Reasonable microstructure design is an effective strategy to obtain high-efficiency microwave absorbers. The current explanation for the mechanism of microwave absorption enhancement by microstructures is limited to impedance matching and attenuation constant variation, which lacks a more intuitive understanding. To investigate the microwave absorption enhancement mechanisms arising from hollow structural features and heterointerfaces, a N-doped carbon framework with hollow cavities (H-NC) and embedded iron nanoparticles (H-NC/Fe) was strategically designed and synthesized.
View Article and Find Full Text PDFNanozymes have emerged as a forefront area in analytical sensing research, especially for the sensitive detection of nitrite, which is essential for human health. We synthesized PtCu rhombic dodecahedral nanocrystals (ERD NCs) via a two-step Cu-seeding method. TEM confirms that these NCs are consist of ultra-thin nanosheets with a thickness of approximately 2.
View Article and Find Full Text PDFMatrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) has emerged as a superior technique for detecting small molecules, owing to the strategic utilization of inorganic nanomaterial matrices. Despite the impressive capabilities of various novel matrices, the underlying interaction mechanisms between inorganic matrices and analytes remain largely unexplored. In this study, we synthesized CoO nanocubes, Co(OH) nanosheets, CoO/Co(OH) heterojunctions, and CoO+Co(OH) composites via a facile one-pot method.
View Article and Find Full Text PDFCurrent methods for preparing single atom catalysts (SACs) often suffer from challenges such as high synthesis temperatures, complicated procedures, and expensive equipment. In this study, a facile and universal atomic diffusion strategy near Tamman temperature (AD-T) was proposed for the synthesis of semiconductor supported non-noble metal SACs, denoted as M/S, where M = Fe, Ni, Cu, Al and S = ZnO, CN, TiO(A), InO. Based on the empirical T (c.
View Article and Find Full Text PDFDirect understanding of the formation and crystallization of low-dimensional (LD) perovskites with varying dimensionalities employing the same bulky cations can offer insights into LD perovskites and their heterostructures with 3D perovskites. In this study, the secondary amine cation of N-methyl-1-(naphthalen-1-yl)methylammonium (M-NMA) and the formation dynamics of its corresponding LD perovskite are investigated. The intermolecular π-π stacking of M-NMA and their connection with inorganic PbI octahedrons within the product structures control the formation of LD perovskite.
View Article and Find Full Text PDFUltrathin crystalline materials are a class of popular materials that can potentially exhibit fascinating physical and chemical properties dictated by their unique stacking freedom. However, it is challenging to achieve the controllable synthesis over their stacking structure for ultrathin crystalline materials. Herein, water is employed as a key regulatory factor to realize phase engineering in ultrathin nanosheets (NSs), thereby altering stacking faults to achieve distinct stacking arrangements.
View Article and Find Full Text PDFJ Am Chem Soc
June 2024
Palladium hydrides (PdH) are pivotal in both fundamental research and practical applications across a wide spectrum. PdH nanocrystals, synthesized by heating in dimethylformamide (DMF), exhibit remarkable stability, granting them widespread applications in the field of electrocatalysis. However, this stability appears inconsistent with their metastable nature.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2023
Breaking atomic monogeneity of catalyst surfaces is promising for constructing synergistic active centers to cope with complex multi-step catalytic reactions. Here, we report a defect-derived strategy for creating surface phosphorous vacancies (P-vacancies) on nanometric Rh P electrocatalysts toward drastically boosted electrocatalysis for alkaline hydrogen oxidation reaction (HOR). This strategy disrupts the monogeneity and atomic regularity of the thermodynamically stable P-terminated surfaces.
View Article and Find Full Text PDFJ Chem Phys
September 2023
Colloidal quantum confined semiconductor-metal heterostructures are promising candidates for solar energy conversion because their light absorbing semiconductor and catalytic components can be independently tuned and optimized. Although the light-to-hydrogen efficiencies of such systems have shown interesting dependences on the morphologies of the semiconductor and metal domains, the mechanisms of such dependences are poorly understood. Here, we use Pt tipped 0D CdS quantum dots (with ∼4.
View Article and Find Full Text PDFEnhancing the catalytic activity of Ru metal in the hydrogen oxidation reaction (HOR) potential range, improving the insufficient activity of Ru caused by its oxophilicity, is of great significance for reducing the cost of anion exchange membrane fuel cells (AEMFCs). Here, we use Ru grown on Au@Pd as a model system to understand the underlying mechanism for activity improvement by combining direct in situ surface-enhanced Raman spectroscopy (SERS) evidence of the catalytic reaction intermediate (OH) with in situ X-ray diffraction (XRD), electrochemical characterization, as well as DFT calculations. The results showed that the Au@Pd@Ru nanocatalyst utilizes the hydrogen storage capacity of the Pd interlayer to "temporarily" store the activated hydrogen enriched at the interface, which spontaneously overflows at the "hydrogen-deficient interface" to react with OH adsorbed on Ru.
View Article and Find Full Text PDFAmorphous metals and alloys are promising candidates for superior catalysts in many catalytic and electrocatalytic reactions. It is of great urgency to develop a general method to construct amorphous alloys and further clarify the growth mechanism in a wet-chemical system. Herein, inspired by the conservation of energy during the crystallization process, amorphous PdCu nanoalloys have been successfully synthesized by promoting the chemical potential of the building blocks in solution.
View Article and Find Full Text PDFElectromagnetic radiation and noise pollution are two of the four major environmental pollution sources. Although various materials with excellent microwave absorption performances or sound absorption properties have been manufactured, it is still a great challenge to design materials with both microwave absorption and sound absorption abilities due to different energy consumption mechanisms. Herein, a combination strategy based on structural engineering was proposed to develop bi-functional hierarchical Fe/C hollow microspheres composed of centripetal Fe/C nanosheets.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2023
High-entropy alloys (HEAs) have been attracting extensive research interests in designing advanced nanomaterials, while their precise control is still in the infancy stage. Herein, we have reported a well-defined PtBiPbNiCo hexagonal nanoplates (HEA HPs) as high-performance electrocatalysts. Structure analysis decodes that the HEA HP is constructed with PtBiPb medium-entropy core and PtBiNiCo high-entropy shell.
View Article and Find Full Text PDFWater oxidation is one of the most challenging steps in CO photoreduction, but its influence on CO photoreduction is still poorly understood. Herein, the concept of accelerating the water oxidation kinetics to promote the CO photoreduction is realized by incorporating supramolecular porphyrin nanosheets (NS) into the C N catalyst. As a prototype, porphyrin-C N based van der Waals heterojunctions with efficient charge separation are elaborately designed, in which the porphyrin and C N NS serve as the water oxidation booster and CO reduction center, respectively.
View Article and Find Full Text PDFJ Phys Chem Lett
June 2022
The antimony chalcogenide crystals are composed of quasi-one-dimensional [SbX] ribbons, which lead to strong anisotropic optical and electronic properties. An attempt to exploit photoconductivity anisotropy in the device fabrication may introduce a rewarding strategy to propel the development of the antimony chalcogenide solar cells. To achieve this, understanding of the dynamic evolution of the photoconductivity anisotropy is required.
View Article and Find Full Text PDFOwing to their unique electromagnetic properties and structure anisotropy, two-dimensional (2D) magnetic metal flakes are attracting special attention for applications as microwave absorption materials. However, the conductive network formed by the connected metal flakes may lead to impedance mismatching and reduced performance. In this study, a facile and rational strategy was developed to fabricate yolk-shell-structured 2D flaky Fe/void/C composites by using α-FeO hexagonal flakes as the template, followed by the coating of polydopamine (PDA) on the composite surface and calcination under H/Ar.
View Article and Find Full Text PDFPd-based electrocatalysts are considered to be a promising alternative to Pt in anion-exchange membrane fuel cells (AEMFCs), although major challenges remain. Most of the Pd-based electrocatalysts developed for the sluggish oxygen reduction reaction (ORR) have been exclusively evaluated by rotating disk electrode (RDE) voltammetry at room temperature, rather than in membrane electrode assemblies (MEAs), making it challenging to apply them in practical fuel cells. We have developed a series of carbon-supported novel PdH nanosheets (PdH NS), which displayed outstanding ORR performance in room-temperature RDE tests.
View Article and Find Full Text PDFDual-active-sites atomically coupled on ultrafine 1D nanowires (NWs) can offer synergic atomic heterojunctions (AHJs) and high atomic-utilization toward multipurpose and superior catalysis. Here, ≈2-nm-thick PtIr/IrO hybrid NWs are elaborately synthesized with equilibrated Pt/IrO AHJs as high-efficiency bifunctional electrocatalysts for overall water splitting. Mechanism studies reveal the atomically coupled Pt-IrO dual-sites are favorable for facilitating water dissociation, alleviating the binding of H* on Pt sites and inversely regulating the *OH adsorption and oxidation on bridge Ir-Ir sites.
View Article and Find Full Text PDFResearch of detection of low molecular weight compounds on human health and biological systems become increasingly important. Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS), a soft ionization equipment, is a rapid, reliable, high-sensitivity, high-throughput and simple test instrument. However, the application of MALDI-TOF MS in the analysis of small molecules (<500 Da) has become a great challenge because of the interference from the conventional matrices in low mass region when using conventional matrices.
View Article and Find Full Text PDFDecreasing the metal catalyst size into nanoclusters or even single atom is an emerging direction of developing more efficient and cost-effective photocatalytic systems. Because the catalyst particle size affects both the catalyst activity and light driven charge separation efficiency, their effects on the overall photocatalytic efficiency are still poorly understood. Herein, using a well-defined semiconductor-metal heterostructure with Pt nanoparticle catalysts selectively grown on the apexes of CdS nanorods (NRs), we study the effect of the Pt catalyst size on light driven H generation quantum efficiency (QE).
View Article and Find Full Text PDFSmall Methods
March 2021
The intrinsic factors affecting the bulk structures of nanocrystallites are not well explored during crystallization. In this study, it is demonstrated that the chemical potential of growth units plays decisive role in governing the final structure of nanocrystals. It is found that the types of reaction vessels are able to vary the chemical potential of growth units, and make the Pt and Pd nanocrystals (NCs) unexpectedly evolve from the cyclic penta-twinned to the single-crystal nanostructures.
View Article and Find Full Text PDFRenewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.
View Article and Find Full Text PDFEthanol is a promising liquid clean energy source in the energy conversion field. However, the self-poisoning caused by the strongly adsorbed reaction intermediates (typically, CO) is a critical problem in ethanol oxidation reaction. To address this issue, we proposed a joint use of two strategies, alloying of Pt with other metals and building Pt/metal-oxide interfaces, to achieve high-performance electrocatalytic ethanol oxidation.
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