Despite recent progress in 2D nanomaterials-based biosensing, it remains challenging to achieve sensitive and high selective detection. This study develops few-layer graphdiyne (GD) nanosheets (NSs) that are used as novel sensing platforms for a variety of fluorophores real-time detection of DNA with low background and high signal-to-noise ratio, which show a distinguished fluorescence quenching ability and different affinities toward single-stranded DNA and double-stranded DNA. Importantly, for the first time, a few-layer GD NSs-based multiplexed DNA sensor is developed.
methods can be further classified to the soft templating method and hard templating method. [57] It has been discovered that some soft matters, such as supramolecular, surfactant micelles, and polymer vesicles can be applied to induce the formation Yanze Wei received his B.S. and M.S. degrees in chemistry from Shandong University, China (2012 and 2015). He then obtained his Ph.D. degree from University of Science Technology Beijing in 2019. He is also a joint Ph.D. student in Institute of Process Engineering, Chinese Academy of Sciences under the supervision of Prof. Dan Wang. His research interests mainly focus on discovering the structure-performance correlation of hollow multishell structured photocatalysts, and mixed-dimensional inorganic/organic heterojunctions. Shouhua Feng an academician of the Chinese Academy of Sciences (2005), obtained his Ph.D. degree in chemistry at Jilin University, P.R. China (1986). He has been engaged in inorganic solidstate chemistry and preparative chemistry for more than 30 years. He has found the triple valence states and atomic scale p-n junctions in perovskite manganese oxides. In recent years, he focuses on the research of functional composite solids and chemical-medicine interdisciplinary.
Constructing hollow multi‐shelled structures (HoMSs) has a significant effect on promoting light absorption property of catalysts and enhancing their performance in solar energy conversion applications. A facile hydrothermal method is used to design the SrTiO3−TiO2 heterogeneous HoMSs by hydrothermal crystallization of SrTiO3 on the surface of the TiO2 HoMSs, which will realize a full coverage of SrTiO3 on the TiO2 surface and construct the SrTiO3/TiO2 junctions. The broccoli‐like SrTiO3−TiO2 heterogeneous HoMSs exhibited a fourfold higher overall water splitting performance of 10.6 μmol h−1 for H2 production and 5.1 μmol h−1 for O2 evolution than that of SrTiO3 nanoparticles and the apparent quantum efficiency (AQE) of 8.6 % at 365 nm, which can be mainly attributed to 1) HoMS increased the light absorption ability of the constructed photocatalysts and 2) the SrTiO3−TiO2 junctions boosted the separation efficiency of the photogenerated charge carriers.
In nature, sequential harvesting of light widely exists in the old life entity, i.e. cyanobacteria, to maximize the light absorption and enhance the photosynthesis efficiency. Inspired by nature, we propose a brand new concept of temporally-spatially sequential harvesting of light in one single particle, which has purpose-designed heterogeneous hollow multi-shelled structures (HoMSs) with porous shells composed of nanoparticle subunits. Structurally, HoMSs consist of different band-gap materials outside-in, thus realizing the efficient harvesting of light with different wavelengths. Moreover, introducing oxygen vacancies into each nanoparticle subunit can also enhance the light absorption. With the benefit of sequential harvesting of light in HoMSs, the quantum efficiency at wavelength of 400 nm is enhanced by six times compared with the corresponding nanoparticles. Impressively, using these aforementioned materials as photocatalysts, highly efficient photocatalytic water splitting is realized, which cannot be achieved by using the nanoparticle counterparts. This new concept of temporally-spatially sequential harvesting of solar light paves the way for solving the ever-growing energy demand.
Constructing delicate nano-/microreactors with tandem active sites in hierarchical architectures is a promising strategy for designing photocatalysts to realize the challenging but attractive CO 2 reduction. Herein, hollow multi-shelled structure (HoMS) based microreactors with spatial ordered hetero-shells are fabricated, which achieve two-step CO 2 -to-CH 4 photoreduction. The multiple inner CeO 2 shells increase the number of active catalytic sites to ensure efficient firststep reaction for generating CO, along with enriching the local CO concentration. The second-step CO-to-CH 4 reaction is consequently induced by amorphous TiO 2 (A-TiO 2 ) composites on the adjacent outer-most shell, thus realizing the CO 2 -to-CH 4 conversion capability using one CeO 2 @CeO 2 /A-TiO 2 HoMS. In-depth explorations in the microreactors provide compositional, structural, and interfacial guidance for engineering HoMS-based microreactors with temporally-spatially ordered shells toward efficient tandem catalysis.
Quadruple-layered TiO films with controllable macropore size are prepared via a confinement self-assembly method. The inverse opal structure with ordered mesoporous (IOM) presents unique light reflection and scattering ability with different wavelengths. Cyan light (400-600 nm) is reflected and scattered by IOM-195, which is in accord with N719 absorption spectra. By manipulating the macropore size, different light responses are obtained.
Photocatalytic overall water splitting (OWS) is an ideal and sustainable solar-to-chemical energy conversion process. [1][2][3][4][5] One important key to improve the solar energy conversion efficiency in this process is enhancing the harvesting of the incident light, which mainly lies on two factors. [6] First, increasing coverage of the solar spectrum by extending the absorption edge of the photocatalysts, especially utilizing visible light (400-700 nm) which occupies 39% of the energy of the total solar irradiation spectrum. [7][8][9][10] Second, sufficient La-and Rh-co-doped SrTiO 3 (STO:La/Rh) hollow multishelled structures (HoMSs) are fabricated by adding La 3+ and Rh 3+ ions during the hydrothermal process of converting TiO 2 HoMSs to STO HoMSs. STO:La/Rh HoMSs have successfully expanded the light absorption edge to 520 nm. Accompanied with the benefits of the unique hierarchical structure and relatively thin shells, STO:La/Rh HoMSs exhibit elevated light-harvesting capacity and charge separation efficiency. Compared with STO:La/Rh nanoparticles (NPs), STO:La/Rh HoMSs demonstrate enhanced photocurrent response, photocatalytic hydrogen evolution activity, and the quantum efficiency. Moreover, overall water splitting is realized by a Z-scheme system combining STO:La/ Rh HoMSs with BiVO 4 (BVO) nanosheets with 1 wt% Pt as the co-catalyst. Steady evolution of hydrogen and oxygen is performed under both visible light and simulated sunlight irradiation. The solar-to-hydrogen efficiency of double-shelled STO:La/Rh HoMS-BVO photocatalysts reaches 0.08%, which is twofold higher than STO:La/Rh NP-BVO photocatalysts.
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