Collaborative Proposal: INFEWS N/P/H2O: Supramolecular Recognition in the Biocatalytic Transformation of Organic Phosphorus-Containing Environmental Matrices

本项目由化学学部环境化学科学项目资助。它支持康奈尔大学的Ludmilla Aristilde博士和特拉华大学的Deb Jaisi博士研究环境中磷的循环。磷(P)是肥料的基本成分，但过量则是一种污染物。无机磷是植物所需要的形式。动物既可以使用有机磷，也可以使用无机磷。有机磷和无机磷都能溶解或悬浮在水中。有机磷向无机磷的转化尚不清楚。关键的研究目标是更好地了解这种转化的化学控制。推广活动的主题是有机磷的命运，包括肥料、有机废物和土壤中的有机质。推广活动的目的是提高公众的识字率，从市中心的中学生到农民。两位调查人员分别参与了纽约州和特拉华州农民的教育活动。不同的利益相关者获得了有关农业用地养分和肥料管理的宝贵知识。这个项目采用多学科方法。研究活动结合了分子生物学、分析化学和计算建模的工具。分子水平的见解是获得的化学因素，控制无机磷的酶释放从复杂的有机组合。该项目有三个主要目标。首先，研究了有机组合的磷酸酶活性。其次，它解决了矿物表面对酶-底物识别的影响。第三，对外部化学刺激的催化动力学进行了建模。代谢组学分析能够监测不同有机P组合的催化水解。同位素被用来跟踪酶的催化作用。这提供了不同酶在响应环境基质的化学反应中回收有机磷的作用的信息。与实验研究相结合的分子动力学模拟揭示了有机磷环境生物转化的超分子框架，揭示了生物地球化学因子如何控制磷酸酶介导的有机磷组合产生无机磷。这解决了一个长期存在的知识差距，在P物种的环境制图及其命运在土壤和水域。

This project is funded by the Environmental Chemical Sciences program in the Division of Chemistry. It supports Dr. Ludmilla Aristilde of Cornell University and Dr. Deb Jaisi of the University of Delaware to investigate the cycling of phosphorus in the environment. Phosphorus (P) is an essential component of fertilizers, but in excess, a pollutant. Inorganic phosphorus is the form required by plants. Animals can use either organic or inorganic phosphorus. Both organic and inorganic phosphorus can be dissolved or suspended in water. The transformation of organic P to inorganic P is poorly understood. The key research objective is to better understand the chemical controls of this transformation. Outreach activities are carried out on the topic of the fate of organic P including fertilizers, organic wastes, and organic matter in soils. The outreach is aimed at increasing public literacy, from inner-city middle school students to farmers. Both investigators are involved in educational activities for farmers in New York and Delaware, respectively. Different stakeholders gain valuable knowledge regarding nutrient and fertilizer management on agricultural lands.This project applies a multidisciplinary approach. The research activities combine tools from molecular biology, analytical chemistry, and computational modeling. Molecular-level insights are obtained on the chemical factors that control the enzymatic release of inorganic P from complex organic assemblages. The project has three main objectives. First, it studies the activities of phosphatase enzymes with organic assemblages. Second, it addresses the effects of mineral surfaces on enzyme-substrate recognition. Third, the catalytic dynamics in response to external chemical stimuli is modeled. Metabolomics profiling enables the monitoring of catalytic hydrolysis of different organic P assemblages. Isotopes are used to track enzyme catalysis. This provides information on the role of different enzymes in recycling organic P in response to the chemistry of the environmental matrix. Molecular dynamics simulations in concert with the experimental studies illustrate the supramolecular framework responsible for the environmental biotransformation of organic P. The research findings shed light on how biogeochemical factors control phosphatase-mediated inorganic P generation from organic P assemblages. This addresses a long-standing knowledge gap in the environmental mapping of P species and their fate in soils and waters.