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This paper introduces oxygen‐deficient black TiO2 with hierarchically ordered porous structure fabricated by a simple hydrogen reduction as a carbon‐ and binder‐free cathode, demonstrating superior energy density and stability. With the high electrical conductivity derived from oxygen vacancies or Ti3+ ions, this unique electrode features micrometer‐sized voids with mesoporous walls for the effective accommodation of Li2O2 toroid and for the rapid transport of reaction molecules without the electrode being clogged. In the highly ordered architecture, toroidal Li2O2 particles are guided to form with a regular size and separation, which induces the most of Li2O2 external surface to be directly exposed to the electrolyte. Therefore, large Li2O2 toroids (≈300 nm) grown from solution can be effectively charged by incorporating a soluble catalyst, resulting in a very small polarization (≈0.37 V). Furthermore, disordered nanoshell in black TiO2 is suggested to protect the oxygen‐deficient crystalline core, by which oxidation of Ti3+ is kinetically impeded during battery operation, leading to the enhanced electrode stability even in a highly oxidizing environment under high voltage (≈4 V).

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Semiconductor sensitized solar cells, a promising candidate for next-generation photovoltaics, have seen notable progress using 0-D quantum dots as light harvesting materials. Integration of higher-dimensional nanostructures and their multi-composition variants into sensitized solar cells is, however, still not fully investigated despite their unique features potentially beneficial for improving performance. Herein, CdSe/CdSexTe1−x type-II heterojunction nanorods are utilized as novel light harvesters for sensitized solar cells for the first time. The CdSe/CdSexTe1−x heterojunction-nanorod sensitized solar cell exhibits ~33% improvement in the power conversion efficiency compared to its single-component counterpart, resulting from superior optoelectronic properties of the type-II heterostructure and 1-octanethiol ligands aiding facile electron extraction at the heterojunction nanorod-TiO2 interface. Additional ~32% enhancement in power conversion efficiency is achieved by introducing percolation channels of large pores in the mesoporous TiO2 electrode, which allow 1-D sensitizers to infiltrate the entire depth of electrode. These strategies combined together lead to 3.02% power conversion efficiency, which is one of the highest values among sensitized solar cells utilizing 1-D nanostructures as sensitizer materials.

Architectural control over the mesoporous TiO2 film, a common electron-transport layer for organic-inorganic hybrid perovskite solar cells, is conducted by employing sub-micron sized polystyrene beads as sacrificial template. Such tailored TiO2 layer is shown to induce asymmetric enhancement of light absorption notably in the long-wavelength region with red-shifted absorption onset of perovskite, leading to ~20% increase of photocurrent and ~10% increase of power conversion efficiency. This enhancement is likely to be originated from the enlarged CH3NH3PbI3(Cl) grains residing in the sub-micron pores rather than from the effect of reduced perovskite-TiO2 interfacial area, which is supported from optical bandgap change, haze transmission of incident light, and one-diode model parameters correlated with the internal surface area of microporous TiO2 layers. With the templating strategy suggested, the necessity of proper hole-blocking method is discussed to prevent any direct contact of the large perovskite grains infiltrated into the intended pores of TiO2 scaffold, further mitigating the interfacial recombination and leading to ~20% improvement in power conversion efficiency compared with the control device using conventional solution-processed hole blocking TiO2. Thereby, the imperatives that originate from the structural engineering of the electron-transport layer are discussed to understand the governing elements for the improved device performance.Electronic supplementary materialThe online version of this article (doi:10.1186/s11671-016-1809-7) contains supplementary material, which is available to authorized users.