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

这个项目是由化学系环境化学科学项目资助的。它支持康奈尔大学的Ludmila 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，但过量时又是一种污染物。无机磷是植物必需的形态。动物既可以使用有机磷，也可以使用无机磷。有机磷和无机磷都可以溶解或悬浮在水中。对于有机磷向无机磷的转化，人们知之甚少。关键的研究目标是更好地了解这种转变的化学控制。开展了关于包括化肥、有机废物和土壤中有机物质在内的有机磷的去向的外联活动。这项活动旨在提高从市中心的中学生到农民的公众识字率。这两名调查人员分别参与了纽约和特拉华州农民的教育活动。不同的利益相关者获得了关于农田养分和肥料管理的宝贵知识。该项目采用了多学科方法。研究活动结合了分子生物学、分析化学和计算建模的工具。从分子水平上深入了解了控制复杂有机组合中无机磷的酶促释放的化学因素。该项目有三个主要目标。首先，研究了具有有机组合的磷酸酶的活性。其次，它解决了矿物表面对酶-底物识别的影响。第三，模拟了催化剂对外界化学刺激的响应动力学。代谢组学图谱使监测不同有机磷组合的催化水解成为可能。同位素被用来跟踪酶的催化作用。这提供了关于不同的酶在循环有机磷中的作用的信息，以响应环境基质的化学。分子动力学模拟与实验研究相结合，阐明了有机磷环境生物转化的超分子框架。研究结果揭示了生物地球化学因素如何控制磷酸酶介导的有机磷组合生成无机磷。这解决了在土壤和水中磷物种及其去向的环境地图绘制方面长期存在的知识差距。

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.