Dissertations and Theses

Date of Award

2024

Document Type

Dissertation

Department

Chemical Engineering

First Advisor

Xi Chen

Second Advisor

Raymond S. Tu

Keywords

Water-responsive materials, Actuators, Actuation energy, Biomaterials, Bombyx mori silk fibroin

Abstract

Water-responsive (WR) materials mechanically swell and shrink in response to changes in relative humidity, and they have demonstrated the capability to exert higher actuation energy than conventional actuators and artificial muscles. As a result, WR materials have recently gained attention as potential high-energy actuating components for engineering applications. Despite the growing interest in this emerging category of WR materials, the fundamental WR mechanism of their significant performance is still not fully understood, limiting the ability to rationally design engineered systems. This dissertation presents three approaches for understanding the water-responsiveness of materials by engineering Bombyx (B.) mori silkworm silk protein. First, by increasing the silk’s mechanical stiffness as a result of increased silk II structures (β-sheet rich domains) or adding stiff silica nanoparticles, B. mori silk’s WR actuation energy density was dramatically increased from 0.2 to 1.6 MJ m-3, surpassing the energy densities of all known natural muscles. Second, we achieved a remarkable enhancement in the WR energy density of B. mori silk, reaching 3.1 MJ m-3, by adjusting silk’s nano-porosity. Throughout these studies, silk’s programmable secondary structures, mechanical properties, as well as pore structure-dependent water properties were found to play a crucial role in silk's WR behaviors. Third, to further explore the potential for scaling up silk-based WR materials, WR silk composite fibers were developed by coupling nanoscale Bacillus Subtilis peptidoglycan (PG) with silk using a wet-spinning technique. This work provides proof-of-concept demonstrations that use high-energy, muscle-like WR actuators for real-world applications.

Available for download on Friday, December 12, 2025

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