Synthesis of modified fullerenes for oxygen reduction reactions

In the search for carbon based catalysts for Oxygen Reduction Reactions (ORR), two different classes of fullerene hybrids and metal free fullerene derivatives have been prepared by highly selective metal- and organo-catalyzed synthetic methods. They were included as both electron acceptors and catalysts in polymer-based photo-electrochemical cell,fully demonstrating electrocatalytic activity. Remarkably, the activity of the metal free fullerenes proved to be as high as that observed for metallofullerenes based on noble metals, and up to ten-fold higher than by using PCBM

Polymer-based photocathodes with a solution-processable cuprous iodide anode layer and a polyethyleneimine protective coating

Organic semiconductors are proven to efficiently drive photoelectrochemical water splitting

All Solution-Processed, Hybrid Organic-Inorganic Photocathode for Hydrogen Evolution

Nowadays, the efficient, stable, and scalable conversion of solar energy into chemical fuels represents a great scientific, economic, and ethical challenge. Amongst the available candidate technologies, photoelectrochemical water splitting potentially has the most promising technoeconomic trade-off between cost and efficiency. However, research on semiconductors and photoelectrode architectures suitable for H-2 evolution has focused mainly on the use of fabrication techniques and inorganic materials that are not easily scalable. Here, we report for the first time an all solution-processed approach for the fabrication of hybrid organic/inorganic photocathodes based on organic semiconductor bulk heterojunctions that exhibit promising photoelectrochemical performance. The sequential deposition of inorganic material, charge-selective contacts, visible-light sensitive organic polymers, and earth-abundant, nonprecious catalyst by spin coating leads to state-of-the-art photoelectrochemical parameters, comprising a high onset potential [+ 0.602 V vs reversible hydrogen electrode (RHE)] and a positive maximum power point (+0.222 V vs RHE), a photocurrent density as high as 5.25 mA/cm(2) at 0 V versus RHE, an incident photon-to-current conversion efficiency at 0 V versus RHE of above 35%, and 100% faradaic efficiency for hydrogen production. The demonstrated all solution-processed hybrid photoelectrodes represent an eligible candidate for the scalable and low-cost solar-to-H-2 conversion technology that embodies the feasibility requirements for large area, plant-scale applications

Hybrid organic-inorganic H-2-evolving photocathodes: understanding the route towards high performance organic photoelectrochemical water splitting

A promising, yet challenging, route towards renewable production of hydrogen is the direct conversion of solar energy at a simple and low cost semiconductor/water junction. Despite the theoretical simplicity of such a photoelectrochemical device, different limitations among candidate semiconductor materials have hindered its development. After many decades of research on inorganic semiconductors, a conclusive solution still appears out of reach. Here, we report an efficient hybrid organic-inorganic H-2 evolving photocathode, consisting of a donor/acceptor blend sandwiched between charge-selective layers and a thin electrocatalyst layer. The role and stability of the different interfaces are investigated, and the conductive polymer is proven to be an efficient material for a semiconductor/liquid PEC junction. The best performing electrodes show high performances with a photocurrent of 3 mA cm(-2) at 0 V vs. RHE, optimal process stability with 100% faradaic efficiency during electrode's lifetime, excellent energetics with +0.67 V vs. RHE onset potential, promising operational activity of several hours and by-design compatibility for implementation in a tandem architecture. This work demonstrates organic semiconductors as a radically new option for efficient direct conversion of solar energy into fuels, and points out the route towards high performance organic photoelectrochemical water splitting