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1.
The separation efficiency of charge carriers determines the analytical sensitivity of the paper-based photoelectrochemical sensor. Herein, the Lewis base modification strategy is proposed to promote the carrier separation through an in-situ ion exchange method. Firstly, three-dimensional paper-based hierarchically TiO2 (PHT) arrays are prepared with the one-step hydrothermal method. With the aid of Lewis base, the photo-induced charge separation efficiency and the photocurrent signal are obviously increased. Ultimately, sensitive sensing of prostate specific antigen (PSA) is achieved and the linear range is 1 pg/mL–100 ng/mL with the detection limitation of 0.3 pg/mL.  相似文献   
2.
This work investigated the influence of silver plasmon and reduced graphene oxide (rGO) on the photoelectrochemical performance (PEC) of ZnO thin films synthesized by the sol-gel method. The physicochemical properties of the obtained photo-anodes were systematically studied by using several characterization techniques. The x-ray diffraction analysis showed that all samples presented hexagonal wurtzite structure with a polycrystalline nature. Raman and energy dispersive x-ray (EDX) studies confirmed the existence of both Ag and rGO in ZnO:Ag/rGO thin films. The estimated grain size obtained from scanning electron microscopy (SEM) analysis decreased with Ag doping, then increased to a maximum value after rGO addition. The UV-vis transmission spectra of the as-prepared ZnO:Ag and ZnO:Ag/rGO thin films have shown a reduction in the visible range with a redshift at the absorption edges. The bandgaps were estimated to be around 3.17 eV, 2.7 eV, and 2.52 eV for ZnO, ZnO:Ag, and ZnO:Ag/rGO, respectively. Moreover, the electrical measurements revealed that the charge exchange processes were enhanced at the ZnO:Ag/rGO/electrolyte interface, accompanied by an increase in the (PEC) performance compared to ZnO and ZnO:Ag photo-anodes. Consequently, the photocurrent density of ZnO:Ag/rGO (0.2 mA·cm-2) was around 4 and 2.22 times higher than photo-anodes based on undoped ZnO (0.05 mA·cm-2) and ZnO:Ag (0.09 mA·cm-2), respectively. Finally, from the flat band potential and donor density, deduced from the Mott-Schottky, it was clear that all the samples were n-type semiconductors with the highest carrier density for the ZnO:Ag/rGO photo-anode.  相似文献   
3.
The development of nanostructured semiconductor electrodes represented by a mesoporous TiO2 nanocrystalline (mp-TiO2) film is currently bringing great progresses in photoelectrochemical (PEC) devices for solar-to-electricity and solar-to-chemical conversion. Two serious losses can occur in PEC devices: 1) recombination between the conduction band (CB) electrons and valence band (VB) holes in the bulk and at the surface and 2) back reaction or electron trapping by oxidant in the electrolyte solution during transport to the electron-collecting electrode. Thus, the major challenge in common with the nanostructured semiconductor photoanodes is to achieve efficient charge separation and electron transport. In this study, an ultrathin SiOx layer was formed on both the external and the internal surface of mp-TiO2 using an original chemisorption-calcination technique employing 1,3,5,7-tetramethyltetrasiloxane as a starting material. The SiOx surface modification of the mp-TiO2 photoanode drastically prolongs the mean lifetime of CB-electrons in TiO2 because of enhanced charge separation and electron transport by the negative charge applied in aqueous electrolyte solution. We have demonstrated that the performance of a one-compartment H2O2-photofuel cell using mp-TiO2 as the photoanode is greatly boosted by the surface modification with the SiOx layer. We anticipate that this methodology is widely applicable to nanostructured metal oxide semiconductor electrodes, contributing to the improvement in the performance of PEC devices.  相似文献   
4.
Porous tantalum nitride (Ta3N5) single crystals, combining structural coherence and porous microstructure, would substantially improve the photoelectrochemical performance. The structural coherence would reduce the recombination of charge carriers and maintain excellent transport properties while the porous microstructure would not only reduce photon scattering but also facilitate surface reactions. Here, we grow bulk-porous Ta3N5 single crystals on a two-centimeter scale with (002), (023), and (041) facets, respectively, and show significantly enhanced photoelectrochemical performance. We show the preferential facet growth of porous crystals in a lattice reconstruction strategy in relation to lattice match and lattice channel. We present the facet engineering to enhance light absorption, exciton lifetime and transport properties. The porous Ta3N5 single crystal boosts photoelectrochemical oxidation of alcohols with the (002) facet showing the highest performance of >99 % alcohol conversion and >99 % aldehyde/ketone selectivity.  相似文献   
5.
Recent studies on water‐splitting photoelectrochemical cells (PECs) have demonstrated the intriguing possibility of controlling the spin state in this chemical reaction to form H2 and O2 by exploiting the chirality of organic π‐conjugated supramolecular polymers. Although this fascinating phenomenon has been disclosed, the chiral supramolecular materials reported thus far are not optimized for acting as efficient photosensitizer for dye‐sensitized PECs. In this work we report on the design, synthesis, and characterization of chiral supramolecular aggregates based on C3‐symmetric triphenylamine‐based dyes that are able to both absorb visible light and control the spin state of the process. Variable temperature‐dependent spectroscopic measurements reveal the assembly process of the dyes and confirm the formation of chiral aggregates, both in solution as well as on solid supports. Photoelectrochemical measurements on TiO2‐based anodes validate the advantage of using chiral supramolecular aggregates as photosensitizer displaying higher photocurrent compared to achiral analogues. Moreover, fluorimetric tests for the quantification of the hydrogen peroxide produced, confirm the possibility of controlling the spin of the reaction exerting spin‐selection with chiral supramolecular polymers. These results represent a further step towards the next‐generation of organic‐based water‐splitting solar cells.  相似文献   
6.
Zhang  Shicong  Ye  Haonan  Ding  Haoran  Yu  Fengtao  Hua  Jianli 《中国科学:化学(英文版)》2020,63(2):228-236
Dye-sensitized photoelectrochemical tandem cells have shown the promise for light driven hydrogen production from water owing to the low cost,wide absorption spectra in the visible region and ease to process of their constitutive photoelectrode materials.However,most photo-driven water splitting photoelectrochemical cells driven by organic dye sensitized solar cells exhibit unsatisfactory hydrogen evolution rate,primarily attributed to their poor light capturing ability and low photocurrent performance.Here we present the construction of a tandem system consisting of an organic blue-colored S5 sensitizer-based dyesensitized photoelectrochemical cell(DSPEC) wired in series with three spectral-complemental dyes BTA-2,APP-3 and APP-1 sensitizers-based dye-sensitized solar cell(DSC),respectively.The two spectral-complemental chromophores were used in DSC and DSPEC to ensure that the full solar spectrum could be absorbed as much as possible.The results showed that the photocurrent of tandem device was closely related to the open-circuit voltage(Voc) of sensitized DSC,in which the tandem configuration consisting of S5 based DSPEC and BTA-2 based DSC gave the best photocurrent.On this basis,tandem device with the only light energy and no external applied electrical bias was further constructed of BTA-2 based 2-junction DSC and S5 based DSPEC and obtained a photocurrent of 500 μA cm-2 for hydrogen generation.Furthermore,I-/I3-was used as a redox couple between dye regeneration and O2 production on the surface of Pt-IrO2/WO3.The strategy opens up the application of pure organic dyes in DSC/DSPEC tandem device.  相似文献   
7.
染料敏化光电化学电池(DSPECs)是构建人工光合作用体系的潜在方式,其优势在于可通过优化染料结构来拓展可见光吸收范围,从根本上提高太阳能利用效率.染料敏化光阳极在受激发产生电荷分离之后,激发电子注入TiO2半导体导带,由于其导带位置比传统的可见光半导体,如BiVO4和Fe3O4等相比较负,因此理论上可以在较小的偏压下取得较大的光电转换效率,也更有利于和光阴极相耦合实现无偏压分解水.电荷传输动力学研究表明,注入到TiO2导带的电子向氧化态光敏剂和催化剂的回传是造成体系能量损失的主要原因,集中体现在光电流密度和效率的降低.目前,已经报道了多种手段来减少DSPECs光阳极表面的电子回传,包括使用带有长烷基链的锚定基团对水氧化催化剂进行修饰,在半导体表面引入电子中介体以及使用核-壳结构的基底等.其中,SnO2/TiO2基底被广泛应用在染料敏化光阳极中,这种基底可以提高光生电子的注入效率,同时两种金属氧化物之间的异质结有效抑制了电子回传,从而提高了DSPECs的光电活性.然而,核-壳结构基底需要使用原子层沉积技术来制备,所以操作相对复杂.本文基于Ru-bda(bda=2,2'-联吡啶-6,6'-二羧酸)结构的分子水氧化催化剂和带有磷酸修饰基团的三联吡啶钌通过共吸附的方式制备染料敏化光阳极,在不使用核-壳结构基底的情况下,利用吡啶衍生物对TiO2电极表面的修饰来减少电子回传.本文利用一系列吡啶衍生物作修饰负载在TiO2光阳极上(TiO2|RuP,1;RuP=Ru(4,4'-(PO3H2)2-2,2'-联吡啶)(2,2'-联吡啶)2;1=Ru(bda)(L)2,bda=2,2'-联吡啶-6,6'-二羧酸,L=(10-吡啶-4-基氧基)癸基)膦酸.在100 mW/cm2的白光照射下(λ>400 nm),TiO2|RuP,1,P1(P1=4-羟基吡啶)光阳极在0.4 V(vs.NHE)的外加偏压下获得了1 mA/cm2的光电流密度,其光电流比未修饰吡啶的光阳极增加了42%.同时,其入射光子-电流转化效率在470 nm波长的单色光光照下达到最大,为13.6%.经过吡啶衍生物所修饰的光阳极光电性能和文献中利用核-壳结构基底所制备的类似光阳极性能相当,且光电流密度随吡啶对位取代基供电性能的增强而增大.瞬态吸收光谱和电化学阻抗谱测试表明,吡啶吸附在光阳极上能有效地抑制界面上的电子回传,延长电荷分离寿命,是光电流增加的根本原因,这也表明有机小分子修饰是提高染料敏化光阳极性能的简单、有效的策略.  相似文献   
8.
光解水制氢是人们解决未来能源危机的一种重要构想,构建高效的光电化学池是实现这一构想的重要途径,而光驱动水氧化的顺利进行是实现这一过程的关键.本文总结了近年来基于分子催化剂及染料敏化的光驱动水氧化分子器件的研究和进展,介绍了这些分子器件的组装和性能研究等,并根据这些研究的优点和不足提出一些浅见.  相似文献   
9.
A facile photoetching approach is described that alleviates the negative effects from bulk defects by confining the oxygen vacancy (Ovac) at the surface of BiVO4 photoanode, by 10‐minute photoetching. This strategy could induce enriched Ovac at the surface of BiVO4, which avoids the formation of excessive bulk defects. A mechanism is proposed to explain the enhanced charge separation at the BiVO4 /electrolyte interface, which is supported by density functional theory (DFT) calculations. The optimized BiVO4 with enriched surface Ovac presents the highest photocurrent among undoped BiVO4 photoanodes. Upon loading FeOOH/NiOOH cocatalysts, photoetched BiVO4 photoanode reaches a considerable water oxidation photocurrent of 3.0 mA cm?2 at 0.6 V vs. reversible hydrogen electrode. An unbiased solar‐to‐hydrogen conversion efficiency of 3.5 % is realized by this BiVO4 photoanode and a Si photocathode under 1 sun illumination.  相似文献   
10.
In the past years there has been a great interest in self-doped TiO2 nanotubes (blue TiO2 nanotubes) compared to undoped ones owing to their high carrier density and conductivity. In this study, blue TiO2 nanotubes are investigated as photoanode materials for photoelectrochemical water splitting. Blue TiO2 nanotubes were fabricated with enhanced photoresponse behavior through electrochemical cathodic polarization on undoped and annealed TiO2 nanotubes. The annealing temperature of undoped TiO2 nanotubes was tuned before cathodic polarization, revealing that annealing at 500 °C improved the photoresponse of the nanotubes significantly. Further optimization of the blue TiO2 nanotubes was achieved by adjusting the cathodic polarization parameters. Blue TiO2 nanotubes obtained at the potential of –1.4 V (vs. SCE) with a duration of 10 min exhibited twice more photocurrent response (0.39 mA cm-2) compared to the undoped TiO2 nanotube arrays (0.19 mA cm-2). Oxygen vacancies formed through the cathodic polarization decreased charge recombination and enhanced charge transfer rate; therefore, a high photoelectrochemical activity under visible light irradiation could be achieved.  相似文献   
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