Singlet oxygen-dominated peroxymonosulfate activation by layered crednerite for organic pollutants degradation in high salinity wastewater

Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the anions and radicals,especially in high salinity conditions.Here,a singlet oxygen(^(1)O_(2))-dominated non-radical process was developed for organic pollutants degradation in high salinity wastewater,with layered crednerite(CuMnO_(2))as catalysts and peroxymonosulfate(PMS)as oxidant.Based on the experiments and density functional theory calculations,^(1)O_(2)was the dominating reactive species and the constructed Cu-O-Mn with electron-deficient Mn captured electron from PMS promoting the generation of^(1)O_(2).The rapid degradation of bisphenol A(BPA)was achieved by CuMnO_(2)/PMS system,which was 5-fold and 21-fold higher than that in Mn_(2)O_(3)/PMS system and Cu_(2)O/PMS system.The CuMnO_(2)/PMS system shown prominent BPA removal performance under high salinity conditions,prominent PMS utilization efficiency,outstanding total organic carbon removal rate,wide range of applicable pH and good stability.This work unveiled that the^(1)O_(2)-dominated non-radical process of CuMnO_(2)/PMS system overcame the inhibitory effect of anions in high salinity conditions,which provided a promising technique to remove organic pollutants from high saline wastewater.

Biocompatible carbon nitride quantum dots nanozymes with high nitrogen vacancies enhance peroxidase-like activity for broadspectrum antibacterial

Nanozyme antibacterial agents with high enzyme-like catalytic activity and strong bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism.Herein,the carbon nitride quantum dots(CNQDs)nanozymes with high nitrogen vacancies(NVs)were mass-productively prepared by a simple ultrasonic-crushing method assisted by propylene glycol.It was found that the NVs of CNQDs were stemmed from the selective breaking of surface N-(C)_(2)sites,accounting for 6.2%.Experiments and density functional theory(DFT)simulations have demonstrated that the presence of NVs can alter the local electron distribution and extend theπ-electron delocalization to enhance the peroxidase-like activity.Biocompatible CNQDs could enter inside microorganisms by diffusion and elevate the bacteria-binding ability,which enhanced the accurate and rapid attack of·OH to the microorganisms.The sterilization rate of CNQDs against Gram-negative bacteria(E.coli),Gram-positive bacteria(S.aureus,B.subtilis),fungi(R.solani)reaches more than 99%.Thus,this work showed great potential for engineered nanozymes for broad-spectrum antibacterial in biomedicine and environmental protection.

One-Pot Synthesis of Highly Luminescent CdTe Quantum Dots by Microwave Irradiation Reduction and Their Hg^(2+)-Sensitive Properties

A facile one-pot microwave irradiation reduction route has been developed for the synthesis of highly luminescent CdTe quantum dots using Na_(2)TeO_(3) as the Te source in an aqueous environment.The synthesis parameters of this simple and rapid approach,including the reaction temperature and time,the pH of the reaction solution and the molar ratio of the 3-mercaptopropionic acid(MPA)stabilizer to Cd^(2+),have considerable influence on the particle size and photoluminescence quantum yield of the CdTe quantum dots.The photoluminescence quantum yield of CdTe quantum dots prepared using relatively short reaction times(1040 min)reached 40%60%(emission peaks at 550640 nm).Furthermore,the resulting products could be used as fl uorescent probes to detect Hg^(2+)ions in aqueous media.The response was linearly proportional to the concentration of Hg^(2+)ion in the range 8.0×10^(9)mol/L to 2.0×10^(6)mol/L with a detection limit of 2.7×10^(9)mol/L.

Synergistic Lewis acid-base sites of ultrathin porous Co_(3)O_(4)nanosheets with enhanced peroxidase-like activity

Surface Lewis acid-base sites in crystal structure may influence the physicochemical properties and the catalytic performances in nanozymes.Understanding the synergistic effect mechanism of Co_(3)O_(4)nanozymes towards substances(3,3’,5,5’-tetramethylbenzidine(TMB)and hydrogen peroxide(H2O2))induced by surface Lewis acid-base sites is important to enhance the efficiency for peroxidase-like reaction.Herein,ultrathin porous Co_(3)O_(4)nanosheets with abundant Lewis acid-base sites were prepared by sodium borohydride(NaBH4)reduction treatment,which exhibited high-efficiency peroxidase-like activity compared with original Co_(3)O_(4)nanosheets.The Lewis acid-base sites for ultrathin porous Co_(3)O_(4)nanosheets nanozyme were owing to the coordination unsaturation of Co ions and the formation of defect structure.Ultrathin porous Co_(3)O_(4)nanosheets had 18.26-fold higher catalytic efficiency(1.27×10^(-2)s^(-1)·mM^(-1))than that of original Co_(3)O_(4)(6.95×10^(-4)s^(-1)·mM^(-1))in oxidizing TMB substrate.The synergistic effect of surface acid and base sites can enhance the interfacial electron transfer process of Co_(3)O_(4)nanosheets,which can be a favor of absorption substrates and the generation of reactive intermediates such as radicals.Furthermore,the limit of detection of hydroquinol was 0.58μM for ultrathin porous Co_(3)O_(4)nanosheets,965-fold lower than original Co_(3)O_(4)(560μM).Besides,the linear range of ultrathin porous Co_(3)O_(4)nanosheets was widely with the concentration of 5.0-1,000μM.Colorimetric detection of hydroquinol by agarose-based hydrogel membrane was provided based on excellent peroxidase-like properties.This study provided insights into designing high-performance nanozymes for peroxidase-like catalysis via a strategy of solid surface acid-base sites engineering.