Hydrogen is a clean energy source that is environmentally friendly and safe. It is well known that electrolysis is a common
method used to produce hydrogen. Other high cost methods for hydrogen production can be countered by the development
of this low cost pulse width modulated circuit, using direct current provided by naturally existing solar energy as a power
source. Efforts are being made in the scientific community to produce a low cost, portable, solar hydrogen generating
device for a number of clean energy applications such as fuel cells and energy storage. Proof of concept has already been
tested in the laboratory and a small prototype system is being designed and fabricated in the workshop at Alabama A&M
University. Our results of this study and details of the electronic circuit and the prototype are presented.
The development of an efficient catalyst for the oxidative splitting of water into molecular oxygen, protons and electrons is of key importance for producing solar fuels through artificial photosynthesis. We are facing the problem by means of a rational approach aimed at understanding how catalytic performance may be optimized by the knowledge of the reaction mechanism of water oxidation and the fate of the catalytic site under the inevitably harsh oxidative conditions. For the purposes of our study we selected iridium water oxidation catalysts, exhibiting remarkable performance (TOF > 5 s-1 and TON > 20000). In particular, we recently focused our attention on [Cp*Ir(N,O)X] (N,O = 2-pyridincarboxylate; X = Cl or NO3) and [IrCl(Hedta)]Na water oxidation catalysts. The former exhibited a remarkable TOF whereas the latter showed a very high TON. Furthermore, [IrCl(Hedta)]Na was heterogenized onto TiO2 taking advantage of the presence of a dandling –COOH functionality. The heterogenized catalyst maintained approximately the same catalytic activity of the homogeneous analogous with the advantage that could be reused many times. Mechanistic studies were performed in order to shed some light on the rate-determining step and the transformation of catalysts when exposed to “oxidative stress”. It was found that the last oxidative step, preceding oxygen liberation, is the rate-determining step when a small excess of sacrificial oxidant is used. In addition, several intermediates of the oxidative transformation of the catalyst were intercepted and characterized by NMR, X-Ray diffractometry and ESI-MS.
A flux-assisted method was used to synthesize SnNb2O6 as a visible-light-responsive metal oxide photocatalyst. The role of synthesis temperature was investigated in detail using different reaction temperatures (300, 500, 600, 800, 1000 °C). The obtained products were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller method (BET). The synthesis with SnCl2 as a flux led to tin niobate particles in the platelet morphology with smooth surfaces. The synthesized crystal showed 2D anisotropic growth along the (600) plane as the flux ratio increased. The particles synthesized with a high reactant to flux ratio (1:10 or higher) exhibited improved photocatalytic activity for hydrogen evolution from an aqueous methanol solution under visible radiation (λ > 420 nm).
The preparation of SiO2-coated Ag nanoparticles dispersible in various organic solvents has been achieved using a solgel reaction of tetraethylorthosilicate (TEOS), in the localized hydrophilic pool segments designed on Ag nanoparticle surfaces. First, oleylamine-capped core Ag nanoparticles were synthesized, followed by ligand exchange with polyethyleneimine (PEI) and further adsorption of an anionic surfactant comprising hydrophilic polyethylene glycol (PEG) chains and hydrophobic alkyl chains, which has previously been reported to improve the stability of nanoparticles in various solvents. Then, a reaction of TEOS with the localized hydrophilic PEI layer on the Ag nanoparticles’ surface was conducted by stirring a toluene/TEOS solution of surface-modified Ag nanoparticles at various temperatures. It was found that a SiO2 layer was successfully formed on Ag nanoparticles when the reaction temperature was increased to 60 °C. It was also found, however, that at this elevated temperature, the primary particle size of Ag nanoparticles increased to several tens of nm, attributable to the dissolution and re-reduction of Ag+. Because the surface modifier, PEI and anionic surfactant all remained on the nanoparticle surface during the SiO2 coating process, the prepared SiO2-coated Ag nanoparticles were found to be dispersible in various organic solvents near to their primary particle size.
In this report we present the fabrication of III-nitride devices with nanoporous structure used as photoelectrodes for solar water splitting. Photoelectrochemical etching in a KOH solution of the GaN and InGaN/GaN devices at different concentrations and applied voltages has been employed to fabricate both planar and nanorod devices into nanoporous structures with controllable pore sizes. Photoluminescence measurements of the GaN and InGaN/GaN multi-quantum well (MQW) with nanoporous structures have shown an increase in intensity over the un-etched samples as a result of the release of the compressive strain which nitride samples grown on sapphire suffer. An enhancement in both photocurrent and hydrogen generation has been achieved across all samples with the nanoporous structure compared to their standard counterparts. Improved carrier extraction as a result of the enhanced surface area allows for better charge-transfer between the electrode and electrolyte. The significantly enhanced incident photon conversion efficiency (IPCE) of all nanoporous devices has been obtained.
A facile and simple fabrication of Zn-doped α-Fe2O3 thin films as a photocathode for solar hydrogen generation was proposed in this report. Transparent Zn-doped α-Fe2O3 films were prepared by a deposition-annealing (DA) process using nontoxic iron(III) chloride as the Fe precursor and zinc chloride as a acceptor dopant, followed by annealing at 550 °C in air. In terms of the structural examination of as-grown samples, X-ray diffraction analysis demonstrated an increase in the lattice parameters of Zn incorporated in Fe2O3 by substituting Fe in the host lattice. No second phase was determined, indicating no phase separation in the ternary materials. Energy dispersive spectroscopy results demonstrated that Zn, Fe, and O elements existed in the deposits. Furthermore, impedance measurements show that the Zn-dopant serves as an hole acceptor and increases the acceptor concentration by increasing concentration of zinc precursor. Significantly, the photoelectrochemical measurements exhibited remarkable cathodic current, corresponding to the reduction reaction of hydrogen. Finally, the optimum photocurrent can be achieved by controlled variation of the Fe and Zni precursor concentration, annealing conditions, and the number of DA cycles. According to our investigation, the understandings of morphology effect on PEC activity give the blueprint for materials design in the application of solar hydrogen.