Organic molecular hole-transport materials (HTMs) are appealing for the scalable manufacture of perovskite solar cells (PSCs) because they are easier to reproducibly prepare in high purity than polymeric and inorganic HTMs. There is also a need to construct PSCs without dopants and additives to avoid formidable engineering and stability issues. We report here a power conversion efficiency (PCE) of 20.6% with a molecular HTM in an inverted (p-i-n) PSC without any dopants or interlayers. This new benchmark was made possible by the discovery that annealing a spiro-based dopant-free HTM (denoted DFH) containing redox-active triphenyl amine (TPA) units undergoes preferential molecular organization normal to the substrate. This structural order, governed by the strong intermolecular interactions of the DFH dioxane groups, affords high intrinsic hole mobility (1x10-3 cm2 V-1 s-1). Annealing films of DFH also enables the growth of large perovskite grains (up to 2 um) that minimize charge recombination in the PSC. DFH can also be isolated at a fraction of the cost of any other organic HTM.
In this research, the effect of Magnesium Fluoride (MgF2) Anti-Reflection (AR) layer was investigated in quantum dot sensitized solar cells (QDSCs). MgF2 nanoparticles with the dominant size of 20 nm were grown by a thermal evaporation method and a thin layer was formed on the front side of the fluorine-doped tin oxide (FTO) substrate. In order to study the effect of the AR layer on the efficiency of solar cells, this substrate was utilized in CdS QDSCs. In this conventional structure of QDSC, TiO2 nanocrystals (NCs) were applied on the FTO substrate, and then it was sensitized with CdS quantum dots (QDs). According to the results, the QDSCs with MgF2 AR layer represented the maximum Power Conversion Efficiency (PCE) of 3%. This efficiency was increased by about 47% compared to the reference cell without the AR layer. The reason is attributed to the presence of the AR layer and the reduction of incident light reflected from the surface of the solar cell.
Electrochemical CO2 reduction offers a method to use renewable electricity to convert CO2 into CO and other carbon-based chemical building blocks. While nearly all studies rely on a CO2 feed, we show herein that aqueous bicarbonate solutions can also be electrochemically converted into CO gas at meaningful rates in a flow cell. We achieved this result in a flow cell containing a bipolar membrane (BPM) and a silver nanoparticle catalyst on a porous carbon support. Electrolysis upon a N2-saturated 3.0-M potassium bicarbonate electrolyte solution yields CO with a faradaic efficiency (F.E.CO) of 81% at 25 mA cm-2 and 37% at 100 mA cm-2. This output is comparable to the analogous experiment where the electrolyte is saturated with gaseous CO2 (faradaic efficiency for CO is 78% at 25 mA cm-2 and 35% at 100 mA cm-2). The H+ flux from the BPM is critical to this chemistry in that it reacts with the bicarbonate feed to generate CO2, which is then reduced to CO at the gas diffusion electrode. These results are important in that they show that the addition of gaseous CO2 to bicarbonate electrolytes is not necessary in order to obtain reduced carbon products with a flow cell architecture. This process offers a means of using electrolysis to bypass the thermally-intensive step of extracting CO2 from bicarbonate solutions generated in carbon capture schemes.
Methylammonium lead iodide (MAPI) is the archetype of the intensively researched class of perovskites for photovoltaics. Nonetheless, even equilibrium aspects are far from being fully understood. Here we discuss equilibrium space charge effects at the MAPI/TiO2 and MAPI/Al2O3 interfaces, which are of paramount significance for solar cells. Different from the photovoltaic literature in which such built-in potentials are considered as being generated solely by electronic charge carriers, we will apply a generalized picture that considers the equilibrium distribution of both ionic and electronic carriers. We give experimental evidences that it is the ions that are responsible for the equilibrium space charge potential in MAPI, the reason being a pronounced ion adsorption at the contacts. The occurrence of equilibrium space charge effects generated by ionic redistribution has not been considered for photovoltaic materials and as such provides a novel path for modifying charge-selective interfaces in solar cells, as well as a better understanding of the behavior in mesoporous systems.
It is known that an engine with ideal efficiency ($eta =1$ for a chemical engine and $e = e_{rm Carnot}$ for a thermal one) has zero power because a reversible cycle takes an infinite time. However, at least from a theoretical point of view, it is possible to conceive (irreversible) engines with nonzero power that can reach ideal efficiency. Here this is achieved by replacing the usual linear transport law by a sublinear one and taking the step-function limit for the particle current (chemical engine) or heat current (thermal engine) versus the applied force. It is shown that in taking this limit exact thermodynamic inequalities relating the currents to the entropy production are not violated.
Here we use time-resolved and steady-state optical spectroscopy on state-of-the-art low- and high-bandgap perovskite films for tandems to quantify intrinsic recombination rates and absorption coefficients. We apply these data to calculate the limiting efficiency of perovskite-silicon and all-perovskite two-terminal tandems employing currently available bandgap materials as 42.0 % and 40.8 % respectively. By including luminescence coupling between sub-cells, i.e. the re-emission of photons from the high-bandgap sub-cell and their absorption in the low-bandgap sub-cell, we reveal the stringent need for current matching is relaxed when the high-bandgap sub-cell is a luminescent perovskite compared to calculations that do not consider luminescence coupling. We show luminescence coupling becomes important in all-perovskite tandems when charge carrier trapping rates are < 10$^{6}$ s$^{-1}$ (corresponding to carrier lifetimes longer than 1 ${mu}$s at low excitation densities) in the high-bandgap sub-cell, which is lowered to 10$^{5}$ s$^{-1}$ in the better-bandgap-matched perovskite-silicon cells. We demonstrate luminescence coupling endows greater flexibility in both sub-cell thicknesses, increased tolerance to different spectral conditions and a reduction in the total thickness of light absorbing layers. To maximally exploit luminescence coupling we reveal a key design rule for luminescent perovskite-based tandems: the high-bandgap sub-cell should always have the higher short-circuit current. Importantly, this can be achieved by reducing the bandgap or increasing the thickness in the high-bandgap sub-cell with minimal reduction in efficiency, thus allowing for wider, unstable bandgap compositions (>1.7 eV) to be avoided. Finally, we experimentally visualise luminescence coupling in an all-perovskite tandem device stack through cross-section luminescence images.
Yang Cao
,Yunlong Li
,Thomas Morrissey
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(2019)
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"Dopant-free molecular hole transport material that mediates a 20% power conversion efficiency in a perovskite solar cell"
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Curtis Berlinguette
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