CAREER / SusChEM: Bio-inspired synthesis of conformationally flexible analogues of the biological oxygen evolving complex: A redesigned approach to manganese cluster molecules

职业 / SusChEM：生物放氧复合物构象灵活类似物的仿生合成：锰簇分子的重新设计方法

• 批准号: 1254545
• 负责人: Michael Zdilla
• 金额: $ 50万
• 依托单位: Temple University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1254545&HistoricalAwards=false
• 关键词: CAREER; SusChEM; Bio; inspired; synthesis

With this CAREER award, the Chemical Synthesis Program will support the research of Professor Michael J. Zdilla of Temple University on the oxygen evolving complex (OEC) of photosystem II that is nature's solution to the most energetically taxing component of solar water splitting. This catalyst is a manganese-calcium-oxo cluster which undergoes structural rearrangements via a 5-stage catalytic cycle whereby it oxidizes water to oxygen, pumps protons across the thylakoid membrane, and harvests reducing equivalents for energy storage in sugars. In this area there is relatively extensive model chemistry of manganese clusters but the rearrangement chemistry and cluster flexibility, key components to the action of the OEC, are not well represented in the literature. Prof Zdilla's research program has two main foci: 1) the design and preparation of manganese clusters of enhanced flexibility via the avoidance of stabilizing chelating ligands, which lock cluster cores in place, and 2) study of reaction and rearrangement chemistry of these systems, especially in comparison to the well-established, more stable chelate clusters. Global energy demand continues to grow exponentially while fossil fuel reserves continue to be depleted. To meet world energy demands, new solar energy technology must be developed. Nature's selection of a manganese cluster cofactor to achieve the difficult water oxidation reaction of photosynthesis suggests these molecules possess enormous transformative power for solar-powered water activation. The proposed work will pursue these goals in work that affords the opportunity for training of graduate and undergraduate students, and also provides minority training opportunities at Temple, one of the most ethnically and culturally diverse urban schools in the United States. The PI will continue his involvement in science outreach in the Philadelphia area through organizations like the Chemical Heritage Foundation, Nerd Nite Cafe, and the Philadelphia Science Festival. He will also pursue, along with the worldwide crystallographic community, the development of a much needed database of X-ray crystallographic educational resources, accessible to all teachers and students of crystallography, with the aim of providing extensive educational resources for this multi-field discipline.

通过此职业奖，化学综合计划将支持坦普尔大学的迈克尔·兹迪拉教授在光系统II的氧气进化综合体（OEC）的研究中，这是自然界对太阳能水分最有能力征税的组成部分的解决方案。该催化剂是一种锰-氧簇，通过5阶段的催化循环进行结构重排，从而将水氧化为氧气，将质子泵送到诸如类囊体膜上，并收获减少糖存储能量储存的等效物。在这一领域，有相对广泛的锰簇化学模型化学，但是文献中的重排化学和集群柔韧性（OEC作用的关键组成部分）在文献中并不很好。 Zdilla教授的研究计划具有两个主要焦点：1）通过避免稳定螯合配体的设计和制备，增强了灵活性的锰簇的设计和制备，这些配体锁定了核心群核心，以及2）研究这些系统的反应和重排化学，尤其是与稳定的，更稳定的，更稳定的稳定稳定稳定稳定的浮雕相比。全球能源需求继续呈指数增长，而化石燃料储量继续耗尽。为了满足世界能源需求，必须开发新的太阳能技术。大自然对锰簇辅因子的选择来达到光合作用的困难水氧化反应表明，这些分子具有巨大的变化能力，用于太阳能供电的水活化。拟议中的工作将追求这些目标，为研究生和本科生培训提供了机会，并在坦普（Temple）提供少数群体培训机会，Temple是美国最多样化的城市学校之一。 PI将通过化学遗产基金会，Nerd Nite Cafe和费城科学节等组织继续参与费城地区的科学宣传。他还将与全球晶体学界一起追求X射线晶体学教育资源的急需数据库，并为所有晶体学的老师和学生提供访问，目的是为这个多场学科提供广泛的教育资源。