RII Track-4: Molecular understanding of salt-induced selective aggregation and selective sorption of dissolved organic matter to natural particles

RII Track-4：盐诱导选择性聚集和溶解有机物选择性吸附到天然颗粒的分子理解

• 批准号: 1738340
• 负责人: Mohammed Baalousha
• 金额: $ 28.64万
• 依托单位: University of South Carolina at Columbia
• 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: 2017-09-15 至 2021-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1738340&HistoricalAwards=false
• 关键词: RII; Track; Molecular; understanding; salt

Non-technical DescriptionDissolved organic matter (DOM) is ubiquitous in natural soils, sediments, and waters, and is a complex mixture of several thousands of organic compounds that were produced primarily from the decay of plant matter. The amount and composition of DOM affects a range of critical ecosystem functions, and plays important roles in regulating the chemistry of environments as diverse as soils, surface waters, and marine systems. DOM can selectively combine with salts and attach to natural particles, which would change their chemical properties in complex ways. This project aims to determine the molecular-level composition and properties of DOM compounds using advanced analytical techniques available at the Environmental Molecular Sciences Laboratory (EMSL) of the Pacific Northwest National Laboratory. Obtaining molecular-level properties for individual molecules will enable more specific identification of the DOM molecules and improve our understanding of their behaviors, fate, and transport in the environment. The outcome of the proposed research has direct implications for environmental and human health as it may be used by water and wastewater treatment facilities to develop novel approaches to achieve more effective approaches for DOM removal. In addition to providing access to the facilities at EMSL and expanding the PI's research capacity, this project will provide training, mentorship, and continued collaborations for the PI and a post-doctoral fellow at the University of South Carolina at Columbia.Technical DescriptionSelective aggregation and sorption of DOM to natural particles is highly relevant to a wide variety of environmental processes, yet they are poorly understood. Such understanding is currently hampered by the high diversity and complexity of DOM and the limited resolution of available mass spectrometers. The intellectual merit of this proposal lies in the application of ultrahigh resolution mass spectroscopy techniques to identify DOM molecules that selectively aggregate or selectively sorb to natural particles and the characterization of their structural properties at the individual molecular level. The overall aim of this proposed research is to characterize the molecular composition and properties of DOM compounds susceptible to aggregation or sorption to natural particles as a function of DOM composition, salt type and natural particle properties. This aim will be achieved by characterizing the molecular composition and properties of DOM molecules in solution (that is 10 kDa) before and after mixing with salts of Ca2+, Mg2+, Al3+, and Fe3+, and natural clay and metal (Fe, Mn, Al, and Si) oxide particles using 21 T Electrospray ionization ultrahigh resolution-Fourier transform-ion cyclotron resonance-mass spectrometry (ESI-FT-ICR-MS). Molecular-level characterization of DOM will be performed at the Environmental Molecular Sciences Laboratory (EMSL). The EMSL personnel will: facilitate the EPSCoR-NSF fellow access to the molecular analysis facilities; provide hands-on training for sample analysis, data collection, analysis, and interpretation; and provide overall mentorship. This EPSCoR-NSF fellowship will provide a unique training opportunity for the PI and a postdoctoral fellow by spending time at the EMSL.

非技术性描述溶解有机物（DOM）普遍存在于自然土壤、沉积物和沃茨中，是主要由植物物质腐烂产生的数千种有机化合物的复杂混合物。DOM的数量和组成影响着一系列关键的生态系统功能，并在调节土壤、地表沃茨和海洋系统等不同环境的化学方面发挥着重要作用。DOM可以选择性地与盐联合收割机结合并附着在天然颗粒物上，从而以复杂的方式改变其化学性质。该项目旨在利用太平洋西北国家实验室环境分子科学实验室（EMSL）现有的先进分析技术，确定DOM化合物的分子水平组成和性质。获得单个分子的分子水平特性将使DOM分子的识别更加具体，并提高我们对它们在环境中的行为，命运和运输的理解。拟议研究的结果对环境和人类健康有直接影响，因为它可能被水和废水处理设施用来开发新的方法，以实现更有效的DOM去除方法。除了提供在EMSL的设施和扩大PI的研究能力，该项目将提供培训，指导，并继续合作的PI和博士后研究员在南卡罗来纳州大学在哥伦比亚。Technical DescriptionSelective聚集和吸附DOM的天然颗粒是高度相关的各种各样的环境过程，但他们知之甚少。目前，由于DOM的高度多样性和复杂性以及现有质谱仪的分辨率有限，这种理解受到阻碍。这一建议的智力价值在于应用高分辨质谱技术来识别DOM分子，选择性地聚集或选择性地吸附到天然颗粒和表征其结构特性在单个分子水平。这项拟议研究的总体目标是表征DOM化合物的分子组成和性质，容易聚集或吸附到天然颗粒作为DOM组合物，盐的类型和天然颗粒的性能的函数。这一目标将通过使用21 T电喷雾电离质谱解析-傅立叶变换-离子回旋共振-质谱（ESI-FT-ICR-MS）表征溶液（即10 kDa）中DOM分子在与Ca 2+、Mg 2+、Al 3+和Fe 3+的盐以及天然粘土和金属（Fe、Mn、Al和Si）氧化物颗粒混合之前和之后的分子组成和性质来实现。DOM的分子水平表征将在环境分子科学实验室（EMSL）进行。EMSL人员将：促进EPSCoR-NSF研究员访问分子分析设施;提供样品分析，数据收集，分析和解释的实践培训;并提供全面的指导。这个EPSCoR-NSF奖学金将通过在EMSL花费时间为PI和博士后研究员提供独特的培训机会。

项目成果

Natural organic matter composition and nanomaterial surface coating determine the nature of platinum nanomaterial-natural organic matter corona

• DOI: 10.1016/j.scitotenv.2021.150477
• 发表时间: 2021-09-23
• 期刊: SCIENCE OF THE TOTAL ENVIRONMENT
• 影响因子: 9.8
• 作者: Baalousha, Mohammed;Sikder, Mithun;Hess, Nancy J.
• 通讯作者: Hess, Nancy J.

Nanoparticle size and natural organic matter composition determine aggregation behavior of polyvinylpyrrolidone coated platinum nanoparticles

• DOI: 10.1039/d0en00659a
• 发表时间: 2020-11
• 期刊: Environmental science. Nano
• 作者: M. Sikder;Jingjing Wang;Brett A. Poulin;M. Tfaily;Mohammed Baalousha

Natural organic matter composition determines the molecular nature of silver nanomaterial-NOM corona

• DOI: 10.1039/c8en00018b
• 发表时间: 2018-04-01
• 期刊: ENVIRONMENTAL SCIENCE-NANO
• 影响因子: 7.3
• 作者: Baalousha, Mohammed;Afshinnia, Kamelia;Guo, Laodong
• 通讯作者: Guo, Laodong