Achieving high solar-to-hydrogen (STH) efficiency concomitant with long-term durability using low-cost, scalable photo-absorbers is a long-standing challenge. Here we report the design and ...fabrication of a conductive adhesive-barrier (CAB) that translates >99% of photoelectric power to chemical reactions. The CAB enables halide perovskite-based photoelectrochemical cells with two different architectures that exhibit record STH efficiencies. The first, a co-planar photocathode-photoanode architecture, achieved an STH efficiency of 13.4% and 16.3 h to t
, solely limited by the hygroscopic hole transport layer in the n-i-p device. The second was formed using a monolithic stacked silicon-perovskite tandem, with a peak STH efficiency of 20.8% and 102 h of continuous operation before t
under AM 1.5G illumination. These advances will lead to efficient, durable, and low-cost solar-driven water-splitting technology with multifunctional barriers.
Formation of planar heterojunction perovskite solar cells exhibiting both high efficiency and stability under continuous operation remains a challenge. Here, we show this can be achieved by using a ...defective TiO2 thin film as the electron transport layer. TiO2 layers with native defects are deposited by electron beam evaporation in an oxygen-deficient environment. Deep-level hole traps are introduced in the TiO2 layers and contribute to a high photoconductive gain and reduced photocatalytic activity. The high photoconductivity of the TiO2 electron transport layer leads to improved efficiency for the fabricated planar devices. A maximum power conversion efficiency of 19.0% and an average PCE of 17.5% are achieved. In addition, the reduced photocatalytic activity of the TiO2 layer leads to enhanced long-term stability for the planar devices. Under continuous operation near the maximum power point, an efficiency of over 15.4% is demonstrated for 100 h.
The performance of energy materials hinges on the presence of structural defects and heterogeneity over different length scales. Here we map the correlation between morphological and functional ...heterogeneity in bismuth vanadate, a promising metal oxide photoanode for photoelectrochemical water splitting, by photoconductive atomic force microscopy. We demonstrate that contrast in mapping electrical conductance depends on charge transport limitations, and on the contact at the sample/probe interface. Using temperature and illumination intensity-dependent current-voltage spectroscopy, we find that the transport mechanism in bismuth vanadate can be attributed to space charge-limited current in the presence of trap states. We observe no additional recombination sites at grain boundaries, which indicates high defect tolerance in bismuth vanadate. These findings support the fabrication of highly efficient bismuth vanadate nanostructures and provide insights into how local functionality affects the macroscopic performance.
Despite the high charge-carrier mobility in covalent organic frameworks (COFs), the low intrinsic conductivity and poor solution processability still impose a great challenge for their applications ...in flexible electronics. We report the growth of oriented thin films of a tetrathiafulvalene-based COF (TTF-COF) and its tunable doping. The porous structure of the crystalline TTF-COF thin film allows the diffusion of dopants such as I 2 and tetracyanoquinodimethane (TCNQ) for redox reactions, while the closely packed 2D grid sheets facilitate the cross-layer delocalization of thus-formed TTF radical cations to generate more conductive mixed-valence TTF species, as is verified by UV-vis-NIR and electron paramagnetic resonance spectra. Conductivity as high as 0.28 S m −1 is observed for the doped COF thin films, which is three orders of magnitude higher than that of the pristine film and is among the highest for COF materials.
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