Ag nanowire-based catalytic liquid marbles are fabricated as miniature reactors, which demonstrate highly efficient, support-free and rate-controllable heterogeneous degradation of methylene blue, with catalytic efficiency close to 100%. Our miniature catalytic liquid marbles are essential for reactions involving highly toxic/hazardous or costly reactants, where small volume preliminary reactions are preferred.
Current synthesis of gold nanoframes has only demonstrated morphological control over wall thickness and wall length. Here, we demonstrate the ability to control the nanoscale porosity of these nanoframes, using a templated seed-mediated approach. The porosity on these nanoporous gold nanoframes (NGNs) is tuned by controlling the crystallite size of Au nanoparticles deposited on the AgCl templates. The yield of the NGNs approaches 100%. Despite its minimalist architectural construction, the NGNs are mechanically robust, retaining its morphology even after multiple centrifugation and sonication rounds. We further highlight that decreasing the porosity on the NGN leads to improved surface-enhanced Raman scattering (SERS) enhancement. Increasing the constituent Au crystallite size decreases the porosity, but increases the surface roughness of NGN, hence leading to greater SERS enhancement. The introduction of porosity in a gold nanoframe structure through our synthesis method is novel and generic, suggesting the extendibility of our method to other types of templates.
Miniaturizing the continuous multistep operations of a factory into a microchemical plant offers a safe and cost-effective approach to promote high-throughput screening in drug development and enforcement of industrial/environmental safety. While particle-assembled microdroplets in the form of liquid marble are ideal as microchemical plant, these platforms are mainly restricted to single-step reactions and limited to ex situ reaction monitoring. Herein, we utilize plasmonic liquid marble (PLM), formed by encapsulating liquid droplet with Ag nanocubes, to address these issues and demonstrate it as an ideal microchemical plant to conduct reaction-and-detection sequences on-demand in a nondisruptive manner. Utilizing a two-step azo-dye formation as our model reaction, our microchemical plant allows rapid and efficient diazotization of nitroaniline to form diazonium nitrobenzene, followed by the azo coupling of this intermediate with target aromatic compound to yield azo-dye. These molecular events are tracked in situ via SERS measurement through the plasmonic shell and further verified with in silico investigation. Furthermore, we apply our microchemical plant for ultrasensitive SERS detection and quantification of bisphenol A (BPA) with detection limit down to 10 amol, which is 50 000-fold lower than the BPA safety limit. Together with the protections offered by plasmonic shell against external environments, these collective advantages empower PLM as a multifunctional microchemical plant to facilitate small-volume testing and optimization of processes relevant in industrial and research contexts.
Last but not least, thank you to my parents for their upbringing, support, kindness, and love throughout my life. Without them, I would not be who I am today. Also, thank you to my brother for his support and guidance. He paved his way to his doctorate which made me realize the possibility of walking this road. Finally, this thesis is dedicated to my late grandmother, Madam Ho Nya Yan.
Carbon nitride is a material of interest for photocatalytic reactions due to its catalytic and visible light absorption properties. However, the photocatalytic activity is still low. Hence, modifications must be carried out to improve the photocatalytic activity of carbon nitride. In this work, a series of gallium oxide/carbon nitride composites with various gallium to carbon ratios (Ga/C = 1-50 mol%) was prepared by impregnation method for removal of cyclohexane under visible light irradiation for the first time. The successful preparation of gallium oxide/carbon nitride composites was supported by several characterization techniques. X-ray diffraction (XRD) patterns and diffuse reflectance UV-visible (DR UV-vis) spectra revealed that the increased Ga/C ratio resulted in the increased formation of Ga2O3. Furthermore, all the prepared composite samples also showed visible light absorption up to about 430 nm. In the photocatalytic removal of cyclohexane under 6 h of visible light irradiation, sample with low loading of 1 mol% Ga/C improved the photocatalytic activity of carbon nitride for two times. The high activity obtained on the gallium oxide (1 mol%)/carbon nitride composite clearly suggested the presence of synergic effect between small amount of gallium oxide and carbon nitride when they were combined. This study showed that a visible light-driven gallium oxide/carbon nitride composite could be prepared by impregnating a small amount of gallium oxide on carbon nitride and the composite is a potential photocatalyst for removal of cyclohexane under visible light irradiation.
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