Air conditioning is a significant energy consumer in buildings, especially in humid regions where a substantial portion of energy is used to remove moisture rather than cool the air. Traditional dehumidification methods, which cool air to its dew point to condense water vapor, are energy intensive. This process unnecessarily overcools the air, only to reheat it to the desired temperature.This research introduces thermoresponsive materials as efficient desiccants to reduce energy demand for dehumidification. A system using lower critical solution temperature (LCST) type ionic liquids (ILs) as dehumidifiers is presented. Through the Flory-Huggins theory of mixtures, interactions between ionic liquids and water are analyzed. LCST ionic liquids demonstrate superior performance, with a coefficient of performance (COP) four times higher than non-thermoresponsive desiccants under similar conditions. The efficacy of ionic liquids as dehumidifiers is assessed based on properties like LCST temperature and enthalpic interaction parameter. The research also delves into thermoresponsive solid desiccants, particularly polymers, using the Vrentas-Vrentas model. This model offers a more accurate depiction of their behaviors compared to the Flory-Huggins theory by considering elastic energy stored in the polymers. Moisture absorption in thin film polymers is studied under diverse conditions, producing absorption isotherms for various temperatures and humidities. Using temperature-dependent interaction parameters, the behavior of the widely-used thermoresponsive polymer (TRP) PNIPAAm and hypothetical TRPs is investigated. The parameters from the model are used as input to do a finite element analysis of a thermoresponsive dehumidifier. This model demonstrates the complete absorption-desorption cycle under varied conditions such as polymer absorption temperature, relative humidity, and air speed. Results indicate that a TRP with enhanced absorption capacity and an LCST of 50℃ achieves a peak moisture removal efficiency (MRE) of 0.9 at 75% relative humidity which is comparable to other existing thermoresponsive dehumidification systems. But other TRPs with even greater absorption capacity can produce MRE as high as 3.6. This system also uniquely recovers water in liquid form.

Colloidal nanocrystals (NCs) are promising candidates for a wide range of applications (electronics, optoelectronics, photovoltaics, thermoelectrics, etc.). Mechanical and thermal transport property play very important roles in all of these applications. On one hand, mechanical robustness and high thermal conductivity are desired in electronics, optoelectronics, and photovoltaics. This improves thermomechanical stability and minimizes the temperature rise during the device operation. On the other hand, low thermal conductivity is desired for higher thermoelectric figure of merit (ZT). This dissertation demonstrates that ligand structure and nanocrystal ordering are the primary determining factors for thermal transport and mechanical properties in colloidal nanocrystal assemblies. To eliminate the mechanics and thermal transport barrier, I first propose a ligand crosslinking method to improve the thermal transport across the ligand-ligand interface and thus increasing the overall thermal conductivity of NC assemblies. Young’s modulus of nanocrystal solids also increases simultaneously upon ligand crosslinking. My thermal transport measurements show that the thermal conductivity of the iron oxide NC solids increases by a factor of 2-3 upon ligand crosslinking. Further, I demonstrate that, though with same composition, long-range ordered nanocrystal superlattices possess higher mechanical and thermal transport properties than disordered nanocrystal thin films. Experimental measurements along with theoretical modeling indicate that stronger ligand-ligand interaction in NC superlattice accounts for the improved mechanics and thermal transport. This suggests that NC/ligand arranging order also plays important roles in determining mechanics and thermal transport properties of NC assemblies. Lastly, I show that inorganic ligand functionalization could lead to tremendous mechanical enhancement (a factor of ~60) in NC solids. After ligand exchange and drying, the short inorganic Sn2S64- ligands dissociate into a few atomic layers of amorphous SnS2 at room temperature and interconnects the neighboring NCs. I observe a reverse Hall-Petch relation as the size of NC decreases. Both atomistic simulations and analytical phase mixture modeling identify the grain boundaries and their activities as the mechanic bottleneck.