共查询到20条相似文献,搜索用时 62 毫秒
1.
Photoinduced Charge‐Carrier Generation in Epitaxial MOF Thin Films: High Efficiency as a Result of an Indirect Electronic Band Gap? 下载免费PDF全文
Dr. Jinxuan Liu Wencai Zhou Jianxi Liu Dr. Ian Howard Dr. Goran Kilibarda Dr. Sabine Schlabach Damien Coupry Dr. Matthew Addicoat Satoru Yoneda Yusuke Tsutsui Dr. Tsuneaki Sakurai Prof. Dr. Shu Seki Dr. Zhengbang Wang Peter Lindemann Dr. Engelbert Redel Prof. Thomas Heine Prof. Dr. Christof Wöll 《Angewandte Chemie (International ed. in English)》2015,54(25):7441-7445
For inorganic semiconductors crystalline order leads to a band structure which gives rise to drastic differences to the disordered material. An example is the presence of an indirect band gap. For organic semiconductors such effects are typically not considered, since the bands are normally flat, and the band‐gap therefore is direct. Herein we show results from electronic structure calculations demonstrating that ordered arrays of porphyrins reveal a small dispersion of occupied and unoccupied bands leading to the formation of a small indirect band gap. We demonstrate herein that such ordered structures can be fabricated by liquid‐phase epitaxy and that the corresponding crystalline organic semiconductors exhibit superior photophysical properties, including large charge‐carrier mobility and an unusually large charge‐carrier generation efficiency. We have fabricated a prototype organic photovoltaic device based on this novel material exhibiting a remarkable efficiency. 相似文献
2.
Ravirajan P Peiró AM Nazeeruddin MK Graetzel M Bradley DD Durrant JR Nelson J 《The journal of physical chemistry. B》2006,110(15):7635-7639
We report on the effect of nanoparticle morphology and interfacial modification on the performance of hybrid polymer/zinc oxide photovoltaic devices. We compare structures consisting of poly-3-hexylthiophene (P3HT) polymer in contact with three different types of ZnO layer: a flat ZnO backing layer alone; vertically aligned ZnO nanorods on a ZnO backing layer; and ZnO nanoparticles on a ZnO backing layer. We use scanning electron microscopy, steady state and transient absorption spectroscopies, and photovoltaic device measurements to study the morphology, charge separation, recombination behavior and device performance of the three types of structures. We find that charge recombination in the structures containing vertically aligned ZnO nanorods is remarkably slow, with a half-life of several milliseconds, over 2 orders of magnitude slower than that for randomly oriented ZnO nanoparticles. A photovoltaic device based on the nanorod structure that has been treated with an amphiphilic dye before deposition of the P3HT polymer yields a power conversion efficiency over four times greater than that for a similar device based on the nanoparticle structure. The best ZnO nanorod:P3HT device yields a short circuit current density of 2 mAcm(-2) under AM1.5 illumination (100 mW cm(-2)) and a peak external quantum efficiency over 14%, resulting in a power conversion efficiency of 0.20%. 相似文献
3.
4.
Ordered porous carbon with tailored pore size for electrochemical hydrogen storage application 总被引:1,自引:0,他引:1
Ordered porous carbon with tailored pore size represents an innovative concept in electrochemical hydrogen storage. This work deals with physical characteristics and electrochemical hydrogen storage behavior of the ordered porous carbons with well-tailored pore size, synthesized by a replica technique using hexagonal mesoporous silica as templates. By using a mixture of two surfactants (HTAB and C16EO8) at different ratios, it is possible to control the wall thickness of silica and, consequently, the pore diameter of carbons within a narrow range of 2.1-2.8 nm. In addition, highly developed ultramicroporosity (pore size smaller than 0.7 nm), which plays a predominant role in hydrogen storage, can be produced in the ordered porous carbons. A discharge capacity of up to 527 mAh/g (corresponding to 1.95 wt % hydrogen storage) has been achieved in 6 M KOH for the ordered porous carbon. Furthermore, the ordered porous carbons also possess excellent capacity retainability after charge-discharge cycles and rate capability. 相似文献
5.
This paper presents a novel and facile method for the fabrication of nanocomposite films with ordered porous surface structures. In this approach, a water-borne poly(styrene-co-butyl acrylate-co-acrylic acid)/silica nanocomposite dispersion was synthesized in situ by surfactant-free emulsion polymerization by using 3-allyloxy-2-hydroxy-1-propanesulfonate as a polymerizable surfactant. When this dispersion was dried to form a film at a certain temperature, an ordered porous structure could be directly obtained on the surface of the nanocomposite film. SEM, TEM, and AFM were employed to observe the morphology, and XPS and particle analyzer were used to analyze the surface composition of the ordered porous nanocomposite film and the particle size, respectively. 相似文献
6.
Ideally ordered anodic porous TiO2 was fabricated by anodizing an Al/Ti layered specimen. A two-layered specimen composed of an Al top layer and a Ti underlying layer was prepared and then processed by nanoimprinting. The Al top layer was easily pretextured by nanoimprinting owing to its softness and it was straightforward to introduce an ideally ordered pore arrangement by anodization. This pore arrangement was transferred to the underlying Ti layer, resulting in ideally ordered porous structures in TiO2. This process can be applied to the high-throughput fabrication of ideally ordered anodic porous oxides other than TiO2 and also to other metals with high hardness. 相似文献
7.
8.
In this Article, we addressed a facile method for the fabrication of porous polyimide film with an ordered surface based on the solvent-evaporation-assisted in situ self-assembly of polyamic acid (PAA, precursor of polyimide) and silica microspheres during vacuum-drying of PAA/silica colloid solution. Hydroxyl groups on the surface of silica microspheres have strong hydrogen-bonding with PAA chains, which improve the dispersion of silica microspheres in PAA/DMF solution and further help the self-assembly of PAA/silica colloid solution via solvent evaporation. The approach is simple, neither the preparation of special template nor complex preparation process and precise control over condition is necessary. Furthermore, the method could be employed for mass production of ordered porous polyimide films, and by changing the content and size of silica microspheres, the pore size and porous structure of the porous polyimide films could be tunable. The wettability behavior of the as-prepared porous polyimide films is also studied; the ordered surface topography of the porous polyimide films could change the wettability from hydrophilicity to hydrophobicity. 相似文献
9.
π‐Electron Systems That Form Planar and Interlocked Anion Complexes and Their Ion‐Pairing Assemblies 下载免费PDF全文
Dr. Ryohei Yamakado Dr. Tsuneaki Sakurai Dr. Wakana Matsuda Prof. Shu Seki Dr. Nobuhiro Yasuda Prof. Shigehisa Akine Prof. Hiromitsu Maeda 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(2):626-638
Interactions between designed charged species are important for the ordered arrangements of π‐electron systems in assembled structures. As precursors of π‐electron anion units, new arylethynyl‐substituted dipyrrolyldiketone boron complexes, which showed anion‐responsive behavior, were synthesized. They formed a variety of receptor–anion complexes ([1+1] and [2+1] types) in solution, and the stabilities of these complexes were discussed in terms of their thermodynamic parameters. Solid‐state ion‐pairing assemblies of [1+1]‐ and [2+1]‐type complexes with countercations were also revealed by single‐crystal X‐ray analysis. In particular, a totally charge‐segregated assembly was constructed based on negatively and positively charged layers fabricated from [2+1]‐type receptor–anion complexes and tetrabutylammonium cations, respectively. Furthermore, the [1+1]‐type anion complex of the receptor possessing long alkyl chains exhibited mesophases based on columnar assembled structures with contributions from charge‐by‐charge and charge‐segregated arrangements, which exhibited charge‐carrier transporting properties. 相似文献
10.
Using the Debye-Hückel pair potential, the collective interactions between identical charged particles were examined via Monte Carlo simulations. The results have shown that when the number of charges per particle and the particle volume fraction were sufficiently large, the pair long-range electrostatic repulsion generated an effective attractive interaction between identical charged particles because of many-body effects. Disordered liquid-like structures, ordered crystal-like structures, ordered structures dispersed in disordered ones, and disordered structures dispersed in ordered ones have been found. The structures are dependent on the volume fraction and charge of the particles, as well as on the electrolyte concentration. 相似文献
11.
Jin Yi Dongsheng Lu Xiaoping Li Shejun Hu Weishan Li Jianfei Lei Yuan Wang 《Journal of Solid State Electrochemistry》2012,16(2):443-448
A porous titania has been prepared by using polystyrene spheres and tri-block copolymer ((EO)20–(PO)70–(EO)20, P123) as templates, and its structure, composition, and performance as anode of lithium ion battery are characterized by
scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction, and galvanostatic charge/discharge
test. The results from SEM and TEM indicate that the prepared porous titania has a trimodal pore system, in which the pores
are in ordered arrangement and interconnected with the same pore diameter and uniform wall thickness. The charge/discharge
tests show that the battery using the prepared porous titania as anode exhibits good rate capacity and cycle stability. 相似文献
12.
Mesoscopic Simulation on Phase Behavior of Pluronic P104 Aqueous Solution at Moderate Concentrations
The mesoscopic dynamics is used to simulate the microphase separation of a block copolymer P104 in water. With simple models, the hexagonal and lamellar phases are produced at moderate concentrations. For comparison, the phase behavior of charged P104 is also investigated. Simulated results indicate a more ordered hexagonal phase with increasing charge of EO blocks. For lamellar phase, however, its structure becomes ordered first and then turns to disordered when the charge arrives at a certain value. Obtained results might be used to forecast new phase behavior of charged P104. 相似文献
13.
多孔硅的制备与光伏特性研究 总被引:3,自引:0,他引:3
采用特制的电解池在不同条件下制备了一系列多孔硅样品。通过测定其SPS发现,多孔硅的SPS特征带同单晶硅相比有明显蓝移,并且随制备条件不同,蓝移效应也不同。电解质中HF浓度和电解时间对基SPS响应有明显影响,这一现象的出现主要归因于最子线阵的生成。 相似文献
14.
Shuiqin Zhou Fengji Yeh Christian Burger Benjamin Chu 《Journal of Polymer Science.Polymer Physics》1999,37(16):2165-2172
Small‐angle X‐ray scattering was used to investigate the nanostructures of complexes formed by slightly crosslinked anionic copolymer gels of poly(sodium methacrylate‐co‐N‐isopropylacrylamide) [P(MAA/NIPAM)] with cetyltrimethylammonium bromide (CTAB), and didodecyldimethylammonium bromide (DDAB), respectively, at room temperature (∼ 23°C). Several highly ordered supramolecular structures were observed in the polyelectrolyte gel–surfactant complexes. In P(MAA/NIPAM)–CTA systems, in sequence with decreasing charge density of the P(MAA/NIPAM) copolymer chains, structures of the Pm3n space group cubic, face‐centered cubic close packing of spheres, and hexagonal close packing of spheres were determined at a charge content of ≥ 75, 67, and 50%, respectively. The spheres and rods in these structures were the spherical and cylindrical micelles formed by the self‐assembly of CTA cations with their paraffin chains inside. Both the aggregation number and the size of the micelles decreased with a decreasing charge density of the copolymer chains. In the P(MAA/NIPAM)–DDA systems, the bilayer lamellar structures formed at charge contents ≥ 75% transferred to bicontinuous cubic structures of the Ia3d space group at charge contents of 50–67%. The rods in the Ia3d cubic structures were formed by the self‐assembly of double‐tailed DDA cations with polar moieties inside. The formation of these highly ordered structures were driven by both electrostatic and hydrophobic interactions of the charged copolymer chains/surfactants and the surfactants/surfactants inside the charged gels. The structures became less ordered by further decreasing the charge content of the P(MAA/NIPAM) chains. © 1999 John Wiley & Sons, Inc. J Polym Sci B: Polym Phys 37: 2165–2172, 1999 相似文献
15.
16.
Dr. Huan Wang Dr. Jian Qi Prof. Nailiang Yang Dr. Wei Cui Prof. Jiangyan Wang Dr. Qinghao Li Dr. Qinghua Zhang Prof. Xiqian Yu Prof. Lin Gu Dr. Jiong Li Prof. Ranbo Yu Prof. Keke Huang Prof. Shuyan Song Prof. Shouhua Feng Prof. Dan Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(44):19859-19863
To boost the performance for various applications, a rational bottom-up design on materials is necessary. The defect engineering on nanoparticle at the atomic level can efficiently tune the electronic behavior, which offers great opportunities in enhancing the catalytic performance. In this paper, we optimized the surface oxygen vacancy concentration and created the lattice distortion in rare-earth-based perovskite oxide through gradient replacement of the B site with valence alternated element. The dual defects make the electron spin state transit from low spin state to high spin state, thus decreasing the charge transport resistance. Furthermore, assembly the modified nanoparticle subunits into the micro-sized hollow multishelled structures can provide porous shells, abundant interior space and effective contact, which enables an enhanced mass transfer and a shorter charge transport path. As a result, the systemic design in the electronic and nano-micro structures for catalyst has brought an excellent oxygen evolution performance. 相似文献
17.
利用强度调制光电流谱(IMPS)研究了不同微结构的TiO2薄膜在不同的浸泡时间条件下的染料分布情况, 分析了染料分布对染料敏化太阳电池光伏性能的影响. 研究结果表明, TiO2薄膜中确实存在染料的不均匀分布现象, 染料不均匀分布对太阳电池的光伏性能有显著的影响. 相似文献
18.
Recent single-molecular observations have revealed that a single giant DNA molecule assumes (micro) phase separated structures upon the addition of condensing agents. Electron and atomic force microscopy have clearly shown the coexistence of ordered tori and disordered coil structures within a single DNA molecule. Motivated by these experimental findings, we theoretically investigated the collapse transition of a single polyelectrolyte chain driven by the addition of condensing guest molecules. We found that the transition behavior critically depends on the degree of the surviving charge inside the torus. When the torus is charged, even slightly, "rings-on-a-string" structures are expected for a sufficiently long chain, owing to the combinational entropy of segment state distribution along the chain and the unique property of the stability of charged torus. 相似文献
19.
20.
Neyshtadt S Jahnke JP Messinger RJ Rawal A Segal Peretz T Huppert D Chmelka BF Frey GL 《Journal of the American Chemical Society》2011,133(26):10119-10133
The chemical compositions and structures of organic-inorganic interfaces in mesostructurally ordered conjugated polymer-titania nanocomposites are shown to have a predominant influence on their photovoltaic properties. Such interfaces can be controlled by using surfactant structure-directing agents (SDAs) with different architectures and molecular weights to promote contact between the highly hydrophobic electron-donating conjugated polymer species and hydrophilic electron-accepting titania frameworks. A combination of small-angle X-ray scattering (SAXS), scanning and transmission electron microscopy (SEM, TEM), and solid-state NMR spectroscopy yields insights on the compositions, structures, and distributions of inorganic and organic species within the materials over multiple length scales. Two-dimensional NMR analyses establish the molecular-level interactions between the different SDA blocks, the conjugated polymer, and the titania framework, which are correlated with steady-state and time-resolved photoluminescence measurements of the photoexcitation dynamics of the conjugated polymer and macroscopic photocurrent generation in photovoltaic devices. Molecular understanding of the compositions and chemical interactions at organic-inorganic interfaces are shown to enable the design, synthesis, and control of the photovoltaic properties of hybrid functional materials. 相似文献