将能够产生相对较长寿命的电荷分离状态。电荷分离过程是光合作用的第一步，也是最重要的一步，这一结构将使研究人员能够检查支持电荷分离的潜在物理过程。该项目涉及设计一个三协因子螺旋束蛋白结构域，它通过三种正交机制结合其辅助因子：主要供体分子将是锌(II)-酞菁，它特异性地结合到单组氨酸五配位位置。受体辅因子结合部位将是一个六配位的双组氨酸部位，它紧密而稳定地结合各种含铁大环。供体部位将包含使用细胞色素C生物发生系统在体内共价连接的C型血红素。这种电荷分离结构域将共价连接到邻苯二甲酸双加氧酶还原酶的黄素蛋白还原酶域上，使供体能够通过简单地添加NADH通过天然蛋白质嵌合体将电子转移到主要供体酞菁辅助因子。预期的最终产品将是一个简单、健壮的模块化蛋白质结构域，将为许多不同的科学家和工程师创造太阳能驱动的设备提供服务。广泛的影响这项工作不仅将提高对电荷分离工程的理解，还将产生一系列具有可调动力学和能量学的蛋白质结构域，可用于创建光激活纳米设备。CCNY是一所公立城市大学，拥有极其多样化的多民族学生群体。将制定一项教育计划，向本科生、研究生和纽约市公立高中教师介绍生物物理学的跨学科科学。

Intellectual MeritThis research concerns the design, synthesis and analysis of an artificial protein which will have the ability to create a relatively long-lived charge separated state when excited with short bursts of light. The process of charge separation is the first, most important step in photosynthesis, and this construction will allow researchers to examine the underlying physical processes which support charge separation. The project involves the design of a three cofactor helical bundle protein domain which binds its cofactors by three orthogonal mechanisms: the primary donor molecule will be a zinc(II)-phthalocyanine which binds specifically to mono-histidine pentacoordinate sites. The acceptor cofactor binding site will be a hexacoordinate bis-histidine site which tightly and stably binds a variety of iron-containing macrocycles. The donor site will contain a C-type heme covalently attached in vivo using the cytochrome C biogenesis system. This charge separation domain will be covalently attached to the flavoprotein reductase domain of phthalate dioxygenase reductase, enabling the donor to be poised for electron transfer to the primary donor phthalocyanine cofactor via the natural protein chimera by the simple addition of NADH. The intended final product will be a simple, robust modular protein domain which will serve many different scientists and engineers in their creation of solar energy-driven devices.Broader ImpactThis work will not only improve the understanding of the engineering of charge separation, it will result in a series of protein domains with tunable kinetics and energetics which can be used in the creation of light-activated nanodevices. CCNY, a public, city university, has an extremely diverse multi-ethnic student body. An educational plan, which introduces undergraduates, graduate students and New York City Public High School teachers to the interdisciplinary science of biophysics, will be developed.