While Prussian Blue (PB) analogues are attractive catalysts for activating peroxymonosulfate (PMS), PB analogues are very small and thus difficult for recovery. Immobilizing PB particles onto graphene is a useful technique which facilitates recovery and also enhances catalytic activities. As doping graphene with sulfur/nitrogen (S/N) increases its electro-conductivity and active sites, the composite of PB and S/N-doped graphene should enhance PMS activation. Thus, this study aims to fabricate such a composite. Unlike conventional S/N-doped graphene prepared via post-modifications, trithiocyanuric acid is used as a precursor, which is converted to S-doped graphitic carbon nitride (SCN). The composite of PB and SCN (PBSCN) is then fabricated by growing a cobalt-based PB analogue on SCN. The resulting PBSCN preserves the crystalline structures, textural properties and catalytic sites of PB and SCN. As degradation of Acid Red 27 (AR) is used as a model reaction, PBSCN exhibits a higher catalytic activity than PB and SCN individually, as well as CoO to activate PMS for AR degradation possibly because SCN may facilitate electron transfer and enhance catalytic activities of PB. PBSCN also remains effective and re-usable over several cycles for AR degradation. These features indicate that PBSCN is a promising catalyst for activating PMS and the fabrication technique demonstrated here can be employed to prepare composites of various PB analogues and carbon nitride to exhibit enhanced catalytic activities.
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http://dx.doi.org/10.1016/j.jcis.2018.05.039 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Fuzhou University, Chemistry, 523 Gongye Rd, Gulou, 350000, Fuzhou, CHINA.
Conjugated polymers, represented by polymeric carbon nitrides (PCNs), have risen to prominence as new-generation photocatalysts for overall water splitting (OWS). Despite considerable efforts, achieving highly crystalline PCNs with minimal structural defects remains a great challenge, and it is also difficult to examine the exact impact of complex defect states on OWS process, which largely limits their quantum efficiency. Herein, we devise a 'in-situ salt flux' assisted copolymerization protocol by using nitrogen-rich and nitrogen-deficient monomers to precisely manipulate the structural defects of poly (triazine imide) (PTI) single crystals.
View Article and Find Full Text PDFACS Catal
January 2025
Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg, 1, 8093 Zurich, Switzerland.
Buchwald-Hartwig (BH) aminations are crucial for synthesizing arylamine motifs in numerous bioactive molecules and fine chemicals. While homogeneous palladium complexes can be effective catalysts, their high costs and environmental impact motivate the search for alternative approaches. Heterogeneous palladium single-atom catalysts (SAC) offer promising recoverable alternatives in C-C cross-couplings.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Weifang University, School of Chemistry & Chemical Engineering and Environmental Engineering, Dongfeng road 5147, 261061, Weifang, CHINA.
The effective S-scheme homojunction relies on the precise regulation of band structure and construction of advantaged charge migration interfaces. Here, the electronic structural properties of g-C3N4 were modulated through meticulous polymerization of self-assembled supramolecular precursors. Experimental and DFT results indicate that both the intrinsic bandgap and surface electronic characteristics were adjusted, leading to the formation of an in-situ reconstructed homojunction interface facilitated by intrinsic van der Waals forces.
View Article and Find Full Text PDFSmall
January 2025
Department of Chemistry, Materials and Chemical Engineering "Giulio Natta", Politecnico di Milano, Piazza Leonardo da Vinci 32, Milano, 20133, Italy.
Single-atom catalysts (SACs) are gathering significant attention in chemistry due to their unique properties, offering uniform active site distribution and enhanced selectivity. However, their precise structure often remains unclear, with multiple models proposed in the literature. Understanding the coordination environment of the active site at the atomic level is crucial for explaining catalytic activity.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Energy and Process Engineering Division, School of Mechanical, Medical and Process Engineering, Science and Engineering Faculty, Queensland University of Technology, 2 George Street, Brisbane City, Queensland 4001, Australia.
The strategic design and fabrication of efficient electrocatalysts are pivotal for advancing the field of electrochemical water splitting (EWS). To enhance EWS performance, integrating non-noble transition metal catalysts through a cooperative double metal incorporation strategy is important and offers a compelling alternative to conventional precious metal-based materials. This study introduces a novel, straightforward, single-step process for fabricating a bimetallic MoCo catalyst integrated within a three-dimensional (3D) nanoporous network of N, P-doped carbon nitride derived from a self-contained precursor.
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