Designing the next generation of highly selective sorbent materials for remediation of target inorganic contaminants in aqueous systems

项目摘要/摘要 有效去除超级基金站点饮用水中的金属污染物是保护人类健康的关键 健康。然而，这一过程受到了自然共生的、否则有益于健康的 离子。这些离子在常见的处理过程中竞争表面吸附位置，例如吸附剂， 意在去除目标金属污染物。此外，这些竞争对手经常出现在可比或 更高的浓度，表现出相似的化学结构，并表现出类似或更好的亲和力 吸附位置。传统的吸附技术是自上而下的，其中创建表面吸附位置 使用或模仿天然材料的。然而，聚合物和纳米科学的最新进展允许 前所未有的自下而上的能力，可对热力学进行建模、表征和可控合成 吸附剂。在这里，我们将利用化学行为的差异，如极性、电荷分布、大小和 目标含氧阴离子金属污染物与天然竞争离子产生的疏水性 高度选择性和可调谐的聚合物和纳米表面。结合显影含氧阴离子质量 处理过程中的传输模型，这些新的自下而上的设计策略将被应用于开发 与目前商业自上而下设计的相比，具有更高的效率和效果的宏观吸着剂 吸着剂。我们将通过迭代合成、建模和扩展来实现创新的自下而上方法 来自两个平台的高选择性吸附剂，提供多种规模和不同饮用水下的解决方案 系统条件(例如，个人家庭水龙头的使用点(POU)与社区的入口点(PoE)- 规模应用)：1)利用具有各种过渡金属交联剂(TMC)的生物聚合物作为入口点 (POE)应用和2)控制纳米金属氧化物的尺寸、表面积、形貌和结晶度 这些聚合物被集成到多孔电纺聚合物纤维中，用于一次性POU应用。在(1)中， 生成的交联物可以静电和/或立体地排除竞争离子。在第(2)款中， 某些高能晶面的存在和末端表面团的配位形成表面 一种有利于吸附特定目标污染物的化学，使不同的混合物 纤维中的NMOS可以用来瞄准特定的金属混合物。我们的初步结果表明 这两个系统实现超级基金相关金属选择性的潜力是目前无法实现的 吸着剂。因此，我们建议彻底改变从超级基金中清除混合金属污染物的方法。 通过可同时降低运营成本和危险废物的流程提供现场饮用水 在改善公共健康保护的同时，减少发电和违反饮用水合规行为。

PROJECT SUMMARY/ ABSTRACT The effective removal of metal contaminants from drinking water at Superfund sites is critical to protect human health. However, this process is challenged by the presence of naturally co-occurring, otherwise health-benign ions. Such ions compete for surface adsorption sites in common treatment processes, such as adsorbents, intended to remove the target metal pollutants. Further, these competitors frequently occur at comparable or higher concentrations, exhibit analogous chemical structures, and demonstrate similar or superior affinities for sorption sites. Conventional adsorbent technologies are top-down, wherein surface adsorption sites are created using or mimicking natural materials. Yet, recent advances in polymer- and nano-science allow for unprecedented bottom-up capabilities to thermodynamically model, characterize, and controllably synthesize adsorbents. Here, we will exploit chemical behavioral differences such as polarity, charge distribution, size, and hydrophobicity between target oxoanion metal pollutants and naturally occurring competing ions to generate highly selective and tunable polymeric and nano-surfaces. In conjunction with developing oxoanion mass transport models within treatment processes, these new bottom-up design strategies will be applied to develop macro-scale sorbents with improved efficiency and effectiveness over current commercial top-down designed sorbents. We will realize our innovative bottom-up approach by iteratively synthesizing, modeling, and scaling highly selective sorbents from two platforms offering solutions at multiple scales and under varying drinking water system conditions (e.g., point-of-use (POU) at individuals household tap vs. point-of-entry (POE) community- scale applications): 1) utilize biopolymers with various transition metals crosslinkers (TMC) for point of entry (POE) applications and 2) controlling size, surface area, morphology, and crystallinity of nano-metal oxides (NMOs) that are integrated into porous electrospun polymer fibers for single-use POU applications. In (1), resultant crosslinking complexes can exclude competitive ions electrostatically and/or sterically. In (2), the presence of certain high-energy crystal facets and the coordination of terminal surface groups create surface chemistry that is favorable toward the sorption of specific target contaminants such that a blend of different NMOs within a fiber could be used to target specific mixtures of metals. Our preliminary results demonstrate the potential of both systems to realize selectivity of Superfund-relevant metals that cannot be achieved by current sorbents. Thus, we propose to revolutionize the approach to removing mixed metal pollutants from Superfund site drinking water through processes that can simultaneously reduce operational costs, hazardous waste generation, and drinking water compliance violations while improving the protection of public health.