Herein, two mixed-valence Mn16-containing polyanions, (Mn16) [MnIII10MnII6O6(OH)6(PO4)4(A-a-SiW9O34)4]28- (Mn16-Cs) and [MnIII4MnII12(OH)12(PO4)4(A-a-SiW9O34)4]28- (Mn16-Rb), were successfully fabricated on an indium tin oxide (ITO)-coated glass electrode and a glass carbon electrode (GCE) by a layer-by-layer assembly method. Moreover, four composite films, i.e. [PDDA/Mn16-Cs]n, [PDDA/Mn16-Rb]n, [Mn16-Cs/Rubpy]n, and [Mn16-Rb/Rubpy]n (PDDA: poly(diallyldimethylammonium chloride); Rubpy: tris(2,2'-bipyridyl)ruthenium(ii) chloride; n = 1-10), were constructed for comparison and characterized by UV-visible spectroscopy, cyclic voltammetry (CV), and X-ray photoelectron spectroscopy (XPS). Their electrocatalytic activities towards water oxidation were studied under the same experimental conditions. The results of the controlled experiments indicate that (1) all the four films exhibit expected electrocatalytic activities towards water oxidation; (2) the electrocatalytic activity of Mn16-Cs is better than that of Mn16-Rb in solution and composite films; and (3) the electrocatalytic activities of the composite film [Mn16/Rubpy]n are better than those of the composite film [PDDA/Mn16]n.
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http://dx.doi.org/10.1039/c8dt00927a | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Anhui Normal University, School of Chemistry and Materials Science, CHINA.
The space charge effect induced by high-quality heterojunctions is essential for efficient electrocatalytic processes. Herein, we delicately manipulate intermolecular charge transfer by modifying substituents (-g = -CH3, -H, -NO2) with various electron donating/withdrawing capabilities in CoPc-g/CoS organic-inorganic heterostructures. CoPc-CH3, as a typical electron donor, transfers more electrons to CoS due to the presence of -CH3, forming the strongest space electric field and thus regulating the dual active sites at the interface.
View Article and Find Full Text PDFTalanta
January 2025
College of Chemistry and Bioengineering, Guilin University of Technology, Guilin, 541004, China.
Monitoring reactive nitrogen species (RNS) in complex biological media is essential for evaluating the health status of living organisms; however, biofouling on the sensor surface restricts its applications. To overcome this issue, we developed an antifouling electrochemical sensing platform using copper-platinum bimetallic nanoparticles/N-doped biomass porous carbon fibres (Cu-PtNPs/N-BCF) for directly detecting peroxynitrite anion (ONOO), a major type of RNS. Cyclic voltammetry measurements demonstrated that the Cu-PtNPs/N-BCF-2 nanocomposite, synthesised at a molar ratio of 1:1 between Co and Zn, exhibited exceptional electrocatalytic activity for ONOO oxidation.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
Key Laboratory of Fine Chemicals of College of Heilongjiang Province, Qiqihar University, Qiqihar 161006, China; School of Materials Science and Engineering, Jiamusi University, Jiamusi 154007, China. Electronic address:
Most transition metal-based electrocatalysts, when used for the oxygen evolution reaction (OER), undergo significant restructuring under alkaline conditions, forming localized oxides/hydroxides (MOOH), which act as the real active centers, activating adjacent metal sites and creating new active sites that enhance electrocatalytic behavior. Nevertheless, inducing rapid and in-depth self-reconstruction of catalyst surfaces remains a huge challenge. Herein, this work achieves rapid and in-depth self-reconstruction by doping fluorine into the lattice of transition metal oxides (MO).
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December 2024
Department of Chemistry, Chungnam National University, Daejeon, 34134, Republic of Korea.
Catalyst design plays a critical role in ensuring sustainable and effective energy conversion. Electrocatalytic materials need to be able to control active sites and introduce defects in both acidic and alkaline electrolytes. Furthermore, producing efficient catalysts with a distinct surface structure advances our comprehension of the mechanism.
View Article and Find Full Text PDFDoping strategies have been recognized as effective approaches for developing cost-effective and durable catalysts with enhanced reactivity and selectivity in the electrochemical synthesis of value-added compounds directly from CO. However, the reaction mechanism and the specific roles of heteroatom doping, such as N doping, in advancing the CO reduction reaction are still controversial due to the lack of precise control of catalyst surface microenvironments. In this study, we investigated the effects of N doping on the performances for electrochemically converting CO to CO over Ni@NCNT/graphene hybrid structured catalysts (Ni@NCNT/Gr).
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