Scaling-Up of Thin-Film Photoelectrodes for Solar Water Splitting Based on Atomic Layer Deposition.

Atomic layer deposition (ALD) is an established method to prepare protective layers for Si-based photoelectrodes for photoelectrochemical (PEC) water splitting. Although ALD has been widely used in microelectronics and photovoltaics, it remains a great challenge to design simple and effective ALD systems to deposit large and uniform protective films for Si-based photoelectrodes with industrial sizes. This paper describes the design and realization of a simple ALD chamber configuration for photoelectrodes with large sizes, in which the influence of a gas redistributor over the gas flow and heat transfer during film growth was revealed by computational fluid dynamics simulations and experimental investigations. A simple circular baffle-type redistributor was proposed to establish a uniform gas flow field throughout the ALD reactor, resulting in a uniform temperature profile. With this simple baffle redistributor, the large-area Al 2 O 3 monitor film (46 nm thickness) reached a good nonuniformity (Nu %) of 0.88% over a large area of 256 cm 2 . This design enables the fabrication of large-scale photocathodes from standard industrial-grade 166 mm Si(100) wafers (276 cm 2 ) by depositing 50 nm TiO 2 protective films with Nu % less than 5%. The obtained photocathode achieves a saturation current of 6.45 A with a hydrogen production rate of 43.2 mL/min under outdoor illumination. This work elucidates how flow pattern and heat transfer may influence the deposition of protective layers over large photoelectrodes, providing guidance for future industrial applications of PEC water splitting.