Abstract
AbstractStrong interest exists in the development of organic–inorganic lead halide perovskite photovoltaics and of photoelectrochemical (PEC) tandem absorber systems for solar fuel production. However, their scalability and durability have long been limiting factors. In this work, it is revealed how both fields can be seamlessly merged together, to obtain scalable, bias‐free solar water splitting tandem devices. For this purpose, state‐of‐the‐art cesium formamidinium methylammonium (CsFAMA) triple cation mixed halide perovskite photovoltaic cells with a nickel oxide (NiOx) hole transport layer are employed to produce Field's metal‐epoxy encapsulated photocathodes. Their stability (up to 7 h), photocurrent density (–12.1 ± 0.3 mA cm−2 at 0 V versus reversible hydrogen electrode, RHE), and reproducibility enable a matching combination with robust BiVO4 photoanodes, resulting in 0.25 cm2 PEC tandems with an excellent stability of up to 20 h and a bias‐free solar‐to‐hydrogen efficiency of 0.35 ± 0.14%. The high reliability of the fabrication procedures allows scaling of the devices up to 10 cm2, with a slight decrease in bias‐free photocurrent density from 0.39 ± 0.15 to 0.23 ± 0.10 mA cm−2 due to an increasing series resistance. To characterize these devices, a versatile 3D‐printed PEC cell is also developed.
Highlights
To harness sunlight into chemical energy, several routes have been developed spanning from connecting photovoltaic modules to separate electrolysers, [10] to developing solution immersed photoelectrochemical (PEC) systems. [11,12,13] Since the energy conversion efficiency of a single photoabsorber is theoretically limited [14], tandem systems of two complementary absorbers are preferably employed for PV, PEC and hybrid PV-PEC applications. [12,15,16,17,18] Such photoelectrode tandem systems are interesting for the field of solar fuels, where one of the main aims is driving electrochemical processes without applying an additional electrochemical bias
To address some of those issues, in this work we investigate the scalability of tandem photoelectrochemical (PEC) devices for water splitting, combining a cesium formamidinium methylammonium (CsFAMA) triple cation perovskite-driven photocathode with a bismuth vanadate photoanode
By employing the CsFAMA triple cation mixed halide perovskite as the photoabsorber and nickel oxide (NiOx) as the hole selective layer, substantial improvements have been achieved in the performance (–12.1±0.3 mA cm−2 at 0 V vs. reversible hydrogen electrode (RHE)) and stability of 0.25 cm2 photocathodes, with the corresponding PV devices reaching an efficiency of 13.0±1.2%
Summary
As society’s energy demands increase, the production and storage of sustainable energy becomes a critical issue. [1,2,3,4] While photovoltaic (PV) modules may cover this demand on their own, large scale applications still require alternatives to batteries and supercapacitors for a more effective energy storage and transport. [1,2,5,6,7,8,9] From this perspective, solar fuels (e.g. H2, CO) represent a promising option, due to their high specific energy density, which makes them favourable for transport or conversion to more conventional liquid fuels. [61,62] to prevent degradation of the perovskite layer, the photovoltaic component was again physically separated from the solution, with a conductive wire ensuring the connection to the electrocatalyst Such devices mainly combined a perovskite cell with a high band gap oxide layer (i.e. BiVO4, [61,63,64,65,66] WO3, [67] TiO2, [68] or hematite [62,69,70]) to drive water splitting, [63] or CO2 reduction. With an onset potential of 0.95±0.03 V vs RHE, this initial system represented a promising example of a perovskite-based photocathode, on the basis of which wireless tandems for solar fuel production could be developed While most of these initial results employed the moisture, air and temperature sensitive methylammonium lead triiodide (MAPbI3) perovskite, [51,76] more recent photovoltaic reports have shown that improvements in both efficiency and stability can be obtained when using complex precursor solutions. In order to evaluate devices of various sizes, we propose a straightforward design for a modular 3D-printed PEC cell, which can be assembled or adapted for large scale studies
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