Abstract Hole transport layer‐free, carbon‐based, all‐inorganic CsPbI 3 perovskite solar cells (PSCs) have exhibited great potential in photovoltaic applications owing to their low cost and excellent thermal stability. However, the low power conversion efficiency (PCE) hampers its development, mainly due to the existence of defects inside the CsPbI 3 film or at TiO 2 electron transport layer/CsPbI 3 interface. Herein, these issues were addressed through a facile TiO 2 post‐treatment strategy using 1‐butyl‐3‐methylimidazole hexafluorophosphate (BMIMPF 6 ) ionic liquid. First, BMIMPF 6 can passivate TiO 2 /CsPbI 3 interface defects by forming strong bond between the electron‐rich N atoms and uncoordinated ions. Second, BMIMPF 6 ‐modified TiO 2 shows reduced hydrophilicity, inducing decreased heterogeneous nucleation and is favorable for obtaining high‐quality CsPbI 3 film. Thirdly, the non‐volatile BMIMPF 6 can diffuse to the perovskite film surface during annealing, further passivating defects located at perovskite grain boundaries and surface. Based on this one‐step ionic liquid interface‐to‐bulk modification, the modified device achieves a champion PCE of 15.09%, which is 14% higher than the control device (13.27%). In addition, the modified device also shows enhanced long‐term stability, which remains 96% of initial PCE after 30 days storage in dry air. The work demonstrates the superiority of multifunctional ionic liquid applied to all‐inorganic carbon‐based PSCs, providing a guidance for its commercialization.
Abstract In order to improve the thermal stability of perovskite solar cells (PSCs) and reduce production costs, hole transport layer (HTL)‐free carbon‐based CsPbI 3 PSCs (C‐PSCs) have attracted the attention of researchers. However, the power conversion efficiency (PCE) of HTL‐free CsPbI 3 C‐PSCs is still lower than that of PSCs with HTL/ metal electrodes. This is because the direct contact between the carbon electrode and the perovskite layer has a higher requirement on the crystal quality of perovskite layer and matched energy level at perovskite/carbon interface. Herein, the acyl chloride group and its derivative trichloroacetyl chloride are used to passivate CsPbI 3 C‐PSCs for the first time. The results show that the carbonyl group of trichloroacetyl chloride can effectively passivate the uncoordinated Pb 2+ ions in perovskite. At the same time, leaving group Cl − ions can increase the grain size of perovskite and improve the crystallization quality of perovskite layer. In addition, the trichloroacetyl chloride tends to generate cesium chloride acetate, which acts as an electron blocking layer, reduces charge recombination, promotes gradient energy level arrangement, and effectively improves the separation and extraction ability of carriers. The PCE of CsPbI 3 HTL‐free C‐PSCs is successfully increased from 13.40% to 14.82%.
Highly reproducible surface-enhanced Raman scattering (SERS) spectra are obtained on the surface of SnO(2) octahedral nanoparticles. The spot-to-spot SERS signals show a relative standard deviation (RSD) consistently below 20 % in the intensity of the main Raman peaks of 4-mercaptobenzoic acid (4-MBA) and 4-nitrobenzenethiol (4-NBT), indicating good spatial uniformity and reproducibility. The SERS signals are believed to mainly originate from a charge-transfer (CT) mechanism. Time-dependent density functional theory (TD-DFT) is used to simulate the SERS spectrum and interpret the chemical enhancement mechanism in the experiment. The research extends the application of SERS and also establishes a new uniform SERS substrate.
We investigated the configuration characteristic and adsorption behavior of 4,4′-thiobisbenzenethiol (TBBT) on the surface of silver nanoparticles (NPs). Under different conditions and preparation processes, several possible surface species were produced including single-end adsorption on a silicon wafer, double-end adsorption and bridge-like adsorption. Although consisting of the same molecule and nano material, different adsorption systems exhibited different spectral characteristics in the surface-enhanced Raman spectroscopy (SERS). A density functional theory (DFT) study further verified the corresponding adsorption states. The combined SERS-DFT study provided a framework towards investigating and designing adsorption systems at a molecular level, indicating the potential use in applications such as nano-sensors.
Abstract Photosystem II (PSII) catalyzes water oxidization and plastoquinone reduction by utilizing light energy. It is highly susceptible to photodamage under high-light conditions and the damaged PSII needs to be restored through a process known as the PSII repair cycle. The detailed molecular mechanism underlying the PSII repair process remain mostly elusive. Here we report biochemical and structural features of a PSII-repair intermediate complex, likely arrested at an early stage of the PSII repair process in the green alga Chlamydomonas reinhardtii. The complex contains three protein factors associated with a damaged PSII core, namely Thylakoid Enriched Factor 14 (TEF14), Photosystem II Repair Factor 1 (PRF1), and Photosystem II Repair Factor 2 (PRF2). TEF14, PRF1 and PRF2 may function to facilitate release of the manganese-stabilizing protein PsbO, disassembly of peripheral light-harvesting complexes from PSII and blockage of the QB site, respectively. Moreover, an α-tocopherol quinone molecule is located adjacent to the heme group of cytochrome b559, potentially fulfilling a photoprotective role by preventing generation of reactive oxygen species.
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