Cations such as K play a key part in the CO electroreduction reaction, but their role in the reaction mechanism is still in debate. Here, we use a highly symmetric Ni-N structure to selectively probe the mechanistic influence of K and identify its interaction with chemisorbed CO. Our electrochemical kinetics study finds a shift in the rate-determining step in the presence of K.
View Article and Find Full Text PDFOxide semiconductor-supported metal nanoparticles often suffer from a high-temperature gas sensing process, resulting in agglomeration and coalescence, which significantly decrease their surface activity and stability. Here, we develop an in situ pyrolysis strategy to redisperse commercial Ir particles (∼15.6 nm) into monodisperse Ir species (∼5.
View Article and Find Full Text PDFThree-dimensional (3D) porous metal oxide nanomaterials with controllable morphology and well-defined pore size have attracted extensive attention in the field of gas sensing. Herein, hierarchically porous ZnO-450 was obtained simply by annealing Zeolitic Imidazolate Frameworks (ZIF-90) microcrystals at an optimal temperature of 450 °C, and the effect of annealing temperature on the formation of porous nanostructure was discussed. Then the as-obtained ZnO-450 was employed as sensing materials to construct a Micro-Electro-Mechanical System (MEMS) gas sensor for detecting NO.
View Article and Find Full Text PDFAs a carcinogenic and highly neurotoxic hazardous gas, benzene vapor is particularly difficult to be distinguished in BTEX (benzene, toluene, ethylbenzene, xylene) atmosphere and be detected in low concentrations due to its chemical inertness. Herein, we develop a depth-related pore structure in Cu-TCPP-Cu to thermodynamically and kinetically enhance the adsorption of benzene vapor and realize the detection of ultralow-temperature benzene gas. We find that the in-plane π electronic nature and proper pore sizes in Cu-TCPP-Cu can selectively induce the adsorption and diffusion of BTEX.
View Article and Find Full Text PDFReasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction. Herein, we present an ingenious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO sensing. We found that the single Pt sites on the MoS surface can induce easier volatilization of adjacent S species to activate the whole inert S plane.
View Article and Find Full Text PDFPalladium (Pd)-modified metal oxide semiconductors (MOSs) gas sensors often exhibit unexpected hydrogen (H ) sensing activity through a spillover effect. However, sluggish kinetics over a limited Pd-MOS surface seriously restrict the sensing process. Here, a hollow Pd-NiO/SnO buffered nanocavity is engineered to kinetically drive the H spillover over dual yolk-shell surface for the ultrasensitive H sensing.
View Article and Find Full Text PDFAmorphous/crystalline heterophase engineering is emerging as an attractive strategy to adjust the properties and functions of nanomaterials. Here, we reveal a heterophase interface role by precisely tailoring the crystalline Pt coverage density on an amorphous Ru surface (cPt/aRu) for ultrasensitive HS detection. We found that when the atomic ratio of Pt/Ru increased from 10 to 50%, the loading modes of Pt changed from island coverage (1cPt/aRu) to cross-linkable coverage (3cPt/aRu) and further to dense coverage (5cPt/aRu).
View Article and Find Full Text PDFThe unsaturated coordination and abundant active sites endow amorphous metals with tremendous potential in improving metal oxide semiconductors' gas-sensing properties. However, the amorphous materials maintain the metastable status and easily transfer into the lower-active crystals during the gas-sensing process at high working temperatures, significantly limiting their further applications. Here, a bimetal amorphous PtRu catalyst is developed by accurately regulating the introduction of Pt species into amorphous RuO supports to realize the highly active and stable H S gas-sensing detection.
View Article and Find Full Text PDFNanomaterials with natural enzyme-mimicking characteristics have aroused extensive attention in various fields owing to their economical price, ease of large-scale production, and environmental resistance. Previous investigations have demonstrated that composition, size, shape, and surface modification play important roles in the enzymelike activity of nanomaterials; however, a fundamental understanding of the crystal facet effect, which determines surface energy or surface reactivity, has rarely been reported. Herein, fluorite cubic CeO nanocrystals with controllably exposed {111}, {100}, or {110} facets are fabricated as proof-of-concept candidates to study the facet effect on the peroxidase-mimetic activity.
View Article and Find Full Text PDFLow-cost and real-time formaldehyde (HCHO) monitoring is of great importance due to its volatility, extreme toxicity, and ready accessibility. In this work, a low-cost and integrated microelectromechanical system (MEMS) HCHO sensor is developed based on SnO multishell hollow microspheres loaded with a bimetallic PdPt (PdPt/SnO-M) sensitizer. The MEMS sensor exhibits a high sensitivity to HCHO ((/ - 1) % = 83.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2021
Rationally constructing single-atom enzymes (SAEs) with superior activity, robust stability, and good biocompatibility is crucial for tumor therapy but still remains a substantial challenge. In this work, we adopt biocompatible carbon dots as the carrier material to load Ru single atoms, achieving Ru SAEs with superior multiple enzyme-like activity and stability. Ru SAEs behave as oxidase, peroxidase, and glutathione oxidase mimics to synchronously catalyze the generation of reactive oxygen species (ROS) and the depletion of glutathione, thus amplifying the ROS damage and finally causing the death of cancer cells.
View Article and Find Full Text PDFIn recent years, bimetallic nanocrystals have attracted great interest from many researchers. Bimetallic nanocrystals are expected to exhibit improved physical and chemical properties due to the synergistic effect between the two metals, not just a combination of two monometallic properties. More importantly, the properties of bimetallic nanocrystals are significantly affected by their morphology, structure, and atomic arrangement.
View Article and Find Full Text PDFThe catalytic properties of supported metal heterostructures critically depend on the design of metal sites. Although it is well-known that the supports can influence the catalytic activities of metals, precisely regulating the metal-support interactions to achieve highly active and durable catalysts still remain challenging. Here, the authors develop a support effect in the oxide-supported metal monomers (involving Pt, Cu, and Ni) catalysts by means of engineering nitrogen-assisted nanopocket sites.
View Article and Find Full Text PDFSci Bull (Beijing)
December 2020
The development of high-performance glucose sensors is an urgent need, especially for diabetes mellitus diagnosis. However, the glucose monitoring is conventionally operated in an invasive finger-prick manner and their noninvasive alternatives largely suffered from the relatively poor sensitivity, selectivity, and stability, resulted from the lack of robust and efficient catalysts. In this paper, we design a concave shaped nitrogen-doped carbon framework embellished with single Co site catalyst (Co SSC) by selectively controlling the etching rate on different facet of carbon substrate, which is beneficial to the diffusion and contact of analyte.
View Article and Find Full Text PDFHere we report the fabrication of a high performance metal oxide semiconductor (MOS) sensor for the detection of hydrogen sulfide (HS) using PdRh bimetal hollow nanocube (HC) with Rh-rich hollow frame and Pd-rich core frame as sensitizing materials. PdRh bimetal HC with the edge-length about 10 nm was prepared by chemical etching PdRh bimetal solid nanocube (SC) in HNO aqueous solution. The results of gas-sensing tests indicate that the response value order of the MEMS gas sensors based on MOSs (including ZnO, MoO and SnO) is as follows: > > .
View Article and Find Full Text PDFNanomaterials with enzyme-mimicking characteristics have engaged great awareness in various fields owing to their comparative low cost, high stability, and large-scale preparation. However, the wide application of nanozymes is seriously restricted by the relatively low catalytic activity and poor specificity, primarily because of the inhomogeneous catalytic sites and unclear catalytic mechanisms. Herein, a support-sacrificed strategy is demonstrated to prepare a single iron site nanozyme (Fe SSN) dispersed on the porous N-doped carbon.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2019
A surface digging effect of supported Ni NPs on an amorphous N-doped carbon is described, during which the surface-loaded Ni NPs would etch and sink into the underneath carbon support to prevent sintering. This process is driven by the strong coordination interaction between the surface Ni atoms and N-rich defects. In the aim of activation of C-H bonds for methane oxidation, those sinking Ni NPs could be further transformed into thermodynamically stable and active metal-defect sites within the as-generated surface holes by simply elevating the temperature.
View Article and Find Full Text PDFHerein, we report a novel carbothermal welding strategy to prepare atomically dispersed Pd sites anchored on a three-dimensional (3D) ZrO nanonet (Pd@ZrO) via two-step pyrolysis, which were evolved from isolated Pd sites anchored on linker-derived nitrogen-doped carbon (Pd@NC/ZrO). First, the NH-HBDC linkers and Zr-based [Zr(μ-O)(μ-OH)] nodes of UiO-66-NH were transformed into amorphous N-doped carbon skeletons (NC) and ZrO nanoclusters under an argon atmosphere, respectively. The NC supports can simultaneously reduce and anchor the Pd sites, forming isolated Pd-N/C sites.
View Article and Find Full Text PDFTin(II) monosulfide (SnS) nanosheets were synthesized using SnCl•5HO and S powders as raw materials in the presence of HO via a facile chemical bath method. Orthorhombic phase SnS nanosheets with a thickness of ~100 nm and lateral dimensions of 2~10 μm were obtained by controlling the synthesis parameters. The formation of a SnO intermediate is key to the valence reduction of Sn ions (from IV to II) and the formation of SnS.
View Article and Find Full Text PDFBismuth tungstate (BiWO) has many intriguing properties and has been the focus of studies in a variety of fields, especially photocatalysis. However, its application in gas-sensing has been seldom reported. Here, we successfully synthesized assembled hierarchical BiWO which consists of ultrathin nanosheets with crystalline-amorphous composite phase by a one-step hydrothermal method.
View Article and Find Full Text PDFBuilding an effective way for finding the role of surface defects in gas sensing property remains a big challenge. In the present work, we synthesized the ZnO nanodishes (NDs) and first explored the formation process of rich electron donor surface defects by means of studying mechanism for the ZnO NDs synthesis. The test results revealed that ZnO-6, added by 6 mmol Zn powder, had the best gas-sensing properties with the excellent selectivity to ethanol than the others.
View Article and Find Full Text PDFZEITLUPE (ZTL) plays an important role in the control of flowering time and photomorpogenesis in Arabidopsis and is highly conserved throughout the plant kingdom. Here, we report the characterization of a soybean ZTL homolog GmZTL3 (Glycine max ZTL 3). The absorption spectrum of the recombinant GmZTL3 proteins indicates that it may be a UV/blue photoreceptor.
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