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Summary In small-area perovskite solar cells, efficiencies of >25% have been achieved using an antisolvent dripping technique; however, it is not applicable for coatings on an industrial scale. Currently, large-area devices based on scalable perovskite coatings still show a very large gap with small-area devices. This means that a uniform perovskite coating and defect control on large-area devices are not as secure as they are on small devices. Here, we report the deposition of dense and uniform perovskite films using an air-knife-assisted bar-coating employing a perovskite [(FAPbI3)0.95(MAPbBr3)0.05] precursor solution dissolved in 2-methoxyethanol. A pinhole-free and homogeneous surface morphology was achieved by adding n-cyclohexyl-2-pyrrolidone to ensure a balance between rapid nucleation and slowed crystal growth in the precursor solution. By applying surface passivation with acetylcholine bromide and laser etching to thin layers, mini-modules with an aperture area of 31 cm2 were fabricated, attaining an efficiency of >20% (17.53% in the efficiency certified by a quasi-steady-state protocol).

To boost the photoelectrochemical water oxidation performance of hematite photoanodes, high temperature annealing has been widely applied to enhance crystallinity, to improve the interface between the hematite-substrate interface, and to introduce tin-dopants from the substrate. However, when using additional dopants, the interaction between the unintentional tin and intentional dopant is poorly understood. Here, using germanium, we investigate how tin diffusion affects overall photoelectrochemical performance in germanium:tin co-doped systems. After revealing that germanium is a better dopant than tin, we develop a facile germanium-doping method which suppresses tin diffusion from the fluorine doped tin oxide substrate, significantly improving hematite performance. The NiFeOx@Ge-PH photoanode shows a photocurrent density of 4.6 mA cm−2 at 1.23 VRHE with a low turn-on voltage. After combining with a perovskite solar cell, our tandem system achieves 4.8% solar-to-hydrogen conversion efficiency (3.9 mA cm−2 in NiFeOx@Ge-PH/perovskite solar water splitting system). Our work provides important insights on a promising diagnostic tool for future co-doping system design., Germanium (Ge) has potential as a dopant suitable for the hematite-based photoelectrochemical water splitting system. Here, the authors report the fabrication of Ge doped porous hematite and demonstrate an efficient tandem system of Ge doped porous hematite and the perovskite solar cell.

To boost the photoelectrochemical water oxidation performance of a hematite photoanode, high temperature annealing has been widely applied to enhance crystallinity and remove the physical interface between the hematite and the fluorine doped thin oxide (FTO) substrate. However, the high temperature also results in unintentional Sn-doping due to thermal diffusion from the bottom FTO substrate. Therefore, when using additional dopants and the subsequent high temperature annealing process to enhance performance, the procedure should more precisely be considered co-doping of the hematite photoanode. However, at present, the interaction between the unintentional Sn and intentional dopant is poorly understood. Here, using germanium (Ge), which has been proven a promising dopant in previously reported simulations, we investigated how Sn diffusion affects overall PEC performance in Sn:Ge co-doped systems. After revealing the negative interaction of Sn and Ge dopants, we developed a facile Ge-doping method which suppresses Sn diffusion from the FTO substrate, significantly improving hematite performance. The Sn:Ge-hematite photoanode showed a photocurrent density of 4.6 mA cm− 2 at 1.23 VRHE with an excellent low turn-on voltage. After combining with a perovskite solar cell, our tandem system achieved outstanding 4.8% solar-to-hydrogen conversion efficiency (3.9 mA cm− 2 in an unassisted water splitting system). Our work provides important insights on a promising diagnostic tool for future co-doping system design.