Engineering functional biomaterials to advance environmental and resource sustainability

Recovering resources from waste streams offers a sustainable solution to the growing scarcity of resources and the increasing environmental impact of waste. A significant challenge lies in efficiently extracting or converting valuable resources from complex waste mixtures into recoverable forms. In recent years, protein-based biosorption and biocatalysis have emerged as promising alternatives to conventional methods due to their inherent advantages, such as strong substrate affinity, selectivity, rapid adsorption kinetics, potent enzymatic activity, and minimal energy and chemical requirements. The ability to engineer and manipulate proteins opens avenues for creating innovative biomaterials with tailored functionalities, addressing critical environmental and resource sustainability challenges. This dissertation aims to develop novel protein-based biosorbents and enzyme-based biocatalysts for resource recovery, separation, and conversion applications. The research focuses on three key objectives: (1) designing a novel magnetic nanoplatform for protein immobilization; (2) evaluating this nanoplatform by fabricating protein-based biosorbents for the selective recovery and efficient separation of rare earth elements (REEs); and (3) engineering renewable enzyme biocatalysts for phosphate conversion and recovery from biorefinery waste streams. These findings contribute to advancing innovative biosorptive and biocatalytic technologies, addressing critical resource recovery challenges, and promoting sustainable management of phosphorus and rare earth elements, thus fostering a more sustainable Earth. First, we employed SpyTag-SpyCatcher chemistry to conjugate model proteins onto magnetic nanoparticles (MNPs), establishing a modular, magnetic-responsive platform for protein immobilization. This approach significantly enhanced protein stability while retaining functionality. The protein-immobilized MNPs also maintained high colloidal stability and magnetic responsiveness in solution, enabling convenient protein separation and reuse. Next, leveraging the developed nanoplatform, we created a highly specific and reusable lanmodulin-based biosorbent for efficient REE recovery from low-grade waste streams. This biosorbent demonstrated high selectivity, rapid adsorption-desorption kinetics, and stability through multiple uses. Also, the MNP-LanM selectively adsorbed and concentrated REEs from the leachate of coal fly ash and geothermal brine. Finally, we developed a renewable surface-displayed phytase biocatalyst for efficient phosphate conversion and recovery from biorefinery waste streams. This biocatalyst exhibited high activity, storage stability, easy regenerability, and reusability. We also employed a machine learning algorithm to identify phytase variants with enhanced activity and robustness against inhibitory substances in biorefinery solutions.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Environ Engr in Civil Engr

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2024

Author dc:creator

• Ye, Quanhui

Contributors dc:contributor

• Kearns, Daniel
• Lu, Yongqi
• Wei, Na
• Nguyen, Thanh Huong
• Espinosa Marzal, Rosa Maria

• Resource Recovery
• Sustainability
• Protein Engineering
• Environmental Engineering

Statement dc:rights

• Copyright 2024 Quanhui Ye

Language dc:language

eng, en

Handle dc:identifier

https://hdl.handle.net/2142/127321

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/127321