Organic hole-transporting materials (HTM) have shown excellent ability in achieving high efficiency perovskite solar cells. However, their high cost significantly limits their applications in scaling-up perovskite solar cells. Here, we report an efficient, low-cost HTM, called TAT-^tBuSty, comprising a central triazatruxene moiety with 3 terminal tert-butoxy styrene groups and 3 hexyl side chains on the indole nitrogen. For the first time, we use an inexpensive liquid precursor to attach the donor ligand to the molecule. This enables purification of the HTM using a silica plug and recrystallization without the need for complicated column chromatography, which is typically required to purify solid-precursor-prepared HTMs. We estimate that the cost for the purified TAT-^tBuSty is $69.90 g⁻¹, which is 35% cheaper than the widely-used 2,2′7,7′-tetrakis-(N,N-di-p-methoxyphenyl-amine)-9,9′-spirobifluorene (spiro-OMeTAD; ca. $112.05 g⁻¹). Using this low-cost TAT-^tBuSty as the HTM in a caesium-formamidinium mixed-cation perovskite solar cell, we have successfully achieved a champion power conversion efficiency (PCE) of 20.3% (19.4% stabilized efficiency), which is comparable to the efficiency of devices using the reference spiro-OMeTAD HTM. Our work is crucial for up-scaling of next-generation high-performance metal-halide perovskite solar cells.

Nine halloysite nanotubes (HNTs) have been examined using scanning electron microscopy (SEM), atomic force microscopy (AFM) and (cross-sectional) transmission electron microscopy (TEM) to evaluate details of their external and internal morphologies. The samples span morphologies within the cylindrical to prismatic-polygonal framework proposed by Hillier et al. (2016). The ‘carpet roll’ model assumed in the conceptualization of most technological applications of HNTs is shown to be far too simplistic. Both cylindrical and prismatic forms have abundant edge steps traversing their surfaces that, by analogy with plates of kaolinite, correspond to prism faces. The mean value for the diameter of the central lumen of the tubes is 12 nm. Numerous slit-like nanopores, with diameters up to 18 nm, also occur between packets of layers, particularly in prismatic forms at the junction between a central cylindrical core and outer packets of planar layers. These pores expose aluminol and siloxane surfaces, but unlike the lumen, which is assumed only to expose an aluminol surface, they do not extend along the entire length of the nanotube. Edge steps seen most clearly by AFM correspond in height to the packets of layers seen in TEM. TEM cross-sections suggest that tube growth occurs by accretion of a spiralled thickening wedge of layers evolving from cylindrical to polygonal form and reveal that planar sectors may be joined by either abrupt angular junctions or by short sections of curved layers. A more realistic model of the internal and external morphologies of HNTs is proposed to assist with understanding of the behaviour of HNTs in technological applications.

We demonstrate improved performance and colour control of tri-bromide perovskite through co-sensitisation with organic dyes.

Most organic dyes synthesized for dye-sensitized solar cells (DSC) use a single linker group to bind to the metal oxide photo-anode. Here we describe the synthesis and testing of two new triphenylamine dyes containing either two carboxylic acids 5-[2-(4-diphenylamino-phenyl)-vinyl]-isophthalic acid (10) or two cyanoacrylic acids (2Z, 2′Z)-3, 3′-(5-((E)-4-(diphenylamino) styryl)-1, 3-phenylene) bis (2-cyanoacrylic acid) (8) as linker groups. Full characterization data are reported for these dyes and their synthetic intermediates. DSC devices have been prepared from these new dyes either by passive or fast dyeing and the dyes have also been tested in co-sensitized DSC devices leading to a PCE (η = 5.4%) for the double cyanoacrylate linker dye (8) co-sensitized with D149. The dye:TiO₂ surface interactions and dye excitations are interpreted using three modelling methods: density functional theory (at 0 K); molecular dynamics (at 298 K); time dependent density functional theory. The modelling results show the preferred orientation of both dyes on an anatase (1 0 1) TiO₂ surface to be horizontal, and both the simulated and experimental absorption spectra of the dye molecules indicate a red shifted band for (8) compared to (10). This is in line with broader light harvesting and J_sc for (8) compared to (10).