A p-type metal oxide with high surface area and good charge carrier mobility is of paramount importance for development of tandem solar fuel and dye-sensitized solar cell (DSSC) devices. Here, we report the synthesis, hierarchical morphology, electrical properties, and DSSC performance of mesoscale p-type NiO platelets. This material, which exhibits lateral dimensions of 100 nm but thicknesses less than 10 nm, can be controllably functionalized with a high-density array of vertical pores 4−6, 5−9, or 7−23 nm in diameter depending on exact synthetic conditions. Thin films of this porous but still quasi-two-dimensional material retain a high surface area and exhibit electrical mobilities more than 10-fold higher than comparable films of spherical particles with similar doping levels. These advantages lead to a modest, 20−30% improvement in the performance of DSSC devices under simulated 1-sun illumination. The capability to rationally control morphology provides a route for continued development of NiO as a high-efficiency material for tandem solar energy devices.
Sensitized SrTiO3 films were evaluated as potential photoanodes for dye-sensitized photoelectrosynthesis cells (DSPECs). The SrTiO3 films were grown via pulsed laser deposition (PLD) on a transparent conducting oxide (fluorine-doped tin oxide, FTO) substrate, annealed, and then loaded with zinc(II) 5,10,15-tris(mesityl)-20-[(dihydroxyphosphoryl)phenyl] porphyrin (MPZnP). When paired with a platinum wire counter electrode and an Ag/AgCl reference electrode these sensitized films exhibited photocurrent densities on the order of 350 nA/cm(2) under 0 V applied bias conditions versus a normal hydrogen electrode (NHE) and 75 mW/cm(2) illumination at a wavelength of 445 nm. The conditions of the post-deposition annealing step-namely, a high-temperature reducing atmosphere-proved to be the most important growth parameters for increasing photocurrent in these electrodes.
Beneath the seeming straight-forwardness of growing carbon nanotube (CNT) forests by the injection chemical vapor deposition (CVD) method, control of the forest morphology on various substrates is yet to be achieved. Using ferrocene dissolved in xylene as the precursor, we demonstrate that the concentration of ferrocene and the injection rate of the precursor dictate the CNT density of these forests. However, CNT density will also be affected by the substrates and the growth temperature which determine the diffusion of the catalyst adatoms. The CNT growth rate is controlled by the temperature and chemical composition of the gases in the CVD reactor. We show that the final height of the forest is diffusion limited, at least in the conditions of our experiments. Because of the proximity and entanglement of the CNTs in a forest, the growing CNTs can lift-up the inactive CNTs resulting in reduced density toward the base of the forest unless the nucleation rate of the new catalyst particles is sufficiently high to replenish the inactive catalyst particles. Significant loss of CNT attachment by the lift-up effect reduces the adhesion of the forest to the substrate. Optimizing the ferrocene concentration in the precursor, precursor injection rate, gas mixture, substrate, and temperature is necessary to achieve desired forest morphology for specific applications. V
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