Order/disorder interfacial engineering realizes highly efficient co-catalyst free hydrogen generation.

Sub-micrometer-sized colloidal graphite (CG) was tested as a conducting electrode to replace transparent conducting oxide (TCO) electrodes and as a catalytic material to replace platinum (Pt) for I(3)(-) reduction in dye-sensitized solar cell (DSSC). CG paste was used to make a film via the doctor-blade process. The 9 μm thick CG film showed a lower resistivity (7 Ω/◻) than the widely used fluorine-doped tin oxide TCO (8-15 Ω/◻). The catalytic activity of this graphite film was measured and compared with the corresponding properties of Pt. Cyclic voltammetry and electrochemical impedance spectroscopy studies clearly showed a decrease in the charge transfer resistance with the increase in the thickness of the graphite layer from 3 to 9 μm. Under 1 sun illumination (100 mW cm(-2), AM 1.5), DSSCs with submicrometer-sized graphite as a catalyst on fluorine-doped tin oxide TCO showed an energy conversion efficiency greater than 6.0%, comparable to the conversion efficiency of Pt. DSSCs with a graphite counter electrode (CE) on TCO-free bare glass showed an energy conversion efficiency greater than 5.0%, which demonstrated that the graphite layer could be used both as a conducting layer and as a catalytic layer.

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Bulk and surface charge recombination of photoelectrode are two key processes that significantly hinder solar‐to‐fuel conversion of photoelectrochemical cell (PEC). In this study, the function of a “crystal‐deficient” overlayer is unveiled, which outperforms a traditionally used amorphous or crystalline overlayer in PEC water splitting by exhibiting a high conductivity and large electron diffusion length to enable unlimited electron collection. The optimized ≈2.5 nm thickness of the “crystal‐deficient” shell results in a depletion layer with a width of 3 nm, which overcomes the flat band limitation of the photovoltage and increases the light absorptivity in the wavelength range from 300 to 420 nm. In addition, a 50‐fold increase in the conductivity yields a one‐order‐of‐magnitude increase in the diffusion length of an electron (Ln)(≈20 μm), allowing for unlimited electron collection in the 1.9 μm TiO2 nanowire array with the “crystal‐deficient” shell. The controllable “crystal‐deficient” overlayer in rutile TiO2 nanowires photoanode achieves a photocurrent density greater than 2.0 mA cm−2 at 1.23 V versus reversible hydrogen electrode (RHE), a 1.18% applied bias photon‐to‐current efficiency at 0.49 V versus RHE, a faradaic efficiency greater than 93.5% at 0.6 V versus Pt under air mass 1.5G simulated solar light illumination (100 mW cm−2).

A low-cost nanopatterned highly conductive poly(3,4-ethylenedioxythiophene) (PEDOT) thin film was fabricated on a flexible plastic substrate via a chemical polymerization method combined with a nanoimprinting technique and used as a platinum (Pt), TCO-free counter electrode for dye-sensitized solar cells (DSSCs). The catalytic properties of the nanopatterned PEDOT as the counter electrode in DSSCs were studied using cyclic voltammetry, J-V measurements, impedance spectroscopy, and finite-difference time-domain (FDTD) simulations. The nanopatterned PEDOT counter electrodes exhibit better functionality as a counter electrode for tri-iodide reduction when compared to non-patterned PEDOT-based counter electrodes. The Pt and TCO-free DSSCs with a nanopatterned PEDOT-based counter electrode exhibited a power conversion efficiency of 7.1% under one sunlight illumination (100 mW cm(-2)), which is comparable to that of conventional DSSCs with standard platinum Pt/FTO paired counter electrodes. The ability to modulate catalytic functionality with changes in nanoscale morphology represents a promising route for developing new counter electrodes of Pt and TCO-free DSSCs.

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