Engineering the shape and thus surface structure of Pt nanocrystals is an effective strategy for optimizing their catalytic activities toward various reactions. However, different protocols are typically used to produce Pt nanocrystals with distinctive shapes, making it difficult to directly compare their catalytic activities owing to the complication of surface contamination. Here we demonstrate that Pt nanocrystals with a variety of shapes, including those enclosed with low- or high-index facets, can be synthesized using the same protocol by simply adjusting the concentration of reducing agent and/or the reaction time. Specifically, when the reducing agent was used at a relatively low concentration, Pt truncated cubes, cuboctahedrons, truncated octahedrons, and octahedrons were produced sequentially upon the increase in reaction time. When 67% more reducing agent was used, Pt cubes and concave cubes were obtained consecutively as the reaction time was prolonged. Our quantitative analysis suggests that the diversity of shape and difference in size can be resulted from the difference in reduction kinetics. In evaluating their structure–activity relationship for oxygen reduction, it was established that the high-index facets on Pt concave cubes possessed a specific activity of 6.3 and 1.3 times greater than those of Pt cubes and octahedrons exposed by {1?0?0} and {1?1?1} facets, respectively. This work not only offers a general method for the synthesis of Pt nanocrystals having diverse shapes and thus different types of facets but also highlights the significance of reduction kinetics in controlling the structure evolution of other metal nanocrystals. 相似文献
The Al–Si piston alloys always bear different temperatures because of its peculiar component structure and service condition. Therefore, the tensile strength, elongation to fracture, and corresponding damage mechanisms of Al12SiCuNiMg piston alloys (ASPA) have been investigated with in situ technique at different temperatures. The tensile properties show two‐stage tendencies: the former stage (25–280 °C) is determined by easily broken phases with inherent brittleness (such as primary Si), and the fracture behavior presents rapid brittle fracture after reaching the critical stress (about 430 MPa, based on in situ technique and the elastic stress field model). The later one (280–425 °C) is dominated by particles debonding and θphase coarsening. The plastic deformation behavior, dynamic recovery, and flow process become more significant on account of thermal activation. The Considère criterion h = K indicates that the transition of damage behaviors from insufficient local strength to insufficient matrix strength and the corresponding failure model shifts from brittle to ductile fracture. Based on the damage mechanisms, the elastic field model and thermal activation relation model have been established to characterize the strength of the ASPA at different temperature ranges. 相似文献
Herein, a simple self‐assembly method is proposed for the fabrication of MoO2‐based superhydrophobic material with record high contact angles (contact angle up to about 173°) for conductive metal oxides on hard/soft substrates. The spin‐coated surface demonstrates excellent oil–water separation efficiency (>98%) after 50 cycles and robust corrosion resistance after immersion into different pH solutions for 20 d. These water‐resistant coatings retain excellent superhydrophobicity after oil immersion, knife‐scratch, and long‐cycle sandpaper abrasion, which is not observed on most artificial surfaces. Meanwhile, the functionality switching from superhydrophobicity to supercapacity, which have an inverse relationship in aqueous solutions because of poor electrode wettability, is achieved simply by editing the raw materials source. Tuning of the raw materials leads to the same product MoO2/graphitic carbon with different morphologies and functionalities. Different from superhydrophobic MoO2/carbon ball flowers, MoO2 nanotubes with carbon exhibit excellent supercapacity with a large gravimetric capacitance and great cycling stability. 相似文献
The large‐area formation of functional micropatterns with liquid crystals is of great significance for diversified applications in interdisciplinary fields. Meanwhile, the control of molecular alignment in the patterns is fundamental and prerequisite for the adequate exploitation of their photoelectric properties. However, it would be extremely complicated and challenging for discotic liquid crystals (DLCs) to achieve the goal, because they are insensitive to external fields and surface chemistry. Herein, a simple method of patterning and aligning DLCs on flat substrates is disclosed through precise control of the formation and dewetting of the capillary liquid bridges, within which the DLC molecules are confined. Large‐area uniform alignment occurs spontaneously due to directional shearing force when the solvent is slowly evaporated and programmable patterns could be directly generated on desired substrates. Moreover, the in‐plane column direction of DLCs is tunable by slightly tailoring their chemical structures which changes their self‐assembly behaviors in liquid bridges. The patterned DLCs show molecular orientation–dependent charge transport properties and are promising for templating self‐assembly of other materials. The study provides a facile method for manipulation of the macroscopic patterns and microscopic molecular orientation which opens up new opportunities for electronic applications of DLCs. 相似文献
Recombination of photogenerated electron–hole pairs is extremely limited in the practical application of photocatalysis toward solving the energy crisis and environmental pollution. A rational design of the cascade system (i.e., rGO/Bi2WO6/Au, and ternary composites) with highly efficient charge carrier separation is successfully constructed. As expected, the integrated system (rGO/Bi2WO6/Au) shows enhanced photocatalytic activity compared to bare Bi2WO6 and other binary composites, and it is proved in multiple electron transfer (MET) behavior, namely a cooperative electron transfer (ET) cascade effect. Simultaneously, UV–vis/scanning electrochemical microscopy is used to directly identify MET kinetic information through an in situ probe scanning technique, where the “fast” and “slow” heterogeneous ET rate constants (Keff) of corresponding photocatalysts on the different interfaces are found, which further reveals that the MET behavior is the prime source for enhanced photocatalytic activity. This work not only offers a new insight to study catalytic performance during photocatalysis and electrocatalysis systems, but also opens up a new avenue to design highly efficient catalysts in photocatalytic CO2 conversion to useful chemicals and photovoltaic devices. 相似文献
Ultraviolet (UV) light can be used in versatile applications ranging from photoelectronic devices to biomedical imaging. In the development of new UV light sources, in this study, stable UV emission at ≈350 nm is unprecedentedly obtained from carbon nanospheres (CNSs). The origin of the UV fluorescence is comprehensively investigated via various characterization methods, including Raman and Fourier transform infrared analyses, with comparison to the visible emission of carbon nanodots. Based on the density functional calculations, the UV fluorescence is assigned to the carbon nanostructures bonded to bridging O atoms and dangling –OH groups. Moreover, a twofold enhancement in the UV emission is acquired for Au‐carbon core‐shell nanospheres (Au‐CNSs). This remarkable modification of the UV emission is primarily ascribed to charge transfer between the CNSs and the Au surface. 相似文献
Sodium ion batteries (SIB) are considered promising alternative candidates for lithium ion batteries (LIB) because of the wide availability and low cost of sodium, therefore the development of alternative sodium storage materials with comparable performance to LIB is urgently desired. The sodium ions with larger sizes resist intercalation or alloying because of slow reaction kinetics. Most pseudocapacitive sodium storage materials are based on subtle nanomaterial engineering, which is difficult for large‐scale production. Here, ferroelectric Sn2P2S6 with layered nanostructure is developed as sodium ion storage material. The ferroelectricity‐enhanced pseudocapacitance of sodium ion in the interlayer spacing makes the electrochemical reaction easier and faster, endowing the Sn2P2S6 electrode with excellent rate capability and cycle stability. Furthermore, the facile solid state reaction synthesis and common electrode fabrication make the Sn2P2S6 that becomes a promising anode material of SIB. 相似文献
The growth of a Ni(OH)2 coating on conductive carbon substrates is an efficient way to address issues related to their poor conductivity in electrochemical capacitor applications. However, the direct growth of nickel hydroxide coatings on a carbon substrate is challenging, because the surfaces of these systems are not compatible and a preoxidation treatment of the conductive carbon substrate is usually required. Herein, we present a facile preoxidation-free approach to fabricate a uniform Ni(OH)2 coating on carbon nanosheets (CNs) by an ion-exchange reaction to achieve the in situ transformation of a MgO/C composite to a Ni(OH)2/C one. The obtained Ni(OH)2/CNs hybrids possess nanosheet morphology, a large surface area (278 m2/g), and homogeneous elemental distributions. When employed as supercapacitors in a three-electrode configuration, the Ni(OH)2/CNs hybrid achieves a large capacitance of 2,218 F/g at a current density of 1.0 A/g. Moreover, asymmetric supercapacitors fabricated with the Ni(OH)2/CNs hybrid exhibit superior supercapacitive performances, with a large capacity of 198 F/g, and high energy density of 56.7 Wh/kg at a power density of 4.0 kW/kg. They show excellent cycling stability with 93% capacity retention after 10,000 cycles, making the Ni(OH)2/CNs hybrid a promising candidate for practical applications in supercapacitor devices.