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

1260073已经提出了几种生物和仿生能量转换系统的方法。特别是，利用光合作用从生物资源中生产氢气的可能性是有吸引力的，自然微生物和半人工设备都正在各种国内和国际项目中进行研究。目前正在进行的半人工器件研究主要针对基于PSII和PSI这两种天然光系统和氢酶的光电化学体系。最初的模型提出于1979年，需要使用在氧化还原介体存在的情况下漂浮在溶液中的颗粒。纽约州立大学梅德加·埃弗斯学院的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包括将PSII和PSI CCS(核心复合体)和氢酶固定到电极表面。到目前为止，还没有人发表使用分离的核心络合物的完整工作装置。Vittadello和Falkowski建议通过组装基于氧化石墨烯(GO)、天然光系统PSII和PSI的核心络合物以及铂作为催化剂的可行的光合作用杂化系统来展示这种可能性。单层围棋提供了理想的化学帆布？用于光合作用蛋白质的自我组装。残留的含氧化学物种包括聚集在石墨烯量子岛边缘的羟基、羧基、环氧基和酮基官能团。氧化程度可以用来控制电子/空穴输运性质。虽然PSI-GO和PSII-GO已经取得了初步的结果，但这一热切的提议的基础是试图证明在由PSII CCS、GO和PSI CCS组成的三元体系中，光诱导的电子转移是可能的，从而在自然光合作用Z-方案的模型上产生具有最小超势的超分子杂化电子传输链。鉴于他们在光合作用、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，研究人员完全有资格进行这一项目。研究团队包括高级研究员Kamil Woronowicz，他们在扩大半人工光合作用产氢方面的合作努力方面处于非常有利的地位。GO-蛋白质相互作用的研究对生物纳米技术具有很高的变革意义，在燃料生产和化学合成的多酶催化以及药物开发中的蛋白质纯化方面具有潜在的应用前景。概念验证的成功将为进一步的研究奠定基础。这一主题的活力将有助于通过梅德加·埃弗斯学院和罗格斯能源研究所提供的独特机构专业知识，利用STEM教育领域研究人员正在进行的努力。

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.