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

合作提案：INFEWS N/P/H2O：含有机磷环境基质生物催化转化中的超分子识别

• 批准号: 1709626
• 负责人: Ludmilla Aristilde
• 金额: $ 30.48万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-08-01 至 2022-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1709626&HistoricalAwards=false
• 关键词: Collaborative; Proposal; INFEWS; H2O; Supramolecular

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.

该项目由化学系环境化学科学项目资助。它支持康奈尔大学的Ludmilla Aristilde博士和特拉华州大学的Deb Jaisi博士研究环境中磷的循环。磷（P）是肥料的重要成分，但过量则是一种污染物。无机磷是植物所需的形式。动物可以使用有机磷或无机磷。有机磷和无机磷都可以溶解或悬浮在水中。 有机磷向无机磷转化的研究还很少。主要研究目标是更好地了解这种转变的化学控制。开展了关于有机磷（包括肥料、有机废物和土壤中的有机物质）的命运的外联活动。这项推广活动旨在提高从市中心中学生到农民的公众识字率。两位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有关农业土地养分和肥料管理的宝贵知识。研究活动结合了来自分子生物学、分析化学和计算建模的联合收割机工具。分子水平的见解获得控制酶释放无机磷从复杂的有机组合的化学因素。该项目有三个主要目标。首先，研究了有机组合中磷酸酶的活性。其次，它解决了矿物表面对酶-底物识别的影响。第三，催化动力学响应于外部化学刺激建模。代谢组学分析使不同的有机磷组合物的催化水解的监测。同位素被用来追踪酶的催化作用。这提供了不同的酶在回收有机磷在响应于环境基质的化学作用的信息。分子动力学模拟与实验研究相结合，说明了负责有机磷的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的无机磷生成。这解决了长期存在的知识差距，在环境测绘磷物种及其在土壤和沃茨的命运。

项目成果

Hierarchical Reactivity of Enzyme-Mediated Phosphorus Recycling from Organic Mixtures by Aspergillus niger Phytase

• DOI: 10.1021/acs.jafc.0c05924
• 发表时间: 2021-02-24
• 期刊: JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
• 影响因子: 6.1
• 作者: Solhtalab，Mina;Klein，Annaleise R.;Aristilde，Ludmilla
• 通讯作者: Aristilde，Ludmilla

Molecular Coordination, Structure, and Stability of Metal-Polyphosphate Complexes Resolved by Molecular Modeling and X-ray Scattering: Structural Insights on the Biological Fate of Polyphosphate

通过分子建模和 X 射线散射解析金属-聚磷酸盐配合物的分子配位、结构和稳定性：对聚磷酸盐生物命运的结构见解

• DOI: 10.1021/acs.est.1c04782
• 发表时间: 2021
• 期刊: Environmental Science & Technology
• 影响因子: 11.4
• 作者: Park, Yeonsoo;Malliakas, Christos D.;Zhou, Qing;Gu, April Z.;Aristilde, Ludmilla
• 通讯作者: Aristilde, Ludmilla