Contrary to conventional understanding, clean anatase {001} facets exhibit lower photoreactivity than {101} facets. Furthermore, the {010} facets showed the highest photocatalytic reactivity in ...generating OH radicals and hydrogen evolution. This behavior was revealed by studies on crystals grown hydrothermally to have a predominance of {001}, {101}, or {010} facets (left to right in picture (a) and (b)–(d), respectively).
Lithium–sulfur batteries (LSBs) are a class of new‐generation rechargeable high‐energy‐density batteries. However, the persisting issue of lithium polysulfides (LiPs) dissolution and the shuttling ...effect that impedes the efficiency of LSBs are challenging to resolve. Herein a general synthesis of highly dispersed pyrrhotite Fe1−xS nanoparticles embedded in hierarchically porous nitrogen‐doped carbon spheres (Fe1−xS‐NC) is proposed. Fe1−xS‐NC has a high specific surface area (627 m2 g−1), large pore volume (0.41 cm3 g−1), and enhanced adsorption and electrocatalytic transition toward LiPs. Furthermore, in situ generated large mesoporous pores within carbon spheres can accommodate high sulfur loading of up to 75%, and sustain volume variations during charge/discharge cycles as well as improve ionic/mass transfer. The exceptional adsorption properties of Fe1−xS‐NC for LiPs are predicted theoretically and confirmed experimentally. Subsequently, the electrocatalytic activity of Fe1−xS‐NC is thoroughly verified. The results confirm Fe1−xS‐NC is a highly efficient nanoreactor for sulfur loading. Consequently, the Fe1−xS‐NC nanoreactor performs extremely well as a cathodic material for LSBs, exhibiting a high initial capacity of 1070 mAh g−1 with nearly no capacity loss after 200 cycles at 0.5 C. Furthermore, the resulting LSBs display remarkably enhanced rate capability and cyclability even at a high sulfur loading of 8.14 mg cm−2.
Hierarchically porous N‐doped carbon spheres embedded with highly active and dispersed Fe1−xS pyrrhotite nanoparticles act as efficient adsorption and conversion nanoreactors of lithium polysulfides for use as high‐sulfur‐loading cathode material in lithium–sulfur batteries, exhibiting high capacity and exceptional long‐term cyclability.
A novel metal–organic framework (MOF), formulated as Cd2(TTVTC)Cl2(H2O)3·2H2O (1), was synthesized from a tetracarboxylate ligand (TTVTC2–) functionalized with the thiazolothiazole extended viologen ...(TTV2+) fluorophore. The MOF features three-dimensional (10,3)-d frameworks with 6-fold interpenetration. The MOF exhibits reversible photochromism, due to photoinduced electron transfer from carboxylate to TTV2+. The photoactivity benefits from the electron donor–acceptor contacts enabled by mutual interpenetration of the frameworks. This is the first demonstration of photochromism in TTV2+ derivatives. In addition, the fluorescence arising from the TTV2+ fluorophore can be reversibly modulated during the photochromic process. The work demonstrates the great potential of extended viologen based ligands in the construction of MOFs with dual photomodulable optical properties, which could find future applications in photoelectronics.
In this work we present the synthesis of a new type of nitrogen-doped tantalate, Sr2Ta2O7-x N x , which exhibited significantly increased visible light absorption and improved photocatalytic hydrogen ...production by 87% under solar irradiation, compared with its undoped counterpart Sr2Ta2O7. The photocatalyst also exhibited a strong capability in photoinduced reduction of exfoliated graphene oxide (GO) to graphene sheets. By using graphene as a support for a Pt cocatalyst, a new type of composite containing graphene-Pt and Sr2Ta2O7-xN x was designed, which demonstrated an additional ∼80% increase in hydrogen production and an quantum efficiency of 6.45% (∼177% increase from pristine undoped Sr2Ta2O7) due to the efficient charge carrier separation on the photocatalyst. This work suggests that graphene can play an important role as an electron transfer highway, which facilitates the charge carrier collection onto Pt cocatalysts. The method can thus be considered as an excellent strategy to increase photocatalytic hydrogen production in addition to a commonly applied doping method.
Abstract Although siRNAs have surpassed expectations in experiments to alter gene expression in vitro , the lack of an efficient in vivo delivery system still remains a challenge in siRNA ...therapeutics development and has been recognized as a major hurdle for clinical applications. In this paper we describe an inorganic nanoparticle-based delivery system that is readily adaptable for in vivo systems. Layered double hydroxide (LDH) nanoparticles, a family of inorganic crystals, tightly bind, protect, and release siRNA molecules and deliver them efficiently to mammalian cells in vitro . The uptake of siRNA-loaded LDH nanoparticles occurs via endocytosis, whereby the nanoparticles dissolve due to the low pH in the endosome, thereby aiding endosomal escape into the cytoplasm. The influence of LDH nanoparticles on cell viability and proliferation is negligible at concentrations ≤0.050 mg mL−1 , and a pronounced down-regulation of protein expression upon LDH mediated siRNA transfection of HEK293T cells is observed.
During the ongoing outbreak of coronavirus disease (COVID-19), people use social media to acquire and exchange various types of information at a historic and unprecedented scale. Only the situational ...information are valuable for the public and authorities to response to the epidemic. Therefore, it is important to identify such situational information and to understand how it is being propagated on social media, so that appropriate information publishing strategies can be informed for the COVID-19 epidemic. This article sought to fill this gap by harnessing Weibo data and natural language processing techniques to classify the COVID-19-related information into seven types of situational information. We found specific features in predicting the reposted amount of each type of information. The results provide data-driven insights into the information need and public attention.
Waveplates are widely used in photonics to control the polarization of light1,2. Often, they are fabricated from birefringent crystals that have different refractive indices along and normal to the ...crystal axis. Similar optical components are found in the natural world, including the eyes of mantis shrimp3,4 and the iridescence of giant clams5, fish6 and plants7. Optical retardation in biology relies on sophisticated self-assembly, whereas man-made systems comprise multiple-layered materials8–11. Here we report a discovery that bridges these two design principles. We observe wideband achromatic retardation in the visible and near-infrared (532–800 nm) regions for Cs4PbBr6 perovskite crystals embedded with CsPbBr3 nanocrystals. We explain our observations as matched dispersions of the refractive indices of the ordinary and extraordinary rays caused by the ordered embedding of the nanocrystals in the host. The wideband performance and ease of fabrication of these perovskite materials are attractive for future applications.Perovskite crystals of Cs4PbBr6 embedded with CsPbBr3 nanocrystals are shown to act as wideband, achromatic waveplates in the visible and near-infrared regions.
Yolk/shell or 'rattle-typed' nanomaterials with nanoparticle cores inside hollow shells are interesting among the complex hollow nanostructures. Yolk/shell nanoparticles (YSNs) are promising ...functional nanomaterials for a variety of applications such as catalysis, delivery, lithium-ion batteries and biosensors due to their tailorability and functionality in both the cores and hollow shells. This feature article provides an overview of advances in this exciting area of YSNs, covering systematic synthesis approaches and key promising applications based on the literature and our own recent work. We present some strategies for the synthesis of YSNs with controllable sizes, compositions, geometries, structures and functionalities. Applications of these new materials in a wide range of potential areas are discussed including nanoreactors, biomedicine and lithium-ion batteries. Promising future directions of this active research field are also highlighted.
Electronic structure intrinsically controls the light absorbance, redox potential, charge-carrier mobility, and consequently, photoreactivity of semiconductor photocatalysts. The conventional ...approach of modifying the electronic structure of a semiconductor photocatalyst for a wider absorption range by anion doping operates at the cost of reduced redox potentials and/or charge-carrier mobility, so that its photoreactivity is usually limited and some important reactions may not occur at all. Here, we report sulfur-doped graphitic C3N4 (C3N4−x S x ) with a unique electronic structure that displays an increased valence bandwidth in combination with an elevated conduction band minimum and a slightly reduced absorbance. The C3N4−x S x shows a photoreactivity of H2 evolution 7.2 and 8.0 times higher than C3N4 under λ > 300 and 420 nm, respectively. More strikingly, the complete oxidation process of phenol under λ > 400 nm can occur for sulfur-doped C3N4, which is impossible for C3N4 even under λ > 300 nm. The homogeneous substitution of sulfur for lattice nitrogen and a concomitant quantum confinement effect are identified as the cause of this unique electronic structure and, consequently, the excellent photoreactivity of C3N4−x S x . The results acquired may shed light on general doping strategies for designing potentially efficient photocatalysts.
Owing to the weak self-assembly ability of precursor components and the serious crosslinking of neighbouring nanospheres during a hydrothermal process, the synthesis of monodisperse mesoporous ...polymer nanospheres with diameters below 500 nm remains a great challenge. Here we extend the synthesis method of mesoporous silica nanospheres to enable the preparation of ordered mesoporous resorcinol formaldehyde nanospheres with particle size from 80 to 400 nm and mesopores of ~3.5 nm in diameter. By finely tuning the synthesis parameters, multi-layered mesoporous resorcinol formaldehyde hollow nanospheres can be successfully synthesized. Mesoporous carbon nanospheres and hollow nanospheres with high surface area are further obtained through carbonization of the polymer spheres. The resulting mesoporous carbon nanospheres are demonstrated as the host cathode material for lithium-sulphur batteries. The synthesis strategy provides a benchmark for fabricating well-defined porous carbonaceous nanospheres with potential for energy storage and conversion applications.
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