文献速递|华东理工大学JCIS:将单原子光热催化剂与表面定位高温整合到过一硫酸基类芬顿系统中，增强抗生素降解能力

第一作者：Yizhou Wu

通讯作者：雷菊英 教授

通讯单位：华东理工大学资源与环境学院

DOI:10.1016/j.jcis.2024.08.194

Fig. 1. SEM image (a), STEM image (b), HAADF-STEM image and the corresponding EDS elemental mappings (c), and AC-HAADF-STEM image (d) of Co/PMCNs-1; Normalized Co K-edge XANES spectra (e), FT k3-weighted EXAFS spectra (f), and WT-EXAFS plots (g) of Co/PMCNs-1 and its reference samples; EXAFS fitting curve at k space (h) and FT-EXAFS fitting curve at R space (i) of Co/PMCNs-1.

Fig. 2. (a) UV–vis-NIR-DRS spectra of Co/PMCNs-1 and Co/PDA/F127; (b) Temperature change curves of Co/PMCNs-1 solution (0.1 g/L) and pure water under NIR irradiation; (c) The corresponding infrared thermal photos at different time intervals; (d) The heating and cooling curves of Co/PMCNs-1 solution for five cycles.

Fig. 3. (a) Degradation of LEV in different reaction systems; (b) The corresponding pseudo first order reaction constants (kobs) of LEV degradation in different reaction systems; (c) The contribution of four parts on LEV degradation in Co/PMCNs-1+PMS+NIR and PMCNs+PMS+NIR systems; (d) TOC removal efficiency by Co/PMCNs-1+PMS+NIR/Dark system. Reaction conditions: [Catalysts] = 0.1 g/L, [PMS]0 = 1 mM, [Antibiotics]0 = 20 mg/L, with or without NIR (λ ＞ 800 nm) irradiation.

Fig. 4. (a) Effect of initial pH on LEV degradation in Co/PMCNs-1+PMS+NIR system; (b) Effect of Cl−, SO42−, NO3− and H2PO4− on LEV degradation in Co/PMCNs-1+PMS+NIR system ([Cl−] = [SO42−] = [NO3−] = [H2PO4−] = 10 mM); (c) Effect of different simulated water bodies on LEV degradation in Co/PMCNs-1+PMS+NIR system (Surface water quality conditions: pH = 7.8, [COD] = 3.1 mg/L, [TN] = 7.7 mg/L; Ground water quality conditions: pH = 7.3, [TN] = 34.7 mg/L, [Cl−] = 118 mg/L); (d) Degradation efficiency of different antibiotics by Co/PMCNs-1+PMS+NIR system; (e) The device for the larger-scale degradation system; (f) The corresponding LEV degradation efficiency over longer time periods (12 h) (Reaction conditions for the larger-scale degradation system: 50 mg Co/PMCNs-1 on the membrane, [PMS]0 = 1 mM, [LEV]0 = 5 mg/L, the flow rate of peristaltic pump was set at 0.5 rpm, with NIR (λ > 800 nm) irradiation). Reaction conditions for degradation system in (a)-(d): [Catalysts] = 0.1 g/L, [PMS]0 = 1 mM, [Antibiotics]0 = 20 mg/L, with NIR (λ ＞ 800 nm) irradiation.

Fig. 5. (a) The infrared thermal photo of Co/PMCNs-1 sponge immersed in H2O after NIR irradiation for 10 min (the glass vial was filled with H2O); (b, c) Numerical simulation of the temperature distribution and velocity vectors around a single Co/PMCNs-1 nanosphere before (b) and after (c) NIR irradiation; (d, e) PMS decomposition efficiency (d) by different heating methods and the corresponding rate constants (e).

Fig. 6. (a) Quenching tests of Co/PMCNs-1+PMS+NIR system (concentrations and roles of different quenching agents: [MeOH] = 150 mM for quenching SO4·− and ·OH, [TBA] = 150 mM for quenching ·OH; [BQ] = 2 mM for quenching ·O2−; [FFA] = 10 mM for quenching 1O2; [DMSO] = 10 mM for quenching high-valent cobalt-oxo species); (b) EPR spectra of DMPO-SO4·−/·OH adduct in water; (c) EPR spectra of DMPO-·O2− adduct in methanol; (d) EPR spectra of TEMP-1O2 adduct in water.