Direct electrosynthesis of hydrogen peroxide (HO) via the two-electron oxygen reduction reaction presents a burgeoning alternative to the conventional energy-intensive anthraquinone process for on-site applications. Nevertheless, its adoption is currently hindered by inferior HO selectivity and diminished HO yield induced by consecutive HO reduction or Fenton reactions. Herein, guided by theoretical calculations, we endeavor to overcome this challenge by activating a main-group Pb single-atom catalyst via a local micro-environment engineering strategy employing a sulfur and oxygen super-coordinated structure.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
February 2022
Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts.
View Article and Find Full Text PDFPrecise synthesis of porous materials is essential for their applications. Self-assembly is a widely used strategy for synthesizing porous materials, but quantitative control of the assembly process still remains a great challenge. Here, a quantitative coassembly approach is developed for synthesizing resin/silica composite and its derived porous spheres.
View Article and Find Full Text PDFAs one of the extensively used feed additives in livestock and poultry breeding, -arsanilic acid (-ASA) has become an organoarsenic pollutant with great concern. For the efficient removal of -ASA from water, the combination of chemical oxidation and adsorption is recognized as a promising process. Herein, hollow/porous Mn-Fe-mixed oxide (MnFeO) nanocubes were synthesized and used in coupling with peroxymonosulfate (PMS) to oxidize -ASA and remove the total arsenic (As).
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