文献速递|山东大学WR:利用单原子铁位点的孔隙调制实现具有放大电子迁移氧化作用的超快类芬顿化学反应

第一作者：Kexin Yin

通讯作者：高宝玉 教授/高悦 副研究员

通讯单位：山东大学环境科学与工程学院

DOI:10.1016/j.watres.2024.122545

Fig. 1. (a) Synthesis route for pFe-SAC. (b-c) HAADF-STEM image and corresponding EDS mappings of pFe-SAC and Fe-SAC. (d) Normalized Fe K-edge XANES. (e) WT plots of EXAFS spectrum. (f) EXAFS fitting curves of pFe-SAC and Fe-SAC at Fe K-edge in the R space. (g) TEM image of different catalysts. (h) XRD of different catalysts. (i) Fe content and BET surface area of different catalysts.

Fig. 2. (a) PMS decomposition and SMX removal efficiencies in these catalysts/PMS systems. (b) The kSMX and kPMS in these catalysts/PMS systems. (c) The kSMX in pFe-SAC/PMS system compared with other SACs reported in literatures. (d) Effects of different radical scavengers on the degradation of SMX in these catalysts/PMS systems. (e) The kSMX values of SMX oxidation in H2O and D2O solutions. (f) TEMP-1O2 and DMPO-•OH, SO4•− signals in these catalysts/PMS systems. (g) PMSO consumption and PMSO2 generation in these catalysts/PMS systems. (h) The oxidation of trans-stilbene in these catalysts/PMS systems. (i) Oxidation of trans-stilbene in these catalysts/PMS systems with/without the addition of SMX. (SMX: = 10 mg/L; trans stilbene: 1.0 mM; PMSO: 25 μM; catalysts = 0.1 g/L; PMS = 1.0 mM).

Fig. 3. (a) OCP changes of different catalysts coated electrode after adding PMS and SMX. (b) The i-t curves of different catalysts with the addition of PMS and SMX. (c) EIS of different catalysts. (d) The scheme of GOS. (e) The current in GOS coating with different catalysts. (f) The LC-MS spectrum of SMX in the pFe-SAC based GOS system. (g) Electrochemical property of different catalysts. (h) OCP changes of pFe-SAC with the addition of different pollutants. (i) Linear correlation between the ln(kobs) and their potentials changes.

Fig. 4. (a) ELF of Fe-N5 and N5 sites (Blue and red colors represent electron delocalization and localization, respectively). (b) Charge density difference of PMS adsorbed on Fe-N5 and N5 sites (Blue and green colors indicate electron depletion and accumulation, respectively). (c) Gaps between LUMO of Fe-N5/PMS or N5/PMS and HOMO of SMX. (d) Gap between LUMO(Fe-N5/PMS) and HOMOpollutants. (e) Linearity between LUMO(Fe-N5/PMS)-HOMOpollutants and ln(kobs). (f-g) Energy barriers associated with the generation of radicals at Fe-N5 sites. (h) The reaction mechanism in pFe-SAC/PMS system.

Fig. 5. (a) Optimized SMX molecular structure, Fukui index (f-) and electrostatic potential of SMX molecule. (b) Degradation pathways of SMX in the pFe-SAC/PMS system. (c) ChV evaluation (≈based on the fish, daphnid, and green algae estimation) of these catalysts/PMS systems. (d) 3DEEM of the SMX solution before and after degradation in these catalysts/PMS systems. (e) Catalytic performances of pFe-SAC towards SMX in different water matrixes. (f) Catalytic performances of pFe-SAC towards SMX in different pH.

Fig. 6. (a) Photograph of the continuous flow degradation experiment with a schematic diagram. (b)AFM and SEM of these organic membrane surfaces. (c) SEM of these catalytic membrane cross sections. (d) The contact angle of these different membranes. (e) The water flux of these different membranes. (f) Pollutants removal in different membrane continuous flow wastewater treatment systems. (g) The removal of various pollutants in the pFe-SAC@PTFE continuous flow system. (h) Catalytic scheme of these pFe-SAC@M continuous flow systems. (i) LCA for the complete water treatment cycle of pFe-SAC/PMS system. (coated catalysts: 1 mg/cm2; pollutants: 500 μg/L, PMS: 2.0 mM).