Efficient photosynthesis of carbon monoxide from CO2 using perovskite photovoltaics

Artificial photosynthesis, mimicking nature in its efforts to store solar energy, has received considerable attention from the research community. Most of these attempts target the production of H2 as a fuel and our group recently demonstrated solar-to-hydrogen conversion at 12.3% efficiency. Here, in an effort to take this approach closer to real photosynthesis, which is based on the conversion of CO2, we demonstrate the efficient reduction of CO2 to carbon monoxide driven solely by simulated sunlight using water as the electron source. Employing series-connected perovskite photovoltaics and high-performance catalyst electrodes, we reach a solar-to-CO efficiency exceeding 6.5%, which represents a new benchmark in sunlight-driven CO2 conversion. Considering hydrogen as a secondary product, an efficiency exceeding 7% is observed. Furthermore, this study represents one of the first demonstrations of extended, stable operation of perovskite photovoltaics, whose large open-circuit voltage is shown to be particularly suited for this process

New Strategies for Defect Passivation in High-Efficiency Perovskite Solar Cells

Lead halide perovskite solar cells now show excellent efficiencies and encouraging levels of stability. Further improvements in performance require better control of the trap states which are considered to be associated with vacancies and defects at crystallite surfaces. Herein, a reflection on the ways in which these traps can be mitigated is presented by improving the quality of the perovskite layer and interfaces in fully assembled device configurations. In this review, the most recent design strategies reported in the literature, which have been explored to tune grain orientation, to passivate defects, and to improve charge-carrier lifetimes, are presented. Specifically, the advances made with single-cation, mixed-cation and/or mixed-halide, and 3D/2D bilayer-based light absorbers are discussed. The interfacial, compositional, and band alignment engineering along with their consequent effects on the open-circuit voltage, power conversion efficiency, and stability are a particular focus

Highly efficient planar perovskite solar cells through band alignment engineering

The simplification of perovskite solar cells (PSCs), by replacing the mesoporous electron selective layer (ESL) with a planar one, is advantageous for large-scale manufacturing. PSCs with a planar TiO2 ESL have been demonstrated, but these exhibit unstabilized power conversion efficiencies (PCEs). Herein we show that planar PSCs using TiO2 are inherently limited due to conduction band misalignment and demonstrate, with a variety of characterization techniques, for the first time that SnO2 achieves a barrier-free energetic configuration, obtaining almost hysteresis-free PCEs of over 18% with record high voltages of up to 1.19 V

A perspective on using experiment and theory to identify design principles in dye-sensitized solar cells

Dye-sensitized solar cells (DSCs) have been the subject of wide-ranging studies for many years because of their potential for large-scale manufacturing using roll-to-roll processing allied to their use of earth abundant raw materials. Two main challenges exist for DSC devices to achieve this goal; uplifting device efficiency from the 12 to 14% currently achieved for laboratory-scale ‘hero’ cells and replacement of the widely-used liquid electrolytes which can limit device lifetimes. To increase device efficiency requires optimized dye injection and regeneration, most likely from multiple dyes while replacement of liquid electrolytes requires solid charge transporters (most likely hole transport materials – HTMs). While theoretical and experimental work have both been widely applied to different aspects of DSC research, these approaches are most effective when working in tandem. In this context, this perspective paper considers the key parameters which influence electron transfer processes in DSC devices using one or more dye molecules and how modelling and experimental approaches can work together to optimize electron injection and dye regeneration. This paper provides a perspective that theory and experiment are best used in tandem to study DSC device

Self-assembled photosystem-I biophotovoltaics on nanostructured TiO2 and ZnO

The abundant pigment-protein membrane complex photosystem-I (PS-I) is at the heart of the Earth’s energy cycle. It is the central molecule in the “Z-scheme” of photosynthesis, converting sunlight into the chemical energy of life. Commandeering this intricately organized photosynthetic nanocircuitry and re-wiring it to produce electricity carries the promise of inexpensive and environmentally friendly solar power. We here report that dry PS-I stabilized by surfactant peptides functioned as both the light-harvester and charge separator in solar cells self-assembled on nanostructured semiconductors. Contrary to previous attempts at biophotovoltaics requiring elaborate surface chemistries, thin film deposition, and illumination concentrated into narrow wavelength ranges the devices described here are straightforward and inexpensive to fabricate and perform well under standard sunlight yielding open circuit photovoltage of 0.5 V, fill factor of 71%, electrical power density of 81 µW/cm2 and photocurrent density of 362 µA/cm2, over four orders of magnitude higher than any photosystem-based biophotovoltaic to date