Bioorganometallic Chemistry of Enzyme Active Sites with Focus on Hydrogenase

无机、生物无机和有机金属化学项目的研究奖支持德克萨斯州a&m大学Marcetta Darensbourg教授对控制自然界氢代谢的酶活性位点的小分子模型进行基础研究。在本研究中，制备了氢化酶中发现的独特金属有机片段的合成类似物，并对其模拟以微氢经济为生的生物体中发现的产氢和耗氢催化的能力进行了分析。这些天然催化剂的原子间连接、几何结构和光谱足迹在小分子中得以再现。通过将新分子嵌入聚合物微球和环糊精中，研究了周围蛋白质基质的复杂和促进作用。通过这种方法，我们了解了大自然如何将氢处理能力设计成铁和镍的基本金属结构，而商业燃料电池必须依赖于昂贵且资源有限的铂。各级学生（研究生和本科生）都对燃料电池的化学性质感到兴奋，对氢作为一种能量载体的兴趣很高。在打开年轻人对替代能源和挑战所需的研究的过程中，来自大自然的灵感引导到生物学，生物化学，生物物理学以及合成无机化学的文献中。我们的多元文化研究小组作为一个团队在项目中工作，以鼓励文法学校儿童对科学的兴趣；来自传统黑人学院和大学的本科生，以及来自以西班牙裔为主的南德克萨斯州大学的本科生，加入了这个研究小组，通过暑期研究来帮助这些项目。这项工作的成功将导致氢处理催化剂足够可行，可以作为分子燃料电池电极，取代铂作为燃料电池电极，并使节能燃料电池技术在更广泛的应用中成为可能。

The Research award in the Inorganic, Bioinorganic and Organometallic Chemisry program supports work by Professor Marcetta Darensbourg at the Texas A&M University in College Station, TX, to carry out fundamental studies on small molecule models of enzyme active sites responsible for controlling hydrogen metabolism in nature. In this research, synthetic analogues of the unique metal-organic fragments found in hydrogenase enzymes are prepared and assayed for their ability to mimic the hydrogen-producing and hydrogen-consuming catalysis found in organisms that subsist on a micro-hydrogen economy. The atom-atom connections, the geometrical structure, and spectroscopic footprints of these natural catalysts are reproduced in the small molecules. The intricate and facilitating role of the surrounding protein matrix is approached by imbedding the new molecules in polymer beads and cyclodextrins. By this approach we develop understanding of the way Nature has engineered hydrogen processing ability into base metal constructs of iron and nickel, whereas commercial fuel cells must rely on expensive and resource-limited platinum. Students at all levels (graduates and undergraduates) are excited by the chemistry of fuel cells and interest in hydrogen as an energy carrier is high. In the process of opening young minds to the needed research in alternative energy sources and challenges, inspiration from nature leads into the literature of biology, biochemistry, biophysics, as well as synthetic inorganic chemistry. Our culturally diverse research group works as a team in projects to encourage interest in science in grammar school children; undergraduates from historically black colleges and universities and from South Texas, largely Hispanic colleges, join the research group to help in the projects through summer research. A home-run from this work would result in hydrogen processing catalysts feasible enough to serve as a molecular fuel cell electrode, replacing platinum as a fuel cell electrode, and to make energy-efficient fuel cell technology feasible for a broader range of applications.