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Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.
Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.
Full water splitting into hydrogen and oxygen on semiconductor nanocrystals is a challenging task; overpotentials must be overcome for both half-reactions and different catalytic sites are needed to facilitate them. Additionally, efficient charge separation and prevention of back reactions are necessary. Here, we report simultaneous H-2 and O-2 evolution by CdS nanorods decorated with nanoparticulate reduction and molecular oxidation co-catalysts. The process proceeds entirely without sacrificial agents and relies on the nanorod morphology of CdS to spatially separate the reduction and oxidation sites. Hydrogen is generated on Pt nanoparticles grown at the nanorod tips, while Ru(tpy)(bpy)Cl-2-based oxidation catalysts are anchored through dithiocarbamate bonds onto the sides of the nanorod. O-2 generation from water was verified by O-18 isotope labelling experiments, and time-resolved spectroscopic results confirmed efficient charge separation and ultrafast electron and hole transfer to the reaction sites. The system demonstrates that combining nanoparticulate and molecular catalysts on anisotropic nanocrystals provides an effective pathway for visible-light-driven photocatalytic water splitting.
Perovskite solar cells (PSCs) are currently one of the most promising photovoltaic technologies for highly efficient and cost-effective solar energy production. In only a few years, an unprecedented progression of preparation procedures and material compositions delivered lab-scale devices that have now reached record power conversion efficiencies (PCEs) higher than 20%, competing with most established solar cell materials such as silicon, CIGS, and CdTe. However, despite a large number of researchers currently involved in this topic, only a few groups in the world can reproduce >20% efficiencies on a regular n-i-p architecture. In this work, we present detailed protocols for preparing PSCs in regular (n-i-p) and inverted (p-i-n) architectures with >= 20% PCE. We aim to provide a comprehensive, reproducible description of our device fabrication , protocols. We encourage the practice of reporting detailed and transparent protocols that can be more easily reproduced by other laboratories. A better reporting standard may, in turn, accelerate the development of perovskite solar cells and related research fields.
Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
The El Nino-Southern Oscillation (ENSO) is the main driver of the interannual variability in eastern African rainfall, with a significant impact on vegetation and agriculture and dire consequences for food and social security. In this study, we identify and quantify the ENSO contribution to the eastern African rainfall variability to forecast future eastern African vegetation response to rainfall variability related to a predicted intensified ENSO. To differentiate the vegetation variability due to ENSO, we removed the ENSO signal from the climate data using empirical orthogonal teleconnection (EOT) analysis. Then, we simulated the ecosystem carbon and water fluxes under the historical climate without components related to ENSO teleconnections. We found ENSO-driven patterns in vegetation response and confirmed that EOT analysis can successfully produce coupled tropical Pacific sea surface temperature-eastern African rainfall teleconnection from observed datasets. We further simulated eastern African vegetation response under future climate change as it is projected by climate models and under future climate change combined with a predicted increased ENSO intensity. Our EOT analysis highlights that climate simulations are still not good at capturing rainfall variability due to ENSO, and as we show here the future vegetation would be different from what is simulated under these climate model outputs lacking accurate ENSO contribution. We simulated considerable differences in eastern African vegetation growth under the influence of an intensified ENSO regime which will bring further environmental stress to a region with a reduced capacity to adapt effects of global climate change and food security.
From November 2006 to January 2010, a sediment trap that was cleared monthly was deployed in Lake Challa, a deep stratified freshwater lake on the eastern slope of Mt. Kilimanjaro in southern Kenya. Geochemical data from sediment trap samples were compared with a broad range of limnological and meteorological parameters to characterize the effect of single parameters on productivity and sedimentation processes in the crater basin. During the southern hemisphere summer (November-March), when the water temperature is high and the lake is biologically productive (nondiatom algae), calcite predominated in the sediment trap samples. During the "long rain" season (March-May) a small amount of organic matter and lithogenic material caused by rainfall appeared. This was followed by the cool and windy months of the southern hemisphere winter (June-October) when diatoms were the main component, indicating a diatom bloom initiated by improvement of nutrient availability related to upwelling processes. The sediment trap data support the hypothesis that the light-dark lamination couplets, which are abundant in Lake Challa cores, reflect seasonal delivery to the sediments of diatom-rich particulates during the windy months and diatom-poor material during the wet season. However, interannual and spatial variability in upwelling and productivity patterns, as well as El Nino-Southern Oscillation (ENSO)-related rainfall and drought cycles, exert a strong influence on the magnitude and geochemical composition of particle export to the hypolimnion of Lake Challa.
Interannual rainfall variations in equatorial East Africa are tightly linked to the El Nino Southern Oscillation (ENSO), with more rain and flooding during El Nino and droughts in La Nina years, both having severe impacts on human habitation and food security. Here we report evidence from an annually laminated lake sediment record from southeastern Kenya for interannual to centennial-scale changes in ENSO-related rainfall variability during the last three millennia and for reductions in both the mean rate and the variability of rainfall in East Africa during the Last Glacial period. Climate model simulations support forward extrapolation from these lake sediment data that future warming will intensify the interannual variability of East Africa's rainfall.
The strength of the North Atlantic Oscillation (NAO) is considered to be the main driver of climate changes over the European and western Asian continents throughout the last millennium. For example, the predominantly warm Medieval Climate Anomaly (MCA) and the following cold period of the Little Ice Age (LIA) over Europe have been associated with long-lasting phases with a positive and negative NAO index. Its climatic imprint is especially pronounced in European winter seasons. However, little is known about the influence of NAO with respect to its eastern extent over the Eurasian continent. Here we present speleothem records (PC, 8180 and Sr/Ca) from the southern rim of Fergana Basin (Central Asia) revealing annually resolved past climate variations during the last millennium. The age control of the stalagmite relies on radiocarbon dating as large amounts of detrital material inhibit accurate 230Th dating. Present-day calcification of the stalagmite is most effective during spring when the cave atmosphere and elevated water supply by snow melting and high amount of spring precipitation provide optimal conditions. Seasonal precipitation variations cause changes of the stable isotope and Sr/ Ca compositions. The simultaneous changes in these geochemical proxies, however, give also evidence for fractionation processes in the cave. By disentangling both processes, we demonstrate that the amount of winter precipitation during the MCA was generally higher than during the LIA, which is in line with climatic changes linked to the NAO index but opposite to the higher mountain records of Central Asia. Several events of strongly reduced winter precipitation are observed during the LIA in Central Asia. These dry winter events can be related to phases of a strong negative NAO index and all results reveal that winter precipitation over the central Eurasian continent is tightly linked to atmospheric NAO modes by the westerly wind systems. (C) 2017 Elsevier Ltd. All rights reserved.