Heterogeneous dual-atomic-site catalysts (DACs) hold great potential for diverse applications. However, to date, the synthesis of DACs primarily relies on different atoms freely colliding on the support during synthesis, principally leading to low yields. Herein, we report a general metal ion recognition (MIR) strategy for constructing a series of DACs, including but not limited to FeSn, FeCo, FeNi, FeCu, FeMn, CoNi, CoCu, Co, and Cu.
View Article and Find Full Text PDFIron single-atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N-doped carbon nanosheets with densely active sites (FeSAs-UNCNS).
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2024
Constructing heterostructures of dual quantum-dots (QDs) is a promising way to achieve high performance in photocatalysis, but it still faces substantial synthetic challenges. Herein, we developed an in situ transformation strategy to coassemble ZnS QDs and C QDs into dual-quantum-dot heterostructural nanofibers (ZnS/C-DQDH). Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy results revealed the formation of strong Zn-O-C bonds at the interface between ZnS QDs and C QDs, improving the separation efficiency of photogenerated charge carriers.
View Article and Find Full Text PDFModulating the electronic metal-support interaction (EMSI) of the single-atomic sites against leaching via microenvironment regulation is critical to achieving high activity and stability but remains challenging. Herein, this work selectively confines Pt single atoms on CoFe layered double hydroxide (LDH) by three oxygen atoms around cation vacancy (Pt /LDH ) or one oxygen atom at the regular surface (Pt /LDH) via cation vacancy engineering. By characterizing the structural evolution of the obtained catalysts before and after vacancy construction and single-atom anchoring, this work demonstrates how the microenvironments modulate the EMSI and the catalytic performance.
View Article and Find Full Text PDFDeveloping efficient nanozymes to mimic natural enzymes for scavenging reactive radicals remains a significant challenge owing to the insufficient activity of conventional nanozymes. Herein, we report a novel Ru single-atom nanozyme (SAE), featuring atomically dispersed Ru atoms on a biocompatible MgAl-layered double hydroxide (Ru /LDH). The prepared Ru /LDH SAE shows high intrinsic peroxidase (POD)-like catalytic activity, which outperforms the Ru nanoclusters (NCs) nanozyme by a factor of 20 and surpasses most SAEs.
View Article and Find Full Text PDFThe development of artificial enzymes with superior catalytic properties to natural enzymes has been a long-standing goal of chemists. Herein, defect-rich CoFe-layered double hydroxides (d-CoFe-LDHs) nanosheets are developed and used as superior peroxidase-like nanozymes for the detection of ascorbic acid (AA). The d-CoFe-LDHs with an average thickness of ∼3 nm and a lateral size of ∼20 nm are synthesized through rapid nucleation in a colloid mill, which exhibited abundant unsaturated sites (oxygen vacancies and cobalt vacancies).
View Article and Find Full Text PDFSingle-atom catalysts (SACs) show great promise in various applications due to their maximal atom utilization efficiency. However, the controlled synthesis of SACs with appropriate porous structures remains a challenge that must be overcome to address the diffusion issues in catalysis. Resolving these diffusion issues has become increasingly important because the intrinsic activity of the catalysts is dramatically improved by spatially isolated single-atom sites.
View Article and Find Full Text PDFRational design and synthesis of superior electrocatalysts for ethanol oxidation is crucial to practical applications of direct ethanol fuel cells. Here, we report that the construction of Pd-Zn dual sites with well exposure and uniformity can significantly improve the efficiency of ethanol electro-oxidation. Through synthetic method control, Pd-Zn dual sites on intermetallic PdZn nanoparticles, Pd-Pd sites on Pd nanoparticles and individual Pd sites are respectively obtained on the same N-doped carbon coated ZnO support.
View Article and Find Full Text PDFHollow materials with a sophisticated structure are promising for various applications with boosted performances and innovative properties. Herein, we report an in situ transformation strategy using multi-layered MOFs as templates to fabricate multi-shelled hollow NiZnCoFe layered double hydroxides (LDHs), which outperformed the double- and single-shelled hollow LDHs and commercial IrO in the oxygen evolution reaction.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) show great promise for electrochemical CO reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single-atom electrode greatly limit their performance. Herein, we prepared a nickel single-atom electrode consisting of isolated, high-density and low-valent nickel(I) sites anchored on a self-standing N-doped carbon nanotube array with nickel-copper alloy encapsulation on a carbon-fiber paper. The combination of single-atom nickel(I) sites and self-standing array structure gives rise to an excellent electrocatalytic CO reduction performance.
View Article and Find Full Text PDFNoble metals play a momentous role in heterogeneous catalysis but still face a huge challenge in selectivity control. Herein, we report isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles as an effective strategy to optimize the selectivity of Pt catalysts. Contiguous Pt atoms are isolated into single atoms and Pt-Zn intermetallic nanoparticles are formed which are supported on hollow nitrogen-doped carbon nanotubes (PtZn/HNCNT), as confirmed by aberration-corrected high-resolution transmission electron microscopy and X-ray absorption spectrometry measurements.
View Article and Find Full Text PDFStrain regulation has become an important strategy to tune the surface chemistry and optimize the catalytic performance of nanocatalysts. Herein, the construction of atomic-layer IrO on IrCo nanodendrites with tunable IrO bond length by compressive strain effect for oxygen evolution reaction (OER) in acidic environment is demonstrated. Evidenced from in situ extended X-ray absorption fine structure, it is shown that the compressive strain of the IrO layer on the IrCo nanodendrites decreases gradually from 2.
View Article and Find Full Text PDFVanadium oxide has attracted extensive attention for electrochemical capacitors due to its wide range of versatility. However, due to the relative poor conductivity and chemical stability of vanadium oxide, severe losses of capacitance often occur during charge and discharge processes. Herein, a free-standing vanadium dioxide (VO(B)) nanobelts/reduced graphene oxide (VO/rGO) composite film was fabricated by assembly of VO(B) nanobelts and rGO for supercapacitors.
View Article and Find Full Text PDFStructure engineering of ultrathin metal-organic framework (MOF) nanosheets to self-supporting and well-aligned MOF superstructures is highly desired for diverse applications, especially important for electrocatalysis. In this work, a facile layered double hydroxides in situ transformation strategy is developed to synthesize ultrathin bimetal-MOF nanosheets (BMNSs) arrays on conductive substrates. This approach is versatile, and applicable to obtain various BMNSs or even trimetal-MOF nanosheets arrays on different substrates.
View Article and Find Full Text PDFExploring efficient and cost-effective catalysts to replace precious metal catalysts, such as Pt, for electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) holds great promise for renewable energy technologies. Herein, we prepare a type of Co catalyst with single-atomic Co sites embedded in hierarchically ordered porous -doped carbon (Co-SAS/HOPNC) through a facile dual-template cooperative pyrolysis approach. The desirable combination of highly dispersed isolated atomic Co-N active sites, large surface area, high porosity, and good conductivity gives rise to an excellent catalytic performance.
View Article and Find Full Text PDFDeveloping an efficient single-atom material (SAM) synthesis and exploring the energy-related catalytic reaction are important but still challenging. A polymerization-pyrolysis-evaporation (PPE) strategy was developed to synthesize N-doped porous carbon (NPC) with anchored atomically dispersed Fe-N catalytic sites. This material was derived from predesigned bimetallic Zn/Fe polyphthalocyanine.
View Article and Find Full Text PDFA novel polymer encapsulation strategy to synthesize metal isolated-single-atomic-site (ISAS) catalysts supported by porous nitrogen-doped carbon nanospheres is reported. First, metal precursors are encapsulated in situ by polymers through polymerization; then, metal ISASs are created within the polymer-derived p-CN nanospheres by controlled pyrolysis at high temperature (200-900 °C). Transmission electron microscopy and N sorption results reveal this material to exhibit a nanospheric morphology, a high surface area (≈380 m g ), and a porous structure (with micropores and mesopores).
View Article and Find Full Text PDFA facile strategy to prepare sintering- and leaching-resistant core-shell nanocatalysts is reported. ZIF-derived porous carbon supported Pd nanoparticles are coated with a mesoporous silica shell, preventing Pd nanoparticles from sintering at high temperature and leaching in a catalytic process. This nanocatalyst exhibits excellent catalytic activity and recyclability for the oxidation of benzyl alcohol.
View Article and Find Full Text PDFForming heterojunctioned composites is an effective way to develop visible-light-driven photocatalysts. A series of BiOBr/NaBiO composites were synthesized by surface transformation of NaBiO with hydrobromic acid. Commensurate planes of BiOBr and NaBiO enabled the formation of a closely bound interface.
View Article and Find Full Text PDFIn this study, an imprinted silica matrix of pentachlorophenol (PCP) co-loaded with Fe(3)O(4) nanoparticles and ZnS:Mn(2+) quantum dots (QDs) was fabricated. The introduction of Fe(3)O(4) nanoparticles to the imprinted matrix provided an easy way to separate PCP under an external magnetic field. ZnS:Mn(2+) QDs offered a readout signal to monitor the amount of PCP bound to the imprinted matrix and evaluate the efficiency of imprinting.
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