Recent density-functional theory calculations suggest that codoping TiO 2 with donoracceptor pairs is more effective than monodoping for improving photoelectrochemical water-splitting performance because codoping can reduce charge recombination, improve material quality, enhance light absorption and increase solubility limits of dopants. Here we report a novel ex-situ method to codope TiO 2 with tungsten and carbon (W, C) by sequentially annealing W-precursor-coated TiO 2 nanowires in flame and carbon monoxide gas. The unique advantages of flame annealing are that the high temperature (41,000°C) and fast heating rate of flame enable rapid diffusion of W into TiO 2 without damaging the nanowire morphology and crystallinity. This is the first experimental demonstration that codoped TiO 2 :(W, C) nanowires outperform monodoped TiO 2 :W and TiO 2 :C and double the saturation photocurrent of undoped TiO 2 for photoelectrochemical water splitting. Such significant performance enhancement originates from a greatly improved electrical conductivity and activity for oxygen-evolution reaction due to the synergistic effects of codoping.
We report the first experimental study of catalytic CO oxidation over copper oxide (CuO) nanowires (NWs) grown directly on copper meshes. The catalytic activity of CuO NWs is significantly improved by a brief argon or hydrogen radio frequency plasma treatment. The plasma enhancement effect comes from the generation of grain boundaries and the reduction of Cu(II) to the more active oxidation state Cu(I) according to our TEM, XPS, and kinetic study.
The hybrid structure of nanoparticle-decorated nanowires (NP@NW) combines the merits of large specific surface areas for NPs and anisotropic properties for NWs and is a desirable structure for applications including batteries, dye-sensitized solar cells, photoelectrochemical water splitting, and catalysis. Here, we report a novel sol-flame method to synthesize the NP@NW hybrid structure with two unique characteristics: (1) large loading of NPs per NW with the morphology of NP chains fanning radially from the NW core and (2) intimate contact between NPs and NWs. Both features are advantageous for the above applications that involve both surface reactions and charge transport processes. Moreover, the sol-flame method is simple and general, with which we have successfully decorated various NWs with binary/ternary metal oxide and even noble metal NPs. The unique aspects of the sol-flame method arise from the ultrafast heating rate and the high temperature of flame, which enables rapid solvent evaporation and combustion, and the combustion gaseous products blow out NPs as they nucleate, forming the NP chains around NWs.
Doping nanowires (NWs) is of crucial importance for a range of applications due to the unique properties arising from both impurities' incorporation and nanoscale dimensions. However, existing doping methods face the challenge of simultaneous control over the morphology, crystallinity, dopant distribution and concentration at the nanometer scale. Here, we present a controllable and reliable method, which combines versatile solution phase chemistry and rapid flame annealing process (sol-flame), to dope TiO2 NWs with cobalt (Co). The sol-flame doping method not only preserves the morphology and crystallinity of the TiO2 NWs, but also allows fine control over the Co dopant profile by varying the concentration of Co precursor solution. Characterizations of the TiO2:Co NWs show that Co dopants exhibit 2+ oxidation state and substitutionally occupy Ti sites in the TiO2 lattice. The Co dopant concentration significantly affects the oxygen evolution reaction (OER) activity of TiO2:Co NWs, and the TiO2:Co NWs with 12 at% of Co on the surface show the highest OER activity with a 0.76 V reduction of the overpotential with respect to undoped TiO2 NWs. This enhancement of OER activity for TiO2:Co NWs is attributed to both improved surface charge transfer kinetics and increased bulk conductivity.
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