In this study, WO3 and NiO thin films were deposited on the ITO/Glass substrates by radio frequency (RF) magnetron sputtering, respectively. The physical and electrochromic properties of thin films were investigated. On the other hand, the lithium perchlorate (LiClO4) powder was dispersed in propylene carbonate (PC) solvent to complete 1 M electrolyte. Then, as the 4.5 wt.% of ethyl cellulose and 8 wt.% ethylene carbonate (EC) were added to this electrolyte under stirring, a gel polymer electrolyte (GPE) was formed. Finally, the WO3 and NiO thin films obtained with the optimal deposition parameters were combined with the GPE to set up a complementary electrochromic device (CECD). The effects of the various coloring voltages on the electrochromic properties of CECD are investigated. The memory effect, energy-saving efficient, response time and switch lifetime of CECD are also estimated and discussed. Experimental results reveal that the amorphous thin films can be obtained with the RF power of 100 W and oxygen concentration of 60% at room temperature (RT). The thicknesses of WO3 and NiO films were approximately 530 nm and 180 nm, respectively. The stoichiometric of thin films were 2.99 for O/W ratio and 1.01 for O/Ni ratio. The GPE [(1 M LiClO4+PC)+ethyl cellulose(4.5 wt.%)+EC(8 wt.%)] exhibits a viscosity coefficient of 100 mPa∙s, a maximum ion conductivity (£m) of 7.17 mS/cm, a minimum activation energy (Ea) of 0.033 eV and a average visible transmittance of 82% at RT. The optimal electrochromic CECD (Glass/ITO/WO3/GPE/NiO/ITO/Glass) biased with a coloring/bleaching voltage of ¡Ó2.2 V revealed a transmittance variation (£GT%) of 54.53%, an optical density change (£GOD) of 0.790, an intercalation charge (Q) of 6.28 mC/cm2 and a coloration efficiency (£b) of 125.21 cm2/C at a wavelength (£f) of 550 nm. The chromaticity coordinates of CECD were x=0.289 and y=0.365 under the colored state. In addition, the energy-saving efficient of CECD was 15.19 W/V-m2 over the wavelength range between 380 nm and 780 nm. Also, it presented an open-circuit memory effect that the colored transmittance (£f at 550 nm) was 18.9% in 24 h. The total response time of the CECD was about 4 s for coloring and bleaching steps. After the repeated switch of 1,000 times, the £GT% of CECD was 43.57%. In this study, WO3 and NiO thin films with good adhesion, amorphous, and nearly stoichiometric were successfully deposited by RF sputter. Furthermore, high £m and high transmittance of GPE can be prepared easily and inexpensively. Our results demonstrated that the CECD exhibited the advantages of low applied voltage, high £b, fast response time and long-term memory characteristics.

Philosophiae Doctor - PhD / In this work we primarily set out to investigate the technique of Aqueous Chemical Growth as a means of producing WO3 thin films that find applications in gas sensing and electrochromism. For the first time we demonstrated in this work, the heterogenous nucleation and growth of WO3 thin films on plain glass substrates and F-doped SnO2-glass substrates. This was achieved without the use of surfactants and template directing methods, using as a precursor solution Peroxotungstic Acid generated from the action of 30% H2O2 on pure W powder. The substrates used needed no surface-modification. On the plain glass substrates (soda lime silicates) a variety of micronanostructures could be observed prime of which were nanoplatelets that acted as a basic building block for the self-assembly of more hierarchical 3-d microspheres and thin films. On FTO a wide variety of micro-/nanostructures were observed dominant amongst which were urchin-like microspheres. The dominant crystallographic structure observed (through X-ray diffraction analysis, SAED, HRTEM) for the WO3 thin films on both substrate types post-annealing at 500 ˚C for a period of 1 - 2 h, was hexagonal-WO3. Next was monoclinic WO3. On rarer occasions the formation of triclinic and cubic WO3 was observed. The thin films produced showed a fairly high degree of porosity and had thicknesses in the range of 900 nm - 3.5 μm. I-V characterisation measurements using a 4-point collinear probe Keithley source alongside photoluminescence was used to establish the insulating nature of some of the films as well as their sub-stoichiometric nature. X-ray Photoelectron Spectroscopy was used to confirm the substoichiometric nature of some of the films.

Electrochromic devices (ECDs) have emerged as a unique class of optoelectronic devices for the development of smart windows. However, current ECDs typically suffer from low coloration efficiency (CE) and high energy consumption, which have thus hindered their practical applications, especially as components in solar-powered EC windows. Here, the high-performance ECDs with a fully crystalline viologen-immobilized 2D polymer (V2DP) thin film as the color-switching layer is demonstrated. The high density of vertically oriented pore channels (pore size ≈ 4.5 nm; pore density ≈ 5.8 × 1016 m-2) in the synthetic V2DP film enables high utilization of redox-active viologen moieties and benefits for Li+ ion diffusion/transport. As a result, the as-fabricated ECDs achieve a rapid switching speed (coloration, 2.8 s; bleaching, 1.2 s), and a high CE (989 cm2 C-1), and low energy consumption (21.1 µW cm-2). Moreover, it is managed to fabricate transmission-tunable, self-sustainable EC window prototypes by vertically integrating the V2DP ECDs with transparent solar cells. This work sheds light on designing electroactive 2D polymers with molecular precision for optoelectronics and paves a practical route toward developing self-powered EC windows to offset the electricity consumption of buildings.