Dye-sensitized solar cells (DSSCs) have shown significant potential for indoor and building-integrated photovoltaic applications. Herein we present three new D-A-π-A organic sensitizers, XY1, XY2, and XY3, that exhibit high molar extinction coefficients and a broad absorption range. Molecular modifications of these dyes, featuring a benzothiadiazole (BTZ) auxiliary acceptor, were achieved by introducing a thiophene heterocycle as well as by shifting the position of BTZ on the conjugated bridge. The ensuing high molar absorption coefficients enabled the fabrication of highly efficient thin-film solid-state DSSCs with only 1.3 μm mesoporous TiO2 layer. XY2 with a molar extinction coefficient of 6.66 × 10(4) M(-1) cm(-1) at 578 nm led to the best photovoltaic performance of 7.51%.
A new multidentate ligand 1-(9-(1H-1,2,4-triazol-1-yl)anthracen-10-yl)-1H-1,2,4-triazole (tatrz) was designed and synthesized. Using tatrz as a building block, three novel coordination frameworks, namely, {[Cu(tatrz)2(NO3)2]·(CH3OH)·4H2O}n (1), {[Cu(tatrz)2(H2O)2](BF4)2}n (2), and [Mn(tatrz)2(SCN)2(CH3OH)]·2H2O (3) can be isolated. Anion-exchange experiment indicates that NO3(-) anions in the two-dimensional (2D) copper framework of 1 can be completely exchanged by ClO4(-) in an irreversible single crystal-to-single crystal (SC-SC) transformation fashion, as evidenced by the anion-exchange products of {[Cu(tatrz)2(H2O)2](ClO4)2·4CH3OH} (1a). Further, if 1a was employed as a precursor in N,N-dimethylformamide (DMF), an isomorphic solvate of {[Cu(tatrz)2(DMF)2](ClO4)2·2H2O}n (1b) can be generated during the reversible dynamic transformation process. When 1 was immersed in CH3OH, a distinct 2D layer {[Cu(tatrz)2(NO3)2]·4.4CH3OH·0.6H2O}n (1c) was isolated. Interestingly, the solvent-exchange conversion is also invertible between 1 and 1c, which exhibits spongelike dynamic behavior with retention of crystalline integrity. If the 2-fold interpenetrating three-dimensional (3D) framework 2 is selected, it can be transformed into another 2-fold interpenetrating 3D framework {[Cu(tatrz)2(H2O)2](ClO4)2·5.56H2O}n (2a) in a reversible SC-SC transformation fashion. However, when the light yellow crystals of mononuclear complex 3 were exposed to trichloromethane containing aromatic organic anthracene (atan), through our careful observation, the crystals of 3 were dissolved and reassembled into dark brown crystals of 2D crystalline coordination framework {[Mn(tatrz)2(SCN)2]·(atan)}n (3a). X-ray diffraction revealed that in 3a, atan acting as an organic template was encapsulated in the confined space of the 2D grid. Luminescent measurements illustrate that 3a is the first report of multidimensional polymers based on triazole derivatives as luminescent probes of Mg(2+).
For the purpose of investigating the coordination behavior of sterically congested alkenes and exploring the possibility of cofacial complexation in the polycyclic aromatic system for the formation of extended polymeric networks, a new tetradentate ligand, 1,1,2,2-tetrakis[4-(1H-1,2,4-triazol-1-yl)phenyl]ethylene (TTPE), has been designed and synthesized. By using TTPE as a building block with regard to the self-assembly with MnCl2 ⋅4 H2 O, a novel two-dimensional coordination framework {[Mn(TTPE)Cl2 ]⋅4 CHCl3 }n (1) can be isolated. Anion-exchange and organic-group-functionalized aromatic guest TTPE-loaded host-guest complex experimental results indicate that coordinated Cl(-) anions in the 2D framework of 1 can be completely replaced with dissociative ClO4 (-) groups in an irreversible single-crystal-to-single-crystal transformation fashion, as evidenced by the anion-exchange products of {[Mn(TTPE)(H2 O)2 ](ClO4 )2 ⋅0.5 TTPE⋅5.25 H2 O}n (2). Interestingly, TTPE, acting as an organic template, was encapsulated in the confined space of the 2D grid of 2. To the best of our knowledge, such large organic molecules encapsulated in the reactive organic-group-functionalized aromatic-guest-loaded host-guest complex are unprecedented up to now. Luminescence measurements illustrate that 1 and 2 represent novel examples of sensing materials based on triazole derivatives. Further, 2 has been demonstrated by tuning the fluorescence response of porous metal-organic frameworks as a function of adsorbed small analytes.
Three functionally separated donor‐π‐acceptor (D‐π‐A) sensitizers CP‐I–III with a cyano group as the electron‐accepting group and a pyridine as the anchoring group have been developed for dye‐sensitized solar cells (DSSCs). Significantly, the Jsc of CP‐II, which contains a benzo[1,2,5]thiadiazole moiety, is much higher than those of CP‐I and CP‐III, which contain quinoxaline and [1,2,5]thiadiazolo[3,4‐c]pyridine groups, respectively. This is not only a result of the good photon absorption, but also effective intramolecular charge transfer. The conversion efficiency (η) for CP‐II‐based DSSCs is 4.02 %, which is far better than that of CP‐I and CP‐III. Also, the η value for CP‐II is much higher than that for the reference dye P‐II with pyridine as anchoring group.
The effect of plasmon-induced hot carriers (HCs) enables the possibility of applying semiconductors with wide band gaps to visible light catalysis, which becomes an emerging research field in environmental protections. Continued efforts have been made for an efficient heterostructure photocatalytic process with controllable behaviors of HCs. Recently, it has been discovered that the improvement of the utilization of HCs by band engineering is a promising strategy for an enhanced catalytic process, and relevant works have emerged for such a purpose. In this review, we give an overview of the recent progress relating to optimized methods for designing efficient photocatalysts by considering the intrinsic essence of HCs. First, the basic mechanism of the heterostructure photocatalytic process is discussed, including the formation of the Schokkty barrier and the process of photocatalysis. Then, the latest studies for improving the utilization efficiency of HCs in two aspects, the generation and extraction of HCs, are introduced. Based on this, the applications of such heterostructure photocatalysts, such as water/air treatments and organic transformations, are briefly illustrated. Finally, we conclude by discussing the remaining bottlenecks and future directions in this field.
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