Perovskite solar cells are amongst the most exciting photovoltaic systems as they combine low recombination losses, ease of fabrication and high spectral tunability. The Achilles heel of this technology is the device stability due to the ionic nature of the perovskite crystal, rendering it highly hygroscopic, and the extensive diffusion of ions especially at elevated temperatures. Herein, we demonstrate the application of a simple solution-processed perfluorinated self-assembled monolayer (p-SAM) that not only passivates the perovskite surface but also drastically improves the stability of the perovskite absorber and in turn the solar cell under elevated temperature or humid conditions. p-i-ntype perovskite devices employing these SAMs exhibited power conversion efficiencies surpassing 21%. Notably, the best performing devices are stable under standardized maximum-power point (MPP) operation at 85°C in inert atmosphere (ISOS-L-2) for more than 250 h, and exhibit superior humidity resilience, maintaining ~95% device performance even if stored in humid air in the ambient over months (~3000h, ISOS-D-1). Our work, therefore, demonstrates a novel strategy towards efficient and stable perovskite solar cells with easily deposited functional interlayers. Supporting Information.Experimental Methods, Supplementary Notes and Calculations, Details on Simulation, XRD, UV-Vis, XPS, FTIR, KP data, PL vs time, SPV measurements as well as additional experimental methods.
Meeting the current needs for easier, more precise and faster analyses that also follow the principles of green analytical chemistry requires novel analytical chemistry strategies. Since the appearance in this century of the first device based on a paper platform, many studies have been presented in the literature, providing a wide range of designs and possibilities for the application of paper platforms to electroanalytical systems. This Review gives an overview of the field and can pave the way for the future development of electrochemical paper‐based analytical devices. We also present a critical point of view regarding what has been investigated and developed and what is still missing. This Review discusses the efforts made in the field related to important topics such as the choice of the paper substrate, the device construction process, the characterization of the device, and applications in different areas. In this way, we indicate some steps necessary for optimizing the design of the devices, with a focus on multidisciplinary collaborations that could move entire systems from the bench of the laboratory to the field.
In this work, a new hypothesis for the electrocatalytic behavior of CuO electrodes is presented. Different from the established mechanism, here we discuss why Cu species do not participate in the oxidation mechanism of carbohydrates. We show that hydroxyl ion adsorption and the semiconductive properties of the material play a more significant role in this process. The relationship between the flat band potential and the potential that begin oxidation suggests that the concentration of vacancies in the charge region acts upon the reactivity of the adsorbed hydroxyl ions through a partial charge transfer reaction. In the presence of carbohydrate molecules, the electron transfer is facilitated and involves the transfer of electrons from the adsorbed hydroxyl ions to the CuO film. This mechanism is fundamentally relevant since it helps the understanding of several experimental misleads. The results can also lead to obtaining better catalysts, since improvements in the material should focus on enhancing the semiconductive properties rather than the Cu/Cu redox transition. The results shed light on different aspects of carbohydrate molecules oxidation that could lead to novel applications and possibly a better description of other semiconductor mechanisms in electrocatalysis.
We report for the first time on the self-assembly of nanostructures composed exclusively of alternating positively charged and hydrophobic amino acids. A novel arginine/phenylalanine octapeptide, RF8, was synthesized. Because the low hydrophobicity of this sequence makes its spontaneous ordering through solution-based methods difficult, a recently proposed solid-vapor approach was used to obtain nanometric architectures on ITO/PET substrates. The formation of the nanostructures was investigated under different preparation conditions, specifically, under different gas-phase solvents (aniline, water, and dichloromethane), different peptide concentrations in the precursor solution, and different incubation times. The stability of the assemblies was experimentally studied by electron microscopy and thermogravimetric analysis coupled with mass spectrometry. The secondary structure was assessed by infrared and Raman spectroscopy, and the arrays were found to assume an antiparallel β-sheet conformation. FEG-SEM images clearly reveal the appearance of fibrillar structures that form extensive homogeneously distributed networks. A close relationship between the morphology and preparation parameters was found, and a concentration-triggered mechanism was suggested. Molecular dynamics simulations were performed to address the thermal stability and nature of intermolecular interactions of the putative assembly structure. Results obtained when water is considered as solvent shows that a stable lamellar structure is formed containing a thin layer of water in between the RF8 peptides that is stabilized by H-bonding.
Plasmon-driven photocatalysis is an emerging and promising application of noble metal nanoparticles (NPs). An understanding of the fundamental aspects of plasmon interaction with molecules and factors controlling their reaction rate in a heterogeneous system is of high importance. Therefore, the dehalogenation kinetics of 8-bromoguanine (BrGua) and 8-bromoadenine (BrAde) on aggregated surfaces of silver (Ag) and gold (Au) NPs have been studied to understand the reaction kinetics and the underlying reaction mechanism prevalent in heterogeneous reaction systems induced by plasmons monitored by surface enhanced Raman scattering (SERS). We conclude that the time-average constant concentration of hot electrons and the time scale of dissociation of transient negative ions (TNI) are crucial in defining the reaction rate law based on a proposed kinetic model. An overall higher reaction rate of dehalogenation is observed on Ag compared with Au, which is explained by the favorable hot-hole scavenging by the reaction product and the byproduct. We therefore arrive at the conclusion that insufficient hole deactivation could retard the reaction rate significantly, marking itself as rate-determining step for the overall reaction. The wavelength dependency of the reaction rate normalized to absorbed optical power indicates the nonthermal nature of the plasmon-driven reaction. The study therefore lays a general approach toward understanding the kinetics and reaction mechanism of a plasmon-driven reaction in a heterogeneous system, and furthermore, it leads to a better understanding of the reactivity of brominated purine derivatives on Ag and Au, which could in the future be exploited, for example, in plasmon-assisted cancer therapy.
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