Collaborative Research: High-Performance Biocatalytic Membranes with Self-Contained Radical Polymer Mediators for Water Reclamation and Reuse

获得清洁水是21世纪最大的工程挑战之一。有效利用现有淡水资源是应对这一挑战的主要战略。然而，如果没有来自咸淡水和废水等来源的额外水，就无法满足当前的社会需求。这些水源的成功回收和再利用取决于技术的发展，以确保这些水适合使用。该项目解决了这一需求，使用天然酶来降解水中的有毒污染物。利用聚合物化学和增材制造领域的最新进展，这些高效的生物催化剂将被配制成生物催化膜。含有酶和其他定制功能成分的生物催化墨水将以模块化的方式沉积在纳米孔膜支撑上。模块化设计可以通过改变目标酶和/或聚合物介质来定制特定需求。这项技术的成功开发将有助于解决国家面临的关键挑战，以确保安全、清洁和可持续的水资源供应。通过培养下一代跨学科科学家和工程师来解决向国家供水的挑战，该项目将对社会产生更广泛的影响。尽管面对日益增长的需求，有效利用现有淡水资源是供应国家用水的主要策略，但如果没有来自咸淡水和废水等来源的额外水，目前的社会需求就无法满足。这些水源的成功回收和再利用取决于技术的发展，以确保这些水适合使用。酶生物催化是解决这一需求的一个有前途的平台。这样的平台需要小分子量的氧化还原活性介质，以促进酶降解难降解的微污染物。虽然这些小分子提供了明显的好处，但它们很昂贵，并且可能从需要经常补充的过程中浸出。因此，消除介质冲刷是使该水处理技术可行的关键。该项目的总体目标是产生能够设计和制造高性能生物催化膜的科学知识。这将通过确定自由基聚合物基大分子介质设计中的控制因素，并阐明控制它们与酶在纳米孔载体上共沉积的加工-结构-性能关系来完成。实现这一目标的具体研究任务是：1)确定大分子介质设计，促进微污染物的有效降解，同时防止介质冲刷；2)阐明生物催化膜的加工-结构-性能关系，将膜支撑结构与生物催化和运输性能联系起来；3)在多个回收和再利用循环过程中评估生物催化膜的性能，为现场相关应用的膜设计提供信息。这项研究的成功完成将解决我们在生物催化膜设计和制造方面的知识差距。这些知识将在增材制造和水处理领域产生广泛的影响。国家将进一步受益于培训跨学科的科学家和工程师，他们具有推进美国水技术前景所必需的专业知识。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Access to clean water is among the greatest engineering challenges of the 21st century. Efficient use of existing freshwater resources is a primary strategy to address this challenge. However, current societal needs cannot be met without additional water from sources like brackish water and wastewater. Successful reclamation and reuse of these water sources depends on the development of technologies to ensure these waters are fit for use. This project addresses this need using natural enzymes to degrade toxic contaminants present in water. These highly-efficient biological catalysts will be formulated into biocatalytic membranes using recent advances in the fields of polymer chemistry and additive manufacturing. Biocatalytic inks that contain enzymes and other tailor-made functional components will be deposited onto nanoporous membrane supports in a modular fashion. The modular design can be customized for specific needs by changing the target enzymes and/or polymer mediators. Successful development of this technology will help address the critical challenges of the Nation to ensure the supply of safe, clean, and sustainable water resources. Broader impacts for society will result from this project by training the next generation of interdisciplinary scientists and engineers to address the challenge of supplying water to the Nation.Although efficient use of existing freshwater resources is a primary strategy to supply the Nation's water in the face of increasing demand, current societal needs cannot be met without additional water from sources like brackish water and wastewater. Successful reclamation and reuse of these water sources depends on the development of technologies to ensure these waters are fit for use. Enzyme biocatalysis is a promising platform to address this need. Such platforms require small molecular weight redox-active mediators to facilitate the enzymatic degradation of recalcitrant micropollutants. Although these small molecules provide clear benefits, they are costly and can leach from processes necessitating frequent replenishment. Therefore, it is critical to eliminate mediator washout to make this water treatment technology feasible. The overall goal of this project is to generate the scientific knowledge that enables the design and fabrication of high-performance biocatalytic membranes. This will be done by identifying control factors in the design of radical polymer-based macromolecular mediators and elucidating the processing-structure-property relationships that govern their co-deposition with enzymes on nanoporous supports. The specific research tasks to achieve this goal are to: 1) identify macromolecular mediator designs that promote the efficient degradation of micropollutants while preventing mediator washout; 2) elucidate the processing-structure-property relationships for biocatalytic membranes to correlate membrane support architecture with the biocatalytic and transport properties; and 3) evaluate biocatalytic membrane performance over the course of multiple recover and reuse cycles to inform membrane design for field-relevant applications. Successful completion of this research will address gaps in our knowledge on biocatalytic membrane design and manufacture. This knowledge will have broad impact in the fields of additive manufacturing as well as water treatment. The Nation will further benefit by the training of interdisciplinary scientists and engineers with the expertise necessary to advance the water technology landscape of the United States.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.