Adamantyl-Substituted Aminoxyls.

The interaction of perfluoroaromatic compounds with 1-aminoadamantane followed by oxidation of the formed -adamantylanilines with -chloroperoxybenzoic acid led to functionalized -polyfluorophenyl--adamantylaminoxyls (mono- and diradicals) in high total yields. The molecular and crystal structures of -adamantylanilines and the aminoxyl radicals obtained from them by oxidation have been established using single-crystal X-ray diffraction analysis. The introduction of a substituent into the polyfluorinated moiety affects the arrangement of -adamantylanilines in the crystal structure and the formation of hydrogen bonds; in addition, short contacts of the rare N···N type are present in crystals of 4-((adamantan-1-yl)amino)-perfluorobiphenyl.

NEATmap: a high-efficiency deep learning approach for whole mouse brain neuronal activity trace mapping.

Quantitative analysis of activated neurons in mouse brains by a specific stimulation is usually a primary step to locate the responsive neurons throughout the brain. However, it is challenging to comprehensively and consistently analyze the neuronal activity trace in whole brains of a large cohort of mice from many terabytes of volumetric imaging data. Here, we introduce NEATmap, a deep learning-based high-efficiency, high-precision and user-friendly software for whole-brain neuronal activity trace mapping by automated segmentation and quantitative analysis of immunofluorescence labeled c-Fos neurons.

Multifunctional MOF@COF Nanoparticles Mediated Perovskite Films Management Toward Sustainable Perovskite Solar Cells.

Although covalent organic frameworks (COFs) with high π-conjugation have recently exhibited great prospects in perovskite solar cells (PSCs), their further application in PSCs is still hindered by face-to-face stacking and aggregation issues. Herein, metal-organic framework (MOF-808) is selected as an ideal platform for the in situ homogeneous growth of a COF to construct a core-shell MOF@COF nanoparticle, which could effectively inhibit COF stacking and aggregation. The synergistic intrinsic mechanisms induced by the MOF@COF nanoparticles for reinforcing intrinsic stability and mitigating lead leakage in PSCs have been explored.

Molecular near-infrared triplet-triplet annihilation upconversion with eigen oxygen immunity.

Molecular triplet-triplet annihilation upconversion often experiences drastic luminescence quenching in the presence of oxygen molecules, posing a significant constraint on practical use in aerated conditions. We present an oxygen-immune near-infrared triplet-triplet annihilation upconversion system utilizing non-organometallic cyanine sensitizers (λ = 808 nm) and chemically synthesized benzo[4,5]thieno[2,3-b][1,2,5]thiadiazolo[3,4-g]quinoxaline dyes with a defined dimer structure as annihilators (λ = 650 nm). This system exhibits ultrastable upconversion under continuous laser irradiance (>480 mins) or extended storage (>7 days) in aerated solutions.

Lanthanide 3D Supramolecular Framework Boosts Stable Perovskite Solar Cells with High UV Utilization.

In this work, the ligand-to-metal charge transition and Förster resonance energy transfer process is exploited to derive lanthanide-organic framework (Tb-cpon) modified perovskite solar cells (PSCs) with enhanced performance under UV irradiation. Tb-cpon-modified PSCs exhibit rapid response and reduced degradation due to energy downconversion facilitated by effective coupling of UV-sensitive chromophores to lanthanide luminescent centers, enhancing the spectral response range of the composite films. Furthermore, the characteristic changes of precursor particle sizes suggest formation of Tb-cpon adducts as intermediate products, leading to enhanced crystallinity and reduced defect concentrations in the Tb-cpon-perovskite hybrid film.

Synthesis and properties of novel type I photosensitizer polycyclic amide.

Herein, we have designed and synthesized a novel type-I photosensitizer (PhPA) Rh-catalyzed oxidative cyclization of diacetoxyterephthalamide with alkynes. The photoelectric properties, photosensitivity and photodegradation process of PhPA have been systematically investigated. The remarkable fluorescence quenching effect ( < 0.

Regulating Crystallization and Lead Leakage of Perovskite Solar Cell Via Novel Polyoxometalate-Based Metal-Organic Framework.

Despite the unprecedented progress in lead-based perovskite solar cells (PSCs), the toxicity and leakage of lead from degraded PSCs triggered by deep-level defects and poor crystallization quality increase environmental risk and become a critical challenge for eco-friendly PSCs. Here, a novel 2D polyoxometalate (POM)-based metal-organic framework (MOF) (C NH ) (C N H ) Zn (H P Mo O ) ·2H O (POMOF) is ingeniously devised to address these issues. Note that the integration of POM endows POMOF with great advantages of electrical conductivity and charge mobility.

{Mo W }: Polyoxometalate Cages Shaped by π-π Interactions.

Here we report the formation of giant {Mo W } polyoxometalate cages templated by π-conjugated planar ligands. Their inorganic shells incorporate arrays of 18 stacked aromatic carboxylates, such as 1,3,5-benzenetricarboxylate or 5-nitroisophthalate, and the assembly is stabilized by multiple π-π interactions. NMR data confirmed that the cages are stable in solution and the inner aromatic templates can be postsynthetically replaced by selected aliphatic dicarboxylates, paving the way for endo-functionalization and exploration of the reactivities within the cage cavities.

Construction of Ag nanocluster-modified AgPO containing silver vacancies via in-situ reduction: With enhancing the photocatalytic degradation activity of sulfamethoxazole.

Photocatalytic removal of sulfonamide antibiotics is an effective strategy to solve environmental pollution. AgPO is a promising anode material for photocatalytic material with photocatalytic degradation ability under ultraviolet light or natural light. Unfortunately, due to its instability, Ag could be reduced to Ag which loaded onto the surface of AgPO during the photocatalytic process, causing self-photocorrosion and resulting in the reduction of photocatalytic activity and stability.

The Evolution of Classical Spiro-OMeTAD: Synthesis of Arylamine Endcapped Indenone Spirofluorene.

Spiro-OMeTAD is the well-known hole transporting material (HTM) in perovskite solar cells. In this work, its derivatives, namely four D-A shaped triphenylamine or biphenylamine endcapped indenone spirofluorene (SFD-TPA, SFD-OMeTPA, SFD-TAD, and SFD-OMeTAD), were designed and synthesized. With the introduction of electron-donating moieties and the extension of conjugation length, a series of changes in photophysical and electrochemical properties could be detected.

Timing matters: pre-assembly post-assembly functionalization of a polyoxovanadate-organic cuboid.

The pre-assembly and post-assembly approaches in the functionalization of a polyoxovanadate-organic cuboid, [{VS}(QPTC){V}], are discussed. We have shown that the two pathways have led to distinctly different systems, with either an expanded or contracted interior void space, when phenylphosphonate is introduced at different stages of the self-assembly. One leaves the cuboid framework largely intact, whereas the other results in a compact, twisted cuboid.

Investigation on the Mechanism of Radical Intermediate Formation and Moderate Oxidation of Spiro-OMeTAD by the Synergistic Effect of Multisubstituted Polyoxometalates in Perovskite Solar Cells.

Conventional oxidation of 2,2',7,7'-tetrakis[,-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (Spiro-OMeTAD) by air would bring various drawbacks for perovskite solar cells (PSCs), such as low power conversion efficiency (PCE) and poor stability. Here, a series of heteroatom-substituted Keggin-type polyoxometalates (POMs), HPMoVO (PMoV), HPMoVO (PMoV), and HPMoVO (PMoV) are prepared and applied as p-type dopants to realize quantitative and controllable oxidation of Spiro-OMeTAD under an inert condition. The possible mechanism and electron donor regions in the oxidation of Spiro-OMeTAD are investigated using two-dimensional nuclear magnetic resonance (NMR) spectra and the relationship between POM structures and the oxidation degree of Spiro-OMeTAD is proposed.

Chemical doping engineering by utilizing trilacunary Keggin polyoxometalates as a dopant for high performance perovskite solar cells.

Chemical doping engineering is an effective strategy to modify the hole transport layer (HTL) and achieve high-efficiency perovskite solar cells (PSCs). In this work, we synthesize an infrequent trilacunary Keggin type polyoxometalate Na[Zn(HO)(WO)(BiWO)] (BiW-Zn) and apply it as an additive to enhance the hole mobility and electrical conductivity of Spiro-OMeTAD based HTLs. Thanks to the strong electron-accepting properties of polyoxometalate molecules, the as-synthesized BiW-Zn can directly oxidize Spiro-OMeTAD under an inert atmosphere and avoid the tedious long-term oxidation process.

Rigidly Fused Spiro-Conjugated π-Systems.

Spiro-fused π-systems have gained considerable attention for their application as semiconductors in molecular electronics. Here, a synopsis regarding recent breakthroughs in ladderized spirobifluorenes and indeno-spirobifluorenes, along with further spiro-condensed heteroatomic hydrocarbons with donor-acceptor moieties, is provided. Additionally, an extended range of rigid spirobifluorene polymers and specific doubly linked spiro-systems with partial chiral character is discussed.

Self-Assembly of Hybrid Oxidant POM@Cu-BTC for Enhanced Efficiency and Long-Term Stability of Perovskite Solar Cells.

The controllable oxidation of spiro-OMeTAD and improving the stability of hole-transport materials (HTMs) layer are crucial for good performance and stability of perovskite solar cells (PSCs). Herein, we report an efficient hybrid polyoxometalate@metal-organic framework (POM@MOF) material, [Cu (BTC) (H O) ] [H PMo O ] or POM@Cu-BTC, for the oxidation of spiro-OMeTAD with Li-TFSI and TBP. When POM@Cu-BTC is introduced to the HTM layer as a dopant, the PSCs achieve a superior fill factor of 0.

Sulfur-Containing Bent N-Heteroacenes.

A series of novel sulfur-containing bent N-heteroacenes were constructed and characterized by NMR and UV/Vis spectroscopy, cyclic voltammetry, and single-crystal X-ray diffraction. By introducing sulfur-containing groups (thio, sulfinyl, and sulfonyl) into bent azaacenes, their electronic delocalization was improved and frontier energy levels were modulated. The target products displayed tunable optical and electronic properties through altering the valence of sulfur and fused length of the azaacenes.

A Copper Coordination Polymer with Matching Energy Level for Modifying Hole Transport Layers to Improve the Performance of Perovskite Solar Cells.

Spiro-OMeTAD is currently the most widely used hole transport material for the preparation of high-performance perovskite solar cells (PSCs), usually requiring the addition of additives to achieve the desired electronic conductivity. However, the quality of the film is degraded owing to the addition of additives. Holes and defects can be observed, and the dispersion of the additives are uneven inside.

Synthesis of π-Conjugated Benzocyclotrimers.

Polycyclic aromatic hydrocarbons (PAHs), especially three branchphene benzocyclotrimers represent a series of molecules with intriguing physical and chemical properties. Benzocyclotrimers are also important precursors to construct fullerenes and graphenes. In this article, we review the recent progress in the preparation methods of π-conjugated benzocyclotrimers.

Hydrodynamic Analysis-Based Modeling and Experimental Verification of a New Water-Jet Thruster for an Amphibious Spherical Robot.

Thrusters are the bottom actuators of the amphibious spherical robot, and play an important role in the motion control of these robots. To realize accurate motion control, a thrust model for a new water-jet thruster based on hydrodynamic analyses is proposed in this paper. First, the hydrodynamic characteristics of the new thruster were numerically analyzed using computational fluid dynamics (CFD) commercial software CFX.

Molecular Ordering of Dithieno[2,3-;2',3'-]benzo[2,1-:3,4-']dithiophenes for Field-Effect Transistors.

Four derivatives of dithieno[2,3-;2',3'-']benzo[1,2-;3,4-']dithiophene () have been synthesized to investigate the correlation between molecular structure, thin-film organization, and charge-carrier transport. Phenyl or thiophene end-capped derivatives at alpha positions of the outer thiophenes of present vastly different optoelectronic properties in comparison with bay-position alkyl-chain-substituted , which was additionally confirmed by density functional theory simulations. The film morphology of the derivatives strongly depends on alkyl substituents, aromatic end-caps, and substrate temperature.