Extrapolating the Concept of Protein Corona for Understanding Nanoparticles at Large

[摘要]柯普春科学界最近已经确定，纳米粒子（NPs）的物理和物理化学性质在应用方面被认为是如此理想，往往是它们在环境中复杂行为的直接原因。NPs通过空气、水和土壤进入环境，在制造、运输、使用和处置的整个生命周期中，“总体上”的NPs在与光、天然有机物（NOM）、微生物和植物的相互作用中不断发生变化。因此，本提案的目标是通过将既定的蛋白质“冠状”概念（即血液中血浆蛋白对NPs的表面修饰）外推到环境中的“生物冠状”来阐明排放的NPs的可变行为和命运。生物冕的概念包括NOM、蛋白质和碳水化合物，它们是自然界无处不在的组成部分。这种建议的处理方法是有效的，因为a)生物系统是生态系统的重要和不可分割的一部分，b)必须评估转化而不是原始材料的潜在环境影响。智力优势：从技术上讲，生物冕的引入利用了为蛋白质吸附和折叠研究领域开发的实验、理论和计算方法，同时整合了与纳米技术和环境系统有关的元素。本文的三个具体目标是阐明a)天然水环境中的np -生物冠状菌，b)植物中的np -生物冠状菌，以及c)水生生物对np -生物冠状菌的生物转化和降解。待绘制的参数空间包括溶剂硬度和pH值、NP大小和溶解度、蛋白质构象和结合热力学、植物细胞易位、运输和植物毒性、ROS产生和光合作用。这些研究结果将为自然水环境中NPs的稳定性和转化提供重要信息，有助于我们了解NPs在植物物种中的吸收、生物分布和毒性，并为评价水生生物对NP暴露的反应提供关键指标。更广泛的影响：最近关于纳米技术（NanoEHS）的环境健康和安全的文献呈指数级增长。目前，许多NanoEHS研究正从现象学观察和大规模测试转向积累提高效率和预测能力的知识库。为了跟上纳米材料的广泛多样性和日益增长的应用，并适应环境的巨大复杂性，系统的方法，如外推生物日冕概念，是纳米技术环境风险评估的合乎逻辑和成本效益的解决方案。除了促进克莱姆森和维克森林大学的跨学科研究和教育外，该提案的资金将催化蛋白质折叠社区与NanoEHS社区的融合，以实现具有潜在经济收益的尖端创新。此外，这项拟议的前沿研究必然会促进pi实验室与他们在特拉华州立大学、丹尼森大学、杜克大学和莱斯大学的合作者以及爱沙尼亚国家化学物理和生物物理研究所之间的交流。

Abstract#1232724 Ke, Pu-ChunThe scientific community has recently determined that the physical and physicochemical properties of nanoparticles (NPs) deemed so desirable in terms of application are often the direct causes for their complex behavior in the environment. Upon entering the environment through air, water and soil, and during the lifecycle of manufacturing, transport, use and disposal, NPs "at large" undergo constant transformations from their interactions with light, natural organic matter (NOM), microorganisms, and plants. The goal of this proposal is therefore to elucidate the mutable behavior and fate of discharged NPs by extrapolating the established concept of protein "corona", i.e., surface modification of NPs by plasma proteins in the bloodstream, to "biocorona" in the environment. The notion of biocorona encompasses NOM, proteins and carbohydrates that are ubiquitous building blocks of nature. This proposed treatment is validated in that a) biological systems are an essential and integral part of ecosystems, and b) it is the transformed rather than the pristine material, that must be evaluated for potential environmental impact. Intellectual Merit: Technically, the introduction of biocorona exploits the established experimental, theoretical and computational approaches developed for the research areas of protein adsorption and folding while integrating the elements pertaining to nanotechnology and environmental systems. The three specific aims of this proposal are to elucidate a) NP-biocoronas in the natural aqueous environment, b) NP-biocoronas in plants, and c) biotransformation and degradation of NP-biocoronas by aquatic organisms. The parameter space to be mapped includes solvent hardness and pH, NP size and solubility, protein conformation and binding thermodynamics, plant cell translocation, transport and phytotoxicity, ROS production, and photosynthesis. Results from these studies will offer essential information on the stability and transformation of NPs in the natural aqueous environment, facilitate our understanding of the uptake, biodistribution and toxicity of NPs in plant species, and provide key indicators for evaluating aquatic response to NP exposure. Broader Impacts: Recent literature on the environmental health and safety of nanotechnology (NanoEHS) has expanded exponentially. Much NanoEHS study is now converging from phenomenological observation and mass testing toward amassing a knowledge base of increasing efficiency and prediction power. To keep pace with the vast variety and growing application of nanomaterials and to accommodate the vast complexity of the environment, methodical approaches such as extrapolated concept of biocorona are logical and cost-effective solutions to environmental risk assessment of nanotechnology. In addition to promoting interdisciplinary research and education at Clemson and Wake Forest University in the Carolinas, funding of this proposal will catalyze fusion of the protein folding community with the community of NanoEHS for cutting-edge innovation with potential economical gains. Furthermore, this proposed frontier research will necessarily foster exchanges between the PIs' labs and their collaborators at Delaware State, Denison, Duke, and Rice Universities, and the National Institute of Chemical Physics and Biophysics in Estonia.