5 years ago

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

Graphene-Based Hole-Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes
Antonio E. Del Rio Castillo, L. Najafi, M. Prato, A. Ansaldo, S. Bellani, F. Bonaccorso, I. Moreels, B. Martín-García
Regioregular poly(3-hexylthiophene-2,5-diyl) (rr-P3HT), the workhorse of organic photovoltaics, has been recently exploited in bulk heterojunction (BHJ) configuration with phenyl-C61-butyric acid methyl ester (PCBM) for solution-processed hydrogen-evolving photocathodes, reaching cathodic photocurrents at 0 V vs RHE (J0 V vs RHE) of up to 8 mA cm–2. The photoelectrochemical performance of these photocathodes strongly depends on the presence of the electron- (ESL) and hole- (HSL) selective layers. While TiO2 and its substoichiometric phases are consolidated ESL materials, the currently used HSLs (e.g., MoO3, CuI, PEDOTT:PSS, WO3) suffer electrochemical degradation under hydrogen evolution reaction (HER) working conditions. In this work, we use solution-processed graphene derivatives as HSL to boost the efficiency and durability of rr-P3HT:PCBM-based photocathodes, demonstrating record-high performance. In fact, our devices show cathodic J0 V vs RHE of 6.01 mA cm–2, onset potential (Vo) of 0.6 V vs RHE, ratiometric power-saved efficiency (φsaved) of 1.11%, and operational activity of 20 h in 0.5 M H2SO4 solution. Moreover, the designed photocathodes are effectively working in different pH environments ranging from acidic to basic. This is pivotal for their exploitation in tandem configurations, where photoanodes operate only in restricted electrochemical conditions. Furthermore, we demonstrate the scalability of our all-solution-processed approach by fabricating a large-area (∼9 cm2) photocathode on flexible substrate, achieving a remarkable cathodic J0 V vs RHE of 2.8 mA cm–2, Vo of 0.45 V vs RHE, and φsaved of 0.31%. This is the first demonstration of highly efficient rr-P3HT:PCBM flexible photocathodes based on low-cost and solution-processed manufacturing techniques.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b05904

DOI: 10.1021/acs.jpcc.7b05904

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