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Activation of peroxymonosulfate by FeVO3-x for the degradation of carbamazepine: Vanadium mediated electron shuttle and oxygen vacancy modulated interface chemistry
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Leiduo Laia, b, Hongyu Zhoua, b, Yichen Hongc, Mengfan Luoa, b, Yang Shi*, a, b, Heng Zhanga, b, Zhaokun Xionga, b, Gang Yaob, d, Bo Lai*, a, b
Chinese Chemical Letters | 2024, 35(1) : 108580
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Chinese Chemical Letters | 2024, 35(1): 108580
• Communication •
Activation of peroxymonosulfate by FeVO3-x for the degradation of carbamazepine: Vanadium mediated electron shuttle and oxygen vacancy modulated interface chemistry
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Leiduo Laia, b, Hongyu Zhoua, b, Yichen Hongc, Mengfan Luoa, b, Yang Shi*, a, b, Heng Zhanga, b, Zhaokun Xionga, b, Gang Yaob, d, Bo Lai*, a, b
Affiliations
  • aState Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China
  • bSino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
  • cChengdu Baixi Environmental Technology Company, Chengdu 610065, China
  • dInstitute of Environmental Engineering, RWTH Aachen University, Germany
Published: 2024-01-15 doi: 10.1016/j.cclet.2023.108580
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Fast Fe(Ⅲ)/Fe(Ⅱ) circulation in heterogeneous peroxymonosulfate (PMS) activation remains as a bottleneck issue that restricts the development of PMS based advanced oxidation processes. Herein, we proposed a facile ammonia reduction strategy and synthesized a novel FeVO3-x catalysts to activate PMS for the degradation of a typical pharmaceutical, carbamazepine (CBZ). Rapid CBZ removal could be achieved within 10 min, which outperforms most of the other iron or vanadium-based catalysts. Electron paramagnetic resonance analysis and chemical probe experiments revealed SO4•−, •OH, O2•− and high valent iron (Fe(Ⅳ)) were all generated in this system, but SO4•− and Fe(Ⅳ) primarily contributed to the degradation of CBZ. Besides, X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy indicated that both the generated low-valent V provides and oxygen vacancy acted as superior electron donors and accelerated internal electron transfer via the unsaturated V−O−Fe bond. Finally, the proposed system also exhibited satisfactory performance in practical applications. This work provides a promising platform in heterogeneous PMS activation.

Peroxymonosulfate  /  Fe(Ⅲ)/Fe(Ⅱ) cycle  /  Electron shuttles  /  Oxygen vacancy  /  Bimetallic catalysts
Leiduo Lai, Hongyu Zhou, Yichen Hong, Mengfan Luo, Yang Shi, Heng Zhang, Zhaokun Xiong, Gang Yao, Bo Lai. Activation of peroxymonosulfate by FeVO3-x for the degradation of carbamazepine: Vanadium mediated electron shuttle and oxygen vacancy modulated interface chemistry[J]. Chinese Chemical Letters, 2024 , 35 (1) : 108580 - . DOI: 10.1016/j.cclet.2023.108580
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Iron induced heterogeneous peroxymonosulfate (PMS) activation processes are promising technologies for the degradation of personal care products (PPCPs) in waters due to the strong oxidation capacity of the generated reactive oxygen species (ROS) [1-3]. However, the rate-limiting step of Fe(Ⅲ) conversion to Fe(Ⅱ) significantly prohibits PMS decomposition and ROS generation, thus inhibiting the degradation of target pollutants [4,5]. In order to expedite the Fe(Ⅲ)/Fe(Ⅱ) cycle and ROS generation, previous works usually introduced homogeneous reducing agents in PMS activation processes as co-catalysts for fast removal of refractory pollutants [6-9]. Unfortunately, the introduction of homogeneous reductants is restricted in the practical applications due to the serious environmental pollution induced by the oxidized by-products in waters [10]. Therefore, it is of great interest to develop novel strategies to accelerate the Fe(Ⅲ)/Fe(Ⅱ) circulation.
It was reported that transition metals serving as electron shuttles can also facilitate the Fe(Ⅲ)/Fe(Ⅱ) conversion in Fenton-like oxidation, since the polyvalent metals as electron-sacrificers can donate electrons to Fe(Ⅲ) until they are oxidized to the highest valence [4,11-13]. Our previous results suggested that when the MnFe2O4, Fe2Mo3O12 and Fe2TiO5 served as catalysts, pollutant degradation efficiencies in PMS activation processes are much lower than that of FeVO4 [4], indicating V species serving as electron shuttles outperform Mo, Ti, Mn. Therefore, modulating Fe-based materials with V species provides a great platform to accelerate Fe(Ⅲ)/Fe(Ⅱ) circulation without environmental pollution caused by dissolved matters in waters. Nevertheless, in most cases, stable state of V species in materials are quinquevalent (V(Ⅴ)) due to the electron-deficient of 3d34s2 orbits, implying the difficulties of V species as electron donators lie in the strategy for V reduction in the V modulated Fe-based materials. Our previous study suggested that adding reducing agents can facilitate V(Ⅴ) species reduction in the FeVO4, further triggering the long-lasting Fe(Ⅲ)/Fe(Ⅱ) circulation to effectively degrade target pollutants [4]. However, reducing agents at inappropriate dosage may impede the pollutant degradation efficiency due to the quenching effect of ROS and the direct consumption of oxidants. Therefore, it is imperative to develop new tactics to reduce V species in the Fe-V bimetallic materials.
In this work, a low valent Fe-V bimetallic material (FeVO3-x) with enriched oxygen vacancy was prepared by a coprecipitation method and an ammonia reduction method to activate PMS for carbamazepine (CBZ) degradation. Notably, the reduction process would not only lead to the reduction of V, but also induce the generation of abundant electron-rich oxygen vacancy, which was reported to be a robust PMS adsorption site as well as a flexible switcher to regulate the mechanism transformation from radical to high valent iron (Fe(Ⅳ)) generation [14-16]. Therefore, the FeVO3-x may exhibit dual functions to activate PMS and generate a myriad of ROS for CBZ degradation: (ⅰ) low valent V species as electron donators raise the efficiency of Fe(Ⅲ)/Fe(Ⅱ) conversion; (ⅱ) oxygen vacancy facilitates the generation of high valent Fe species. This work provides new insights into the heterogeneous Fe(Ⅲ) reduction and ROS production by the defect Fe-V bimetallic catalyst. In addition, the CBZ transformation products and their corresponding toxicity were examined to evaluate the practicability of the FeVO3-x/PMS system.
Details about the chemicals were provided in Text S1 (Supporting information). The FeVO3-x was synthesized by the combination methods of coprecipitation and ammonia reduction. In a typical procedure, 2.8078 g NH4VO3 was dissolved in 150 mL deionized water at 80 ℃, and then 150 mL of transparent orange solution with 9.696 g Fe(NO3)3·9H2O was slowly added into NH4VO3 solution and stirred for 1 h at 80 ℃. The solution was further modulated with dilute ammonia to maintain the pH at 8.0, and aged for several hours at room temperature. Then, the precipitates after filtration and washing with ethanol and water were dried at 110 ℃ and then calcined in the air at 600 ℃ for 4 h. Finally, the obtained precipitates were further calcined under ammonia atmosphere with nitrogen purging (10%, N2 as the carrier gas, the tube furnace is connected with a washing bottle filled with ammonia) at 700 ℃ for 4 h to constitute a defect low valent Fe-V bimetallic catalyst.
For pollutant degradation, all bath experiments were conducted with 150 mL target pollutant solution. The reaction was initiated by adding predetermined amounts of catalysts and PMS. The solution temperature was adjusted at 30 ± 1 ℃ by using water batch. At the predetermined time, certain volume of reaction solution was filtered via a 0.22 µm PTFE syringe filter discs and mixed with 20 µL Na2S2O3 before analysis. Details about the characterization and analytic methods could be seen in Text S2 (Supporting information).
X-ray diffraction (XRD) spectrum suggests that the distinct diffraction peaks of FeVO3-x are indexed to (104), (311), (110), and (116) planes, and the crystal phases of pristine FeVO3-x particles are assigned to γ-Fe2O3 and V2O3 (Fig. 1a), indicating low valent V species exist in FeVO3-x. The vibrating sample magnetometer (VSM) results shows the saturation magnetization of FeVO3-x is ~3 emu/g (Fig. 1b), which might originate from the ferromagnetism of γ-Fe2O3. As shown in Fig. 1c, the fresh FeVO3-x particles are micron-sized and exhibit a unique brain-like morphology with wrinkled surface, which would facilitate the adhesion of PMS in the vicinity of FeVO3-x. Accordingly, the mappings of Fe, V, O species (Figs. 1d-f) show that only Fe and V species are uniformly distributed on FeVO3-x, indicating enriched oxygen vacancy was created on the surface of FeVO3-x. Moreover, since the photoluminescence (PL) emission peak at 450 nm is correlated with the electron transition from shallow level to the top of the valence band, the existence of oxygen vacancy in the FeVO3-x is also verified by PL spectrum (Fig. S1 in Supporting information) [17]. In addition, the N2 adsorption-desorption results (Fig. S2 in Supporting information) manifest that the surface area of fresh FeVO3-x is 1.1 m2/g, suggesting the poor pollutant adsorption ability of FeVO3-x.
The performance of FeVO3-x/PMS system was compared with several systems, including FeO/PMS, Fe3O4/PMS, Fe2O3/PMS, V2O3/PMS, V2O4/PMS, FeVO3-x alone and PMS alone systems. Results shown in Fig. 2a and Fig. S3 (Supporting information) suggest that PMS in the absence of catalyst cannot oxide CBZ, and FeVO3-x has no adsorption effect on CBZ, indicating CBZ was degraded by the generated ROS in the FeVO3-x/PMS system. In addition, the CBZ degradation efficiency in the FeVO3-x/PMS system within 10 min treatment is much higher (100%) than those in other systems (6%−36%), implying FeVO3-x can effectively activate PMS to generate substantial ROS for CBZ degradation.
The electron paramagnetic resonance (EPR) test using 5,5-dimethyl-1-pyrroline N-oxide (DMPO) as the in situ radical spin-trapping reagent was conducted to qualitatively analyze the existence of the main ROS in the FeVO3-x/PMS system. In contrast to PMS alone and FeVO3-x alone systems (Fig. 2b), two signals appearing in the FeVO3-x/PMS system are assigned to DMPO-HO adduct (four characteristic peaks with height ratio of 1:2:2:1, αN = αH = 14.9 G) and DMPO-SO4 adduct (αN = 13.8 G, αH = 10.1 G, αH = 1.4 G, and αH = 0.8 G) [18-20], implying both hydroxyl radicals (•OH) and sulfate radicals (SO4•−) were generated in the FeVO3-x/PMS system. However, since DMPO-SO4 adduct is easily converted into DMPO-HO adduct [21], the signal intensity of DMPO-SO4 adduct is weak in the FeVO3-x/PMS system. To further disclose the identity of •OH and SO4•− in the FeVO3-x/PMS system, tert-butyl alcohol (TBA) was introduced for •OH quenching (kTBA/SO4•−: 4.0–9.1 × 105 L mol−1 s−1, kTBA/•OH: 3.8–7.6 × 108 L mol−1 s−1) [22-24], and ethanol (EtOH) was introduced for both •OH and SO4•− quenching (kEtOH/SO4•−: 1.6 × 107 L mol−1 s−1, kEtOH/•OH: 1.9 × 109 L mol−1 s−1) [22]. Fig. 2c suggests that the quenching effects of EtOH increase as a function of concentration (50-200 mmol/L), while TBA has a feeble quenching effect on CBZ degradation regardless of the concentration (50-200 mmol/L). Besides, the semi-quantitative analysis of •OH in the FeVO3-x/PMS system were conducted with the terephthalic acid (TPA), since 2-hydroxyterephthalic acid (HTPA) as the characteristic product can be produced after the attack of •OH [25]. Surprisingly, we found that the degradation trend of CBZ in the FeVO3-x/PMS system was similar to that in the classic co-catalytic Fenton system (hydroxylamine/Fenton, Fig. S4a in Supporting information). The ROS in the hydroxylamine/Fenton system are undoubtedly •OH. Therefore, the contribution of •OH and SO4•− formed in the FeVO3-x/PMS system can be better investigated by comparing with the hydroxylamine/Fenton system. Clearly, the generation concentration of HTPA in the FeVO3-x/PMS system was much lower (Fig. S4b in Supporting information) when the degradation trend of CBZ in the FeVO3-x/PMS system was similar to that in the classic co-catalytic Fenton system (hydroxylamine/Fenton). The collective results indicate that though both •OH and SO4•− are generated in the FeVO3-x/PMS system, the amounts of SO4•− are much more than that of •OH.
Since some studies pointed out that high-valent iron-oxo species (Fe(Ⅳ)) might be produced in the Fe mediated Fenton-like systems and the reaction rate between Fe(Ⅳ) and ethanol (kEtOH/Fe(Ⅳ): 2.51 × 103 L mol−1 s−1) is obviously faster than that between Fe(Ⅳ) and TBA (kEtOH/Fe(Ⅳ): 6 × 101 L mol−1 s−1) [19,26,27], the existence of Fe(Ⅳ) in FeVO3-x/PMS system was further qualitatively analyzed by the chemical probe method. Methyl phenyl sulfoxide (PMSO) was applied as a chemical probe because the reaction between PMSO with Fe(Ⅳ) proceeds through an oxygen atom transfer and methyl phenyl sulfone (PMSO2) is quantitatively generated [27]. From the HPLC chromatograms, it is obvious that the concentration of PMSO was decreased while PMSO2 was accumulated in the FeVO3-x/PMS system (Fig. 2d). We further quantified the concentrations of PMSO2 and PMSO to confirm the existence of Fe(Ⅳ). Results show that conversion efficiency of PMSO to PMSO2 is 68.2% (Fig. 2e), implying the role of Fe(Ⅳ) in the FeVO3-x/PMS system for CBZ degradation cannot be ignored. Moreover, some researchers argued that high-valent iron-oxo species might induce the production of O2•− [28,29]. Therefore, EPR test was conducted with DMPO in the dimethyl sulfoxide (DMSO) solution to identify the existence of O2•−. The EPR spectrum with hyperfine splitting parameters of αH = 14.25 G, αN = 12.45 G, and an intensity ratio of 1:1:1:1 is indexed to DMPO-O2 adduct (Fig. 2f) [30], indicating high-valent iron-oxo species reacting with PMS induces the formation of O2•−. Combined with the results of quenching experiment, although O2•− is produced in the FeVO3-x/PMS system, O2•− has a negligible effect on CBZ degradation.
To further elucidate the generation of ROS in the FeVO3-x/PMS system, the chemical compositions of FeVO3-x were scrutinized by XPS analysis. The spectra of Fe 2p core level in the pristine and reacted FeVO3-x show that the ratio of Fe(Ⅲ) to Fe(Ⅱ) is nearly invariable Figs. 3a and b), indicating the generated Fe(Ⅲ) induced by the reaction between PMS and Fe(Ⅱ) can be quickly reduced during treatment process. In contrast with the chemical state of Fe, pronounced changes occurred in the V species after the final reaction (Figs. 3c and d), where a new peak located at 517.20 eV assigned to V(Ⅴ) [31,32] was found. The oxidation of V species in the FeVO3-x/PMS system follows two pathways: (ⅰ) low valent V species (V(Ⅲ) and V(Ⅳ)) react with PMS (HSO5−) to generate V(Ⅴ) (Eqs. 1 and 2); (ⅱ) low valent V species as electron donators transfer electrons to Fe(Ⅲ) for fast Fe(Ⅱ) regeneration and finally convert to V(Ⅴ) (Eqs. 3 and 4). The first pathway is confirmed by Fig. 2a since 32% and 25% CBZ can be degraded in the V2O3/PMS and V2O4/PMS systems, respectively. The second pathway of low valent V species for Fe(Ⅲ) reduction is further scrutinized in the following content. In addition, compared with fresh FeVO3-x, the decrease of oxygen vacancy in the used FeVO3-x (Figs. 3e and f) also verifies that oxygen vacancy participated in the CBZ degradation.
To further investigate the role of low valent V species for Fe(Ⅲ) reduction, the electronic structure and coordination environment of Fe and V species in the FeVO3-x, along with some other Fe and V-based oxides (FeO, Fe3O4, Fe2O3, V2O5, V2O4, and V2O3 standards) were evaluated by X-ray absorption spectroscopy (XAS). E0 was calculated as the maximum peak energy of the first derivative of the spectrum, which was used to identify the Fe oxidation state of different materials. According to the Fe K-edge X-ray absorption near edge structure (XANES) of FeVO3-x and other Fe-based oxides (Fig. 4a), the value (7112.2 eV) of E0 in FeO spectrum is lowest, while in Fe2O3 spectrum is highest (7114.1 eV), indicating E0 in Fe K-edge XANES spectrum increases as a function of chemical valence of Fe. Since the value (7112.7 eV) of E0 in the FeVO3-x is between that of FeO and Fe2O3, both Fe(Ⅱ) and Fe(Ⅲ) exist in the FeVO3-x. However, only Fe(Ⅲ) exists in the FeVO3-x precursor because its E0 is the same as that of Fe2O3. In addition, in contrast with Fe3O4, the pre-edge peak intensity of FeVO3-x is weaker than that of Fe3O4, implying the amount of Fe(Ⅱ) in the FeVO3-x is more than that of in the Fe3O4, since the 3d orbital of Fe(Ⅱ) possesses less electron number than that of Fe(Ⅲ), and the pre-edge peak represents the 1s → 3d electron transition [33].
As for the valence of V, the FeVO3-x precursor, V2O5, V2O4, and V2O3 standards have a pre-edge peak with prominent intensity, which drastically increases with V species oxidation states (Fig. 4b). However, the pre-edge peak pattern of FeVO3-x is in remarkable contrast to those of other V-based materials. Since the symmetry of the V species in FeVO3-x differs from FeVO3-x precursor, V2O3, V2O4, and V2O5, the oxidation states of V species in the FeVO3-x cannot be defined only by the pre-edge peak intensity. On the other hand, the V K-edge XANES spectrum of FeVO3-x is in line with the literature reports [4,34], indicating the oxidation state of V species in the FeVO3-x is trivalent and tetravalent.
The Fourier-transformed (FT) extended X-ray absorption fine structures of Fe K-edge (EXAFS k3χ(k)) are shown in Fig. 4c. The peak at ~1.5 Å (without phase correction) can be identified as Fe-O bond. Comparing FeVO3-x precursor versus FeVO3-x, the peak at ~1.5 Å shifts to much lower intensity in FeVO3-x (Fig. 4c), suggesting the coordination number decreases in FeVO3-x, which further well-documents the existence of oxygen vacancies. Since the FT curves of V K-edge EXAFS k3χ(k) functions (Fig. 4d) are more complicated than that of Fe K-edge EXAFS k3χ(k), the fitting curves of FeVO3-x compared with FeVO3-x precursor and V foil are shown in Fig. 4e,Fig. 4f and Table S1 (Supporting information). The well-resolved peaks at ~1.4 Å and ~3.0 Å (without phase correction) in FeVO3-x and FeVO3-x precursor are indexed to V-O bond and V−O−Fe bond, respectively. The coordination numbers of V-O and V−O−Fe shells in the FeVO3-x are 3.0 and 0.6, which is in marked contrast to that of in the FeVO3-x precursor (5.6 and 3.0, respectively, Table S1), also indicating the existence of existence of oxygen vacancies. Moreover, the wavelet transform plots (Fig. 4g) of FeVO3-x and FeVO3-x precursor also reflect the existence of V-O and V−O−Fe bonds. The existence of V−O−Fe bond facilitates the interpretation of the interelectronic interaction of Fe and V species in FeVO3-x. Specifically, the electron-riched t2g d-orbitals of V species donating electrons to the electron-deficient t2g d-orbitals of Fe(Ⅲ) species through the bridging O2− via π-donation [4]. Moreover, CBZ degradation and Fe(Ⅱ) generation after external addition of Fe(Ⅲ) into V2O4/PMS and V2O3/PMS systems (Fig. S5 in Supporting information) also imply low-valent V species as electron-rich promoters mediate electron shuttles to expedite Fe(Ⅲ) reduction and pollutant degradation. To further confirm the interaction of oxygen vacancy and PMS molecules, we further conducted in-situ Raman spectroscopy analysis. The in situ Raman spectroscopy shows that the peak intensities of FeVO3-x at 146, 286, and 703 cm−1 increase after adding PMS (Fig. S6 in Supporting information), indicating peroxo species bound to the surface oxygen vacancies might be formed [17].
Previous studies suggested that co-existing anions in water might react with •OH and SO4•− (Eqs. 5-12) [35-37]. Therefore, the effects of different anions, such as Cl−, H2PO4−, NO3− and HCO3−, on CBZ degradation in the FeVO3-x/PMS system were investigated. From Fig. 5a, it is clear that the common anions, such as Cl−, H2PO4− and NO3− in natural water almost show negligible effects on CBZ degradation, which suggests the great matrix resistance of this system. The obvious inhibition of CBZ degradation in the presence of HCO3− might originate from the considerable alkalinity induced by the introduction of HCO3−. However, in actual water samples such as tap water, Jinjiang water and Jiangan water, the degradation performance severely decreased (Fig. 5b). This might be ascribed to the pH buffer effects of natural water samples and the presence of natural organic matters, which could severely compete with target contaminants for oxidative ROS. Finally, the system exhibited satisfactory cyclic performance during consecutive runs (Fig. 5c). Despite a little decrease of CBZ removal from 100% to 80%, a facile N2 or NH3 regeneration could effectively restore the reactivity of used FeVO3-x and ensure the long-term stability.
Based on the detected seven intermediates, we proposed the possible degradation pathway of CBZ in the FeVO3-x/PMS system (Fig. 6a, Table S2 and Figs. S7-S14 in Supporting information). First, the olefinic unsaturated bond of central heterocyclic ring is readily attacked [4,38], and thus P1 (m/z = 251.0821) and P2 (m/z = 269.0922) are formed owing to the attack of SO4•−, •OH and Fe(Ⅳ). P2 is then oxidized to P5 (m/z = 267.0772) via intramolecular cyclisation and carboxylation reactions. In addition, the dialdehyde moieties of P2 are unstable, which leads to the rotation of benzene ring of P2 to generate P6 (m/z = 267.0774). The aldehyde moiety on the P6 can be further oxidized by the ROS to form a carboxylic acid product (P7, m/z = 283.0723). Subsequently, P7 could be oxidized to form P4 (m/z = 196.0766) via deamination, acrylamido abstraction, and decarboxylation reactions. Moreover, P1 can also be oxidized to generate P3 (m/z = 180.0813) via intramolecular cyclisation, amine/acrylamido cleavage and de-formyl, which further be oxidized to produce P4. Finally, these detected intermediates are mineralized to CO2 and H2O. Specifically, the TOC removal drastically increased with treatment time (Fig. S15 in Supporting information): the TOC removal reached 17% after 10 min treatment, while it increased to 55% after 120 min treatment.
Furthermore, we also evaluated the developmental toxicity, acute toxicity, bioaccumulation factor and mutagenicity of original CBZ and its intermediates through the Toxicity Estimation Software Tool. Fig. 6b shows the oral rat LD50 of P1 and P5 are 213.16 and 287.73 mg/kg, respectively, which are much lower than that of CBZ (1636.63 mg/kg), implying the acute toxicities of P1 and P5 are quite more toxic than original CBZ. However, the acute toxicities of most types of intermediates are much lower than CBZ. Since the potential hazards of these intermediates are negative correlation with bioaccumulation factor, and Fig. 6c shows the bioaccumulation factors of P2, P5, P6, P7 (9.56, 7.41, 19.70, and 4.98, respectively) are much lower than that of CBZ (27.38), four intermediates have quite lower risks than CBZ. However, the results of developmental toxicity (Fig. 6d) and mutagenicity (Fig. 6e) suggest that five developmental toxicants (P1, P2, P5, P6 and P7) and five mutagenicity negative intermediates (P1, P3, P4, P5 and P7) are generated after treatment process.
In this work, we synthesized a novel catalysts FeVO3-x via a facile ammonia reduction method. The high-temperature reduction process endowed the catalysts with abundant low-valent V species and electron-rich oxygen vacancy, which are both conducive to the circulation of Fe(Ⅲ) to Fe(Ⅱ). Through quenching experiments and EPR analysis, we found that •OH, SO4•−, O2•− and Fe(Ⅳ) were all generated in this system, but only SO4•− and Fe(Ⅳ) primarily contributed to the degradation of CBZ. X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy indicated that both the low-valent V provides and oxygen vacancy could accelerate the internal electron transfer to Fe(Ⅲ) via the unsaturated V−O−Fe bond. Despite a little decrease of performance after consecutive runs, the activity could be effectively regenerated via re-calcination treatment. Finally, the degradation product and the corresponding toxicity analysis revealed that this system is basically a toxicity attenuation process, demonstrating its potential in practical application.
Declaration of competing interest
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The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
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The first author is funded by the Shanghai Tongji Gao Tingyao Environmental Science & Technology Development Foundation. Additionally, the authors acknowledge the staff at beamline 1WB at the Beijing Synchronic Radiation Facility (BSRF) for their assistance during the XAS measurements. And the authors would like to acknowledge the financial support from National Natural Science Foundation of China (Nos. 52070133, 2022NSFSC0972), Sichuan Science and Technology Program: Key Research and Development Program (Nos. 2019YFG0314, 2017SZ0180 and 2019YFG0324).
Supplementary materials
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Supplementary material associated with this article can be found, in the online version, at doi:10.1016/j.cclet.2023.108580.
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doi: 10.1016/j.cclet.2023.108580
  • Receive Date：2023-01-31
  • Online Date：2025-11-20
  • Published：2024-01-15
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  • Received：2023-01-31
  • Revised：2023-04-27
  • Accepted：2023-05-16
Affiliations
    aState Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China
    bSino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
    cChengdu Baixi Environmental Technology Company, Chengdu 610065, China
    dInstitute of Environmental Engineering, RWTH Aachen University, Germany
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表12种不同金属材料的力学参数
科
Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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