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Regio-regular poly(3-hexylthiophene-2,5-diyl) (rr-P3HT), the work-horse oforganic photovoltaics, has been recently exploited in bulk heterojunction (BHJ)configuration with phenyl-C61-butyric acid methyl ester (PCBM) forsolution-processed hydrogen-evolving photocathodes, reaching cathodicphotocurrents at 0 V vs. RHE (J0V vs RHE) of up to 8 mA cm-2. Thephotoelectrochemical performance of these photocathodes strongly depends on thepresence of the electron (ESL) and hole (HSL) selective layer. While TiO2 andits sub-stoichiometric phases are consolidated ESL materials, the currentlyused HSLs (e.g., MoO3, CuI, PEDOTT:PSS, WO3) suffer electrochemical degradationunder hydrogen evolution reaction (HER)-working conditions. In this work, weuse solution-processed graphene derivatives as HSL to boost efficiency anddurability of rr-P3HT:PCBM-based photocathodes, demonstrating record-highperformance. In fact, our devices show cathodic J0V vs RHE of 6.01 mA cm-2,onset potential (Vo) of 0.6 V vs. RHE, ratiometric power-saved efficiency({\phi}saved) of 1.11% and operational activity of 20 hours in 0.5 M H2SO4solution. Moreover, the designed photocathodes are effectively working indifferent pH environments ranging from acid to basic. This is pivotal for theirexploitation in tandem configurations, where photoanodes operate only inrestricted electrochemical conditions. Furthermore, we demonstrate thescalability of our all-solution processed approach by fabricating a large-area(~9 cm2) photocathode on flexible substrate, achieving remarkable cathodic J0Vvs RHE of 2.8 mA cm-2, Vo of 0.45 V vs. RHE and {\phi}saved of 0.31%. This isthe first demonstration of high-efficient rr-P3HT:PCBM flexible photocathodesbased on low-cost and solution-processed manufacturing techniques.

Graphene-Based Hole Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes