INFEWS N/P/H20: Supramolecular Recognition and Catalysis Targeting Phytate, an Organic Sink for Phosphate in the Human Phosphorus Cycle

在过去的70年里，世界上可获得的磷的消耗以惊人的速度增长。不断减少的磷供应对作物生长和农业可持续性产生负面影响。世界各地的化学家都致力于设计新的分子策略来满足不断增长的人口对食物的需求。鲍曼-詹姆斯教授和她在堪萨斯大学的学生们专注于深入了解磷的化学性质，同时解决与植酸盐（土壤中发现的关键含磷分子之一）相关的不利化学问题。该项目更广泛的影响包括堪萨斯大学本科生和研究生的培训，以及国际学生交流。合作者包括堪萨斯州立大学的土壤科学家Ganga Hettiarachchi教授和两名国际研究人员，乌拉圭共和国大学的Carlos Kremer教授和意大利佛罗伦萨大学的Antonio Bianchi教授。植酸盐（肌醇-1,2,3,4,5,6-己基磷酸）是一种相对较小的，但化学上复杂的有机分子，含有六种磷酸盐。它是金属营养物的主要清道夫。不幸的是，许多含有金属离子营养素的盐，如铁、锌和钙，是不溶的，因此它被归类为抗营养素。植酸盐在其分子结构中也含有大量急需的磷。在美国国家科学基金会化学部大分子、超分子和纳米化学项目的支持下，鲍曼-詹姆斯教授和他的同事们正在设计分子来帮助释放捕获的金属离子营养物质，并探测植酸盐？磷酸化学。本研究将超分子主客体化学与金属离子化学相结合，为调控植酸盐的理化性质提供了新的途径。目标是在分子水平上更好地理解植酸盐和磷酸盐化学。目的1和2提供了深入的结构概况植酸及其不同的构象形式。除了克服植酸盐外，还通过超分子氢键和静电相互作用，利用非环和环螯合物络合植酸盐来解决营养不溶性和递送问题。S不良性质。Aim 3通过探索使用含多胺的大环作为磷酸盐水解和其他磷酸酶活性的催化剂，努力探索植酸的磷酸化转移化学。固体化学和溶液化学的x射线晶体学和多核、多维核磁共振波谱学在阐明植酸盐的物理和化学性质方面发挥着重要作用。

Depletion of the world's available supply of phosphorus has grown at alarming rates over the last seven decades. The dwindling phosphorus supplies negatively impact crop growth and agricultural sustainability. Chemists worldwide are focused on devising new molecular strategies to meet the food needs of a growing population. Professor Bowman-James and her students at the University of Kansas are focusing on gaining insight into phosphorus chemistry while addressing the adverse chemical issues associated with phytate, one of the key phosphorus-containing molecules found in soils. Broader impacts of this project include the training of undergraduate and graduate students at the University of Kansas, as well as international student exchanges. Collaborators include a soil scientist, Professor Ganga Hettiarachchi, at Kansas State University, and two international researchers, Professor Carlos Kremer at the University of the Republic in Uruguay, and Professor Antonio Bianchi at the University of Florence in Italy. Phytate (myo-inositol-1,2,3,4,5,6-hexakisphosphate) is a relatively small, but chemically complex, organic molecule loaded with six phosphates. It is a major scavenger of metal nutrients. Unfortunately, many of its salts with metal ion nutrients, such as iron, zinc, and calcium, are insoluble, resulting in its classification as an antinutrient. Phytate also holds a significant amount of much-needed phosphorus hostage within its molecular structure. With the support of the Macromolecular, Supramolecular and Nanochemistry Program of the NSF Chemistry Division, Prof. Bowman-James and coworkers are designing molecules to assist in releasing captured metal ion nutrients and to probe phytate?s phosphate chemistry. This research combines supramolecular host-guest and metal ion chemistry tactics to provide new ways to manipulate the physical and chemical properties of phytate. Goals are to gain a better understanding of phytate and phosphate chemistry at the molecular level. Aims 1 and 2 provide an in-depth structural profile of phytate and its different conformational forms. Nutrient insolubility and delivery issues are being addressed by using noncyclic and cyclic chelates to complex phytate via supramolecular hydrogen bond and electrostatic interactions, in addition to overcoming phytate?s adverse properties. Aim 3 strives to probe the phosphoryl transfer chemistry of phytate by exploring the use of polyamine-containing macrocycles as catalysts for phosphate hydrolysis and other phosphatase activity. X-ray crystallography and multi-nuclear, multi-dimensional NMR spectroscopy for both solid state and solution chemistry, respectively, are playing major roles in elucidating the physical and chemical properties of phytate in all three aims.