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

在过去的七十年里，世界上可用的磷供应的消耗以惊人的速度增长。 磷供应的减少对作物生长和农业可持续性产生了负面影响。 全世界的化学家都在致力于设计新的分子策略，以满足不断增长的人口的食物需求。 鲍曼-詹姆斯教授和她在堪萨斯大学的学生们正专注于深入了解磷化学，同时解决与植酸盐相关的不良化学问题，植酸盐是土壤中发现的关键含磷分子之一。 该项目的更广泛影响包括在堪萨斯大学培训本科生和研究生，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卡洛斯克雷默教授和意大利佛罗伦萨大学的安东尼奥比安奇教授。 植酸盐（肌醇-1，2，3，4，5，6-六磷酸）是一种相对较小但化学结构复杂的有机分子，含有六种磷酸盐。 它是金属营养素的主要清除剂。 不幸的是，它的许多盐与金属离子营养素，如铁，锌和钙，是不溶性的，导致其分类为抗营养素。 植酸盐在其分子结构中还含有大量急需的磷。 在NSF化学部的大分子，超分子和纳米化学计划的支持下，Bowman-James教授和同事正在设计分子，以帮助释放捕获的金属离子营养素和探测植酸盐。磷酸盐化学。 本研究将超分子主客体化学和金属离子化学策略相结合，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提供植酸盐及其不同构象形式的深入结构概况。 营养素不溶性和交付问题正在解决使用非环状和环状螯合物复杂植酸盐通过超分子氢键和静电相互作用，除了克服植酸盐？的不利性质。 目标3通过探索含多胺的大环化合物作为磷酸盐水解和其他磷酸酶活性的催化剂来探索植酸盐的磷酰基转移化学。 X射线晶体学和多核，多维核磁共振光谱的固态和溶液化学，分别发挥着重要作用，在阐明的物理和化学性质的植酸盐在所有三个目标。

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.