Emerging Hexagonal Mo2C Nanosheet with (002) Facet Exposure and Cu Incorporation for Peroxymonosulfate Activation Toward Antibiotic Degradation.

Abstract

The catalyst with a special exposed active facet and multivalent element synergism is much desired for advanced oxidation progress (AOP) reaction. Herein, an emerging substrate, Cu-incorporated Mo2C, with an active (002) facet exposed was developed by one-step calcination to activate peroxymonosulfate (PMS) toward antibiotic degradation. Combining the multivalent Cu-Mo synergistic effect and Cu complexing interaction, Cu was incorporated onto the Mo2C surface to further enhance its antibiotic removal through PMS activation. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) measurements indicated the 5% Cu-Mo2C exhibited in the hexagonal nanosheet with Cu uniformly dispersed on the surface. Moreover, 5% Cu-Mo2C displayed excellent PMS activation which could fully degrade the tetracycline (TC) within 20 min, and the degradation rate was found to be at least 20 times higher than those of pure Mo2C, classical Fe2O3 and Co3O4, and Fenton reaction of 5% Cu-Mo2C. The results were found to be ascribed to enhanced electrical conductivity, multivalent Cu-Mo synergism, and increased generation of active radicals which contributed in the sequence SO4•- > •OH > O2•-. Surface chemical analysis combined with density functional theory (DFT) calculations confirmed that both Cu2+/Cu+ and Mo6+/Mo4+/Mo2+ redox cycles occurred on the (002) plane of Mo2C, which dominated more free electrons and mainly accounted for facilitating PMS activation. Meanwhile, systematically conditional experiments uncovered that the 5% Cu-Mo2C exhibited superb catalysis even under a wide pH and temperature, various natural polluted waters and coexisting ions, and long-time recycle. In addition, the as-prepared catalyst presented excellent adaptability for the degradation of different organic effluents originated from medical, dyeing, and beneficiation wastewaters. Considering its great performance, stability, and applicability, 5% Cu-Mo2C would be a capable candidate for PMS activation toward large-scale practical application in environmental remediation.