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Highly dispersed metal (Pd, Pt) nanoparticles and uniformly distributed metal (Au, Ag) nanowires have been synthesized in ordered mesoporous silica SBA-15 via conventional incipient wetness impregnation followed by novel glow discharge plasma reduction. N 2 adsorption-desorption isotherms and the low-angle X-ray diffraction (XRD) patterns indicate that the parent ordered mesoporous structure was well-maintained during the synthesis process. The wide-angle XRD patterns and transmission electron microscope images demonstrate that spherical Pd and Pt nanoparticles as well as rodlike Au and Ag nanowires were fabricated within the channels of SBA-15. The diameters of the metal nanoparticles and the metal nanowires were effectively controlled by the mesopores of the SBA-15 host. The population of the metal nanoparticles and the length of the metal nanowires can be tuned by the metal loading amount. In particular, the novel plasma reduction at ambient temperature is green, economical, and non-time-consuming, showing great advantages over the traditional hydrogen reduction at elevated temperature. This very simple synthesis method with the use of plasma reduction will be very promising as a general technique for the preparation of metal nanostructured materials confined in the host architectures.

Rich chemistry and surface functionalization provide MXenes enhanced electrochemical activity yet severely exacerbate their self-discharge behavior in supercapacitors. However, this self-discharge behavior and its related mechanism are still remaining issues. Herein, we propose a chemically interface-tailored regulation strategy to successfully unravel and efficiently alleviate the self-discharge behavior of Ti3C2T x MXene-based supercapacitors. As a result, Ti3C2T x MXenes with fewer F elements (∼0.65 atom %) show a positive self-discharge rate decline of ∼20% in comparison with MXenes with higher F elements (∼8.09 atom %). Such decline of the F elements can highly increase tight-bonding ions corresponding to an individual self-discharge process, naturally resulting in a dramatic 50% increase of the transition potential (V T). Therefore, the mixed self-discharge rate from both tight-bonding (contain fewer F elements) and loose-bonding ions (contain more F elements) is accordingly lowered. Through chemically interface-tailored engineering, the significantly changed average oxidation state and local coordination information on MXene affected the interaction of ion counterparts, which was evidently revealed by X-ray absorption fine structures. Theoretically, this greatly improved self-discharge performance was proven to be from higher adsorption energy between the interface of the electrode and the electrolyte by density functional theory. Therefore, this chemically interface-tailored regulation strategy can guide the design of high-performance MXene-based supercapacitors with low self-discharge behavior and will promote its wider commercial applications.

Heterogeneous catalytic ozonation (HCO) processes have been widely studied for water purification. The reaction mechanisms of these processes are very complicated because of the simultaneous involvement of gas, solid, and liquid phases. Although typical reaction mechanisms have been established for HCO, some of them are only appropriate for specific systems. The divergence and deficiency in mechanisms hinders the development of novel active catalysts. This critical review compares the various existing mechanisms and categorizes the catalytic oxidation of HCO into radical-based oxidation and nonradical oxidation processes with an in-depth discussion. The catalytic active sites and adsorption behaviors of O 3 molecules on the catalyst surface are regarded as the key clues for further elucidating the O 3 activation processes, evolution of reactive oxygen species (ROS) or organic oxidation pathways. Moreover, the detection methods of the ROS produced in both types of oxidations and their roles in the destruction of organics are reviewed with discussion of some specific problems among them, including the scavengers selection, experiment results analysis as well as some questionable conclusions. Finally, alternative strategies for the systematic investigation of the HCO mechanism and the prospects for future studies are envisaged.

The peroxone reaction between O3 and H2O2 has been deemed a promising technology to resolve the increasingly serious water pollution problem by virtue of the generation of superactive hydroxyl radicals (•OH), but it suffers greatly from an extremely limited reaction rate constant under acidic conditions (ca. less than 0.1 M–1 s–1 at pH 3). This article describes a heterogeneous catalyst composed of single Mn atoms anchored on graphitic carbon nitride, which effectively overcomes such a drawback by altering the reaction pathway and thus dramatically promotes •OH generation in acid solution. Combined experimental and theoretical studies demonstrate Mn–N4 as the catalytically active sites. A distinctive catalytic pathway involving HO2 • formation by the activation of H2O2 is found, which gets rid of the restriction of HO2 – as the essential initiator in the conventional peroxone reaction. This work offers a new pathway of using a low-cost and easily accessible single-atom catalyst (SAC) and could inspire more catalytic oxidation strategies.