ABSTRACT
To solve the intrinsic deficiency inherited from the large band gap of ZnSn(OH)6 (ZSH), a gradual sulfur doping strategy is first proposed here to expand the optical absorption range, improve the separation efficiency of photogenerated electron-hole pairs, and thus enhance the photocatalytic activity. It is demonstrated that the distribution of sulfur in the flower-like ZSH (the sulfur doped sample is denoted as S-ZSH) tends to be largest on the outer most surface and becomes smaller towards the interior. The S-ZSH therefore has a gradual bandgap structure that is beneficial for transferring photogenerated charge carriers from the interior to the surface, which will greatly enhance the utilization of photoelectrons. As a result, the visible light photocurrent density of S-ZSH and the photocatalytic degradation rate of rhodamine (RhB) are about 5 and 10 times higher than with pristine ZSH, respectively.
ABSTRACT
Herein, we have successfully introduced the stimuli-response concept into the controllable synthesis of gold nanoparticles (AuNPs) with designed properties. We used a pH-responsive zwitterionic polymer that acted as a template and a stabilizer. Gold colloids prepared in situ from the polymer solution have a narrow size distribution of about 5 nm. The assembly and disassembly of AuNPs can be finely tuned by modulating the net charges of the zwitterionic polymer so that they are either positive or negative as a function of the solution pH. Different aggregates and colors appear on altering the solution pH. In acidic solutions, gold colloids form large symmetrical aggregates, while the AuNPs disperse in solutions with a pH approximately 9.6. However, as the solution pH increases (>9.6), needle-like aggregates with a small interparticle distances are formed. On the basis of TEM, SEM, 1H NMR and UV/Vis measurements, we attribute pH-triggered aggregation and color changes of the gold colloids to the ionization process and conformational change of the polymer. The ionization process governs the choice of ligand anchored on the surface of AuNPs, and the conformational change of the polymer modulates the interspaces between AuNPs. The present approach, which is based on a rational design of the physicochemical properties of the template used in the synthesis process, provides a powerful means to control the properties of the nanomaterial. Furthermore, the colorimetric readout can be visualized and applied to future studies on nanoscale switches and sensors.
