h i g h l i g h t sRecent progress in enhancing solar-to-hydrogen (STH) efficiency is reviewed. Light absorption, charge separation-migration and surface reaction are evaluated. Doping, quantum dot, and plasmon enhancement are the keys to high STH efficiency. Co-catalysts and nanostructured surfaces improve surface reactions effectively. Multiple excitons, upconversion, and synergic strategies are promising areas.
a b s t r a c tSolar water splitting is a promising and ideal route for renewable production of hydrogen by using the most abundant resources of solar light and water. Focusing on the working principal of solar water splitting, including photon absorption and exciton generation in semiconductor, exciton separation and transfer to the surface of semiconductor, and respective electron and hole reactions with absorbed surface species to generate hydrogen and oxygen, this review covers the comprehensive efforts and findings made in recent years on the improvement for the solar-to-hydrogen efficiency (STH) determined by a combination of light absorption process, charge separation and migration, and catalytic reduction and oxidation reactions. Critical evaluation is attempted on the strategies for improving solar light harvesting efficiency, enhancing charge separation and migration, and improving surface reactions. Towards the end, new and emerging technologies for boosting the STH efficiency are discussed on multiple exciton generation, up-conversion, multi-strategy modifications and the potentials of organometal hybrid perovskite materials.
Hybrid inorganic-organic perovskites have quickly evolved as a promising group of materials for solar cells and optoelectronic applications mainly owing to the inexpensive materials, relatively simple and versatile fabrication and high power conversion efficiency (PCE). The certified energy conversion efficiency for perovskite solar cell (PSC) has reached above 20%, which is compatible to the current best for commercial applications. However, long-term stabilities of the materials and devices remain to be the biggest challenging issue for realistic implementation of the PSCs. This article discusses the key issues related to the stability of perovskite absorbing layer including crystal structural stability, chemical stability under moisture, oxygen, illumination and interface reaction, effects of electron-transporting materials (ETM), hole-transporting materials (HTM), contact electrodes and preparation conditions. Towards the end, prospective strategies for improving the stability of PSCs are also briefly discussed and summarized. We focus on recent understanding of the stability of materials and devices and our perspectives about the strategies for the stability improvement.
The Ta3N5 semiconductor photocatalyst possesses a 720 nm (about 1.72 eV) sub-band-gap optical absorption but the mechanism of this optical absorption is still controversial. In this study, the hybrid density functional theory calculations are performed to unravel the mechanism of 720 nm sub-band-gap optical absorption of Ta3N5. By studying the possible optical absorption initiated by the ON impurity and the VN defect, we find that the 720 nm sub-band-gap optical absorption of Ta3N5 may be ascribed to the electron transition from V(·)(N) to V(···)(N). In addition, we propose that the 720 nm sub-band-gap optical absorption can be used to qualitatively evaluate the photocatalytic water splitting ability of Ta3N5.
The arrangement of the electrode materials is a significant contributor for constructing high performance supercapacitor. Here, vertically-aligned Mn(OH)2 nanosheet thin films were synthesized by cathodic electrodeposition technique on flexible Au coated polyethylene terephthalate substrates. Morphologies, microstructures, chemical compositions and valence state of the nanosheet films were characterized systematically. It shows that the nanosheets arranged vertically to the substrate, forming a porous nanowall structures and creating large open framework, which greatly facilitate the adsorption or diffusion of electrolyte ions for faradaic redox reaction. Electrochemical tests of the films show the specific capacitance as high as 240.2 F g−1 at 1.0 A g−1. The films were employed to assemble symmetric all-solid-state supercapacitors with LiCl/PVA gel severed as solid electrolyte. The solid devices exhibit high volumetric capacitance of 39.3 mF cm−3 at the current density 0.3 mA cm−3 with robust cycling stability. The superior performance is attributed to the vertically-aligned configuration.
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