EAGER: A Hybrid Photosynthetic Electron Transport Chain Based on Graphene Oxide

EAGER：基于氧化石墨烯的混合光合电子传输链

• 批准号: 1260073
• 负责人: Michele Vittadello
• 金额: $ 9.43万
• 依托单位: CUNY Medgar Evers College
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-15 至 2013-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1260073&HistoricalAwards=false
• 关键词: EAGER; Hybrid; Photosynthetic; Electron; Transport

1260073VittadelloSeveral approaches for biological and biomimetic energy conversion systems have been proposed. In particular, the possibility of using photosynthesis to produce hydrogen from biological resources is attractive, and both natural microorganisms and semi-artificial devices are being investigated within various national and international programs. The approaches of semi-artificial device research being followed are aimed at a photoelectrochemical system based on PSII and PSI, which are natural photosystems, and hydrogenase. The original model, proposed in 1979, entailed the use of particles floating in solution in the presence of redox mediators. New strategies proposed by the research team of Professor Michele Vittadello of CUNY Medgar Evers College and Professor Paul Falkowski of Rutgers University involve the immobilization of PSII and PSI CCs (core complexes) and hydrogenases onto electrodic surfaces. So far, no one has published a full working device using isolated core complexes.Vittadello and Falkowski propose to demonstrate the possibility by assembling a viable photosynthetic hybrid system for water splitting based on graphene oxide (GO), core complexes of natural photosystems PSII and PSI, and Pt as a catalyst. Single-layered GO provides an ideal chemical ?canvas? for the self-assembly of photosynthetic proteins. The residual oxygen-containing chemical species include hydroxyl, carboxyl, epoxy, and ketonic functional groups concentrated at the edges of graphene quantum islands. The degree of oxidation can be used to control electron/hole transport properties. Although preliminary results for the PSI-GO and PSII-GO have been attained, the basis for this EAGER proposal is the attempt to demonstrate that photoinduced vectorial electron transfer is possible in triads comprised of PSII CCs, GO, and PSI CCs in a direct or facilitated fashion, giving rise to a supramolecular hybrid electron-transport chain with minimized overpotentials, on the model of the natural photosynthetic Z-scheme. The investigators are well qualified for conducting this project given their background knowledge in photosynthesis, electrochemistry, biophysics, biochemistry, materials science and engineering. The research team includes Senior Research Associate Kamil Woronowicz and is in an excellent position to expand the collaborative effort in semi-artificial photosynthesis for hydrogen generation. The investigation of GO-protein interactions is highly transformational for bionanotechnologies with potential applications in multi-enzyme catalysis for fuel production and chemical synthesis, and protein purification for drug development. The successful proof-of-concept will lay the foundation for further studies. The vibrancy of the topic will help leverage the ongoing effort of the investigators in the STEM educational area, through the unique institutional expertise available at Medgar Evers College and at the Rutgers Energy Institute.

已经提出了用于生物和仿生能量转换系统的几种方法。 特别是，利用光合作用从生物资源中产生氢的可能性是有吸引力的，并且在各种国家和国际计划中正在研究天然微生物和半人工装置。半人工器件研究的方向是基于天然光系统PSII和PSI以及氢化酶的光电化学系统。1979年提出的原始模型需要使用在氧化还原介质存在下漂浮在溶液中的颗粒。纽约市立大学Medgar Evers学院的Michele Vittadello教授和罗格斯大学的Paul Falkowski教授的研究小组提出的新策略涉及将PSII和PSI CC（核心复合物）和氢化酶固定在电极表面上。到目前为止，还没有人发表一个完整的工作装置使用孤立的核心复合物。Vittadello和Falkowski建议通过组装一个可行的光合混合系统来证明这种可能性，该系统基于氧化石墨烯（GO），天然光系统PSII和PSI的核心复合物，以及Pt作为催化剂。单层GO提供了一种理想的化学品？帆布？进行光合作用蛋白的自我组装。残留的含氧化学物质包括集中在石墨烯量子岛边缘的羟基、羧基、环氧基和酮基官能团。氧化程度可用于控制电子/空穴传输特性。尽管已经获得了PSI-GO和PSII-GO的初步结果，但EAGER提案的基础是试图证明光诱导矢量电子转移在由PSII CC、GO和PSII CC组成的三元组中以直接或促进的方式是可能的，从而产生超分子混合电子传递链，具有最小化的过电位，基于自然光合Z-方案的模型。 研究人员在光合作用、电化学、生物物理学、生物化学、材料科学和工程方面的背景知识使他们完全有资格进行这个项目。该研究团队包括高级研究助理Kamil Woronowicz，在扩大半人工光合作用制氢的合作方面处于有利地位。GO-蛋白质相互作用的研究对于生物纳米技术具有高度的变革性，在燃料生产和化学合成的多酶催化以及药物开发的蛋白质纯化中具有潜在的应用。成功的概念验证将为进一步的研究奠定基础。该主题的活力将有助于利用研究人员在STEM教育领域的持续努力，通过Medgar Evers College和Rutgers Energy Institute提供的独特机构专业知识。