Organic–inorganic hybrid perovskite solar cells with mixed cations and mixed halides have achieved impressive power conversion efficiency of up to 22.1%. Phase segregation due to the mixed compositions has attracted wide concerns, and their nature and origin are still unclear. Some very useful analytical techniques are controversial in microstructural and chemical analyses due to electron beam‐induced damage to the “soft” hybrid perovskite materials. In this study photoluminescence, cathodoluminescence, and transmission electron microscopy are used to study charge carrier recombination and retrieve crystallographic and compositional information for all‐inorganic CsPbIBr2 films on the nanoscale. It is found that under light and electron beam illumination, “iodide‐rich” CsPbI(1+x)Br(2−x) phases form at grain boundaries as well as segregate as clusters inside the film. Phase segregation generates a high density of mobile ions moving along grain boundaries as ion migration “highways.” Finally, these mobile ions can pile up at the perovskite/TiO2 interface resulting in formation of larger injection barriers, hampering electron extraction and leading to strong current density–voltage hysteresis in the polycrystalline perovskite solar cells. This explains why the planar CsPbIBr2 solar cells exhibit significant hysteresis in efficiency measurements, showing an efficiency of up to 8.02% in the reverse scan and a reduced efficiency of 4.02% in the forward scan, and giving a stabilized efficiency of 6.07%.
Aging in super glassy polymers such as poly(trimethylsilylpropyne) (PTMSP), poly(4‐methyl‐2‐pentyne) (PMP), and polymers with intrinsic microporosity (PIM‐1) reduces gas permeabilities and limits their application as gas‐separation membranes. While super glassy polymers are initially very porous, and ultra‐permeable, they quickly pack into a denser phase becoming less porous and permeable. This age‐old problem has been solved by adding an ultraporous additive that maintains the low density, porous, initial stage of super glassy polymers through absorbing a portion of the polymer chains within its pores thereby holding the chains in their open position. This result is the first time that aging in super glassy polymers is inhibited whilst maintaining enhanced CO2 permeability for one year and improving CO2/N2 selectivity. This approach could allow super glassy polymers to be revisited for commercial application in gas separations.
Porosity loss, also known as physical aging, in glassy polymers hampers their long term use in gas separations. Unprecedented interactions of porous aromatic frameworks (PAFs) with these polymers offer the potential to control and exploit physical aging for drastically enhanced separation efficiency. PAF-1 is used in the archetypal polymer of intrinsic microporosity (PIM), PIM-1, to achieve three significant outcomes. 1) hydrogen permeability is drastically enhanced by 375% to 5500 Barrer. 2) Physical aging is controlled causing the selectivity for H2 over N2 to increase from 4.5 to 13 over 400 days of aging. 3) The improvement with age of the membrane is exploited to recover up to 98% of H2 from gas mixtures with N2 . This process is critical for the use of ammonia as a H2 storage medium. The tethering of polymer side chains within PAF-1 pores is responsible for maintaining H2 transport pathways, whilst the larger N2 pathways gradually collapse.
The design, synthesis, and characterization of a hierarchically ordered composite whose structure and optical properties can be reversibly switched by adjustment of solvent conditions are described. Solvent‐induced swelling and de‐swelling is shown to provide control over the internal packing arrangement and hence, optical properties of in situ synthesized metal nanoparticles. Specifically, a gold‐nanoparticle‐containing ionic‐liquid‐derived polymer is synthesized in a single step by UV irradiation of a metal‐ion‐precursor‐doped, self‐assembled ionic liquid gel, 1‐decyl‐3‐vinylimidazolium chloride. Small‐angle X‐ray scattering (SAXS) studies indicate that in the de‐swollen state, the freestanding polymer adopts a perforated lamellar structure. Optical spectroscopy of the dried composite reveals plasmon resonances positioned in the near‐IR. Strong particle–particle interactions arise from matrix‐promoted formation of aggregated 1D clusters or chains of gold nanoparticles. Upon swelling in alcohol, the composite undergoes a structural conversion to a disordered structure, which is accompanied by a color change from purple to pale pink and a shift in the surface plasmon resonance to 527 nm, consistent with isolated, non‐interacting particles. These results demonstrate the far‐field tuning of the plasmonic spectrum of gold nanoparticles by solvent‐mediated changes in its encapsulating matrix, offering a straightforward, low‐cost strategy for the fabrication of nanophotonic materials.
Promising efficiencies and a high open-circuit voltage are demonstrated for a novel low band-gap all-polymer photovoltaic blend.
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