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Bismuth vanadate (BiVO4) is one of the most promising metal oxide semiconductors for photoelectrochemical (PEC) water oxidation. Much efforts have been dedicated on accelerating the sluggish surface water oxidation kinetics. In this study, plasma enhanced atomic layer deposition and subsequent removal of Al2O3 ultrathin overlayers on bismuth vanadate were implemented to achieve the successful passivation of surface states and significant enhancement of PEC performance. Al2O3 ultrathin overlayers were first coated on BiVO4 surface via plasma enhanced atomic layer deposition with various deposition cycles, which resulted in the decrease of PEC water oxidation activity due to the poor conductivity. The subsequent removal of surface amorphous Al2O3 passivated the surface states of the photoanodes and significantly enhanced the photocurrent densities. The passivated BiVO4 exhibited a photocurrent density of 1.34 mA·cm−2 at 1.23 V vs. RHE, which is 73% higher than that of unmodified BiVO4. This work provides a novel strategy and deep insights on surface modification of semiconductor for photoelectrochemical energy conversion.

Porous photoelectrodes show high efficiency in hydrogen production by water splitting. However, fabrication of porous nanorods is usually difficult. Here, we report a simple approach to fabricate a kind of novel porous rutile titanium dioxide nanorod array by an advanced ion implantation method using multiple-energy helium ion implantation and subsequent annealing. The porous nanostructure enhances the photoelectrochemical performance of the titanium dioxide nanorod array photoelectrodes under Uv-visible light illumination, where the highest photocurrent density was relatively about 10 times higher than that of the pristine titanium dioxide nanorod array. The formation of nanocavities mainly contributes to the enhancement of the photocurrent density by trapping holes inside to separate the charge carriers. The study demonstrates that ion implantation could be an effective approach to develop novel porous nanostructural photoelectrodes for the application of hydrogen production.

Novel hybrid tetra-nitro-phthalocyanine Copper(II) (TNCuPc)/TiO2 films were successfully synthesized using a simple hydrothermal and solvothermal method. The successful deposition of TNCuPc on the TiO2 nanorods was confirmed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The precursor concentration for hydrothermal deposition of TiO2 was optimized for light absorption and photoelectrochemical (PEC) water splitting. The hierarchical nanostructure exhibited increased light absorption ability and enhanced PEC properties. Moreover, the concentration of the precursor solution for TNCuPc deposition was also optimized for the performance of the TNCuPc/TiO2 hybrid nanostructure. The optimal sample achieved the highest photocurrent of 1.1 mA cm−2 and the highest IPCE of 51% at 610 nm.

Anisotropic nanopatterns have potentials in constructing novel plasmonic structures which have various applications in such as super-resolution microscopy, medicine, and sensors. However, it remains challenging to build big anisotropic nanopatterns that are suitable for big noble metal nanoparticles. Herein, we report a simple and reliable strategy for constructing DNA origami-based big anisotropic nanopatterns with controlled size and shape, nanoscale resolution, and fully addressability. Two kinds of basic DNA origami nanoblocks - cross-shaped and rectangular DNA origami units were used. We have demonstrated that by encoding nanoblocks' edges, anisotropic higher-order nanopatterns, such as dimer, trimer, tetramer and mini "windmill" like pentamer nanopatterns could be constructed. To show the potential use as template to direct the assembly of anisotropic nanoparticles arrays, a proof of concept work was conducted by anchoring streptavidin nanoparticles on the "windmill" template to form a chiral array. Significantly, these nanopatterns have the sizes of hundreds of nanometers, which are in principle also suitable for big noble metal nanoparticles arrays.

Ta-doped hematite (α-Fe2O3) nanorod array films were successfully prepared on fluorine-doped tin dioxide (FTO) coated glass substrates via a facile solution growth process with TaCl5 as a Ta doping precursor. Under 1 sun illumination and at an applied potential of 1.0 V vs. Ag/AgCl, the Ta-doped α-Fe2O3 photoanode with optimized dopant concentration showed a photocurrent density as high as 0.53 mA cm(-2), which was about 3.5 times higher than that of the undoped sample. As demonstrated by Mott-Schottky and X-ray absorption spectroscopy measurements, considerable increase in photoelectrochemical (PEC) performance achieved for Ta-doped α-Fe2O3 nanorod films should be mainly attributed to the increased electron donor density induced by Ta doping. However, with superfluous Ta doping, the [110]-oriented nanorod structure was destroyed, which caused greatly restrained photoinduced holes transferring to the surface and retarded surface water oxidation reaction, leading to decreased PEC water splitting activity. This study clearly demonstrated that doping could be effective to enhance the PEC activity of α-Fe2O3 nanorods as photoanodes, while it is of great necessity to balance the trade-off between the electronic structure and nanostructure evolution by optimizing the dopant concentration, for increased donor density and meanwhile with the nanorod nanostructure well preserved for directed charge transfer.

Apart from providing the material for genetic information storage, DNA has also been regarded as a useful building block in the field of nanotechnology, which is known as DNA nanotechnology. Based on the Watson-Crick base-pairing and the famous double helical structure, a library of DNA 2D or 3D nanostructures has been designed, constructed and characterized, by either tile-based or origami-based self-assembly. More significantly, other molecules/nanomaterials can be organized on those DNA ensembles to achieve highly ordered arrays or specific patterns in nanometer spatial resolution. In this review, we summarize recent progress in creating DNA nanoarchitectures, and discuss potential applications in DNA-based nanofabrication.

A solution-phase DNA chip is produced using DNA origami-based asymmetric self-assembled tiles incorporating single-stranded DNA linear probes. This DNA origami chip is fully spatially addressable, without having to use position index oligonucleotides. The DNA hybridization is readily detected via atomic force microscopy.

Molecular computing holds great promise for diagnosis and treatment of diseases at the molecular level; nevertheless, designing molecular logic gates to operate programmably and autonomously for molecular diagnostics still remains challenging. We designed logic gates on DNA Origami for microRNA analysis. As a demonstration, two indicators of heart failure, microRNA-21 and microRNA-195, were selected as the logic inputs. The logic gates contain two main modules: computation module and output module, performing in a single DNA Origami nanostructure. The computation module recognizes disease indicators, while the output module display different nanoscale symbols, “+” (positive) or “–” (negative), depending on the computing results. We demonstrated that the molecular logic gates worked well with single and two input combinations.

Self-assembled DNA origami nanostructures have shown great promise for bottom-up construction of complex objects with nanoscale addressability. Here we show that DNA origami-based ID nanoribbons and nanotubes are one-pot assembled with controllable sizes and nanoscale addressability with high speed (within only 10-20 min), exhibiting extraordinarily high cooperativity that is often observed in assembly of natural molecular machines in cells (e.g. ribosome). By exploiting the high specificity of DNA-based self-assembly, we can precisely anchor proteins on these DNA origami nanostructures with sub-10 nm resolution and at the single-molecule level. We attach a pair of enzymes (horseradish peroxidase and glucose oxidase) at the inner side of DNA nanotubes and observe high coupling efficiency of enzyme cascade within this confined nanospace. Hence, DNA nanostructures with such unprecedented properties shed new light on the design of nanoscale bioreactors and nanomedicine and provide an artificial system for studying enzyme activities and cascade in highly organized and crowded cell-mimicking environments.

Individual biomolecular binding events were recorded in situ by combining time-lapse atomic force microscopy and DNA origami. Single streptavidin molecules bound to specifically biotinyated DNA origami were simply counted as a function of time to obtain a direct measure of the binding rate.

ZnFe2O4 modified α-Fe2O3 nanorod array films were successfully synthesized by aqueous solution growth followed by a spin coating process and studied for photoelectrochemical (PEC) water splitting under solar light. Through the spin coating process, ZnFe2O4 was found mainly to exist at the top surface of the α-Fe2O3 nanorod arrays. After being modified by ZnFe2O4, the α-Fe2O3 nanorod film was identified as a suitable surface treatment, and showed an increased photocurrent density when used as the photoanode. It was demonstrated that ZnFe2O4 increased the charge carrier density and acted as the oxidation cocatalyst. These results suggested that surface treatment by ZnFe2O4 should be a practical strategy to improve the efficiency of α-Fe2O3 or other metal oxide photoanodes for PEC solar fuel conversion.