Water Cycle
·
2024
·
IF 0
Guoting Li,Haozhe Li,Shude Zhang,Xiao Mi,Yujie Guo,Zhixin Song,Yuhao Liu,Hongwei Pan,Baogui Wang,Yingxu Liu,Weigao Zhao,Tannaz Pak
Mn oxides are confined within the porous structure of activated coke (ACO) via impregnation followed by calcination treatment. The Mn-ACO sample calcined at 600°C (Mn-ACO600) demonstrated superior performance despite containing only a minute atomic ratio of 0.11% Mn on its surface. This treatment led to a slight increase in the specific surface area and pore volume of ACO, with a significant enhancement in the proportion of micropores, rising from 54.2% in ACO to 71.8% in Mn-ACO600. Raman spectroscopy indicated additional defects in Mn-ACO, while XPS analysis confirmed the coexistence of Mn(II), Mn(III), and Mn(IV) oxides. Although ACO adsorption alone was ineffective in removing acesulfame (ACE), Mn-ACO600 achieved a removal rate of 19.0%. The introduction of peroxydisulfate (PDS) further boosted the degradation of Mn-ACO600, with a K app value that was 2.28 times of that of the combined Mn-ACO600 adsorption and PDS oxidation process, indicating a remarkable synergistic effect. To optimize the experimental conditions, a response surface methodology design analysis was conducted, revealing that solution pH and the dosage of Mn-ACO600 were crucial factors. Furthermore, the study confirmed non-radical oxidizing species, such as 1 O 2 and h + , played a predominant role in the process, with relatively minor contributions from radical oxidizing species.
研究领域:
环境科学
·
材料化学
·
化学工程
✓ 已验证
DOI
CATALYSIS LETTERS
·
2023
·Vol. 154
·期 5
·2182-2196
·
IF 2.8
Liu Jialu,Song Zhi,Liu Boxia,Zhang Xiayan,Huang Yeqiong,Han Dongxu
Because of its high toxicity and severe degradation, phenol has caused serious environmental pollution, and it is urgent to explore a stable and efficient degradation method of phenol. In this study, Ni/Fe bimetallic atomic cluster composite catalyst activated peroxymonosulfate (PMS) to degrade phenol efficiently. The experimental results show that the phenol degradation rate can reach 100% in a wide range of pH (3–11), and the system offers good stability in repeated experiments. The free radical quenching investigation and electrochemical characterization showed that the non-free radical pathway dominated the degradation system, and a large amount of singlet oxygen and rapid electron transfer promoted the efficient degradation of phenol in wastewater. This study opens up a new way for bimetallic atom cluster catalysts to activate PMS to degrade organic pollutants. Graphical
研究领域:
环境科学
·
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
Frontiers of Materials Science
·
2025
·Vol. 19
·期 3
·1-16
·
IF 2.3
Li Yumei,Deng Bingqian,Wang Jiexin,Li Jialong,An Wenbin,Fan Jian,Sun Peng
A molybdenum (Mo)-modified LaFeO 3 (LFMO) perovskite catalyst was synthesized to activate peroxymonosulfate (PMS) for the degradation of indole in solution. The catalyst was characterized by XRD, SEM, and XPS. Results indicate that LFMO possesses a higher specific surface area and more catalytic active sites compared to unmodified LaFeO 3 . XPS analysis reveals that the activation of PMS is mediated by Fe 2+ /Fe 3+ and Mo 4+ /Mo 6+ reduction–oxidation cycles. Oxygen vacancies generated by molybdenum substitution serve as reaction sites, which accelerate the dissociation of PMS and the production of reactive oxygen species. Chemical quenching experiments and EPR spectroscopic analyses were employed to elucidate the mechanism, highlighting the significant role of non-radical species in the removal of indole. Under optimal reaction conditions, the degradation efficiency of indole reached 90.53% within 30 min, demonstrating strong anti-interference against inorganic anions and natural organic matter. LFMO particles exhibit sustained catalytic activity and stability over five consecutive cycles. This LFMO/PMS system provides valuable insights for the development of non-radical degradation pathways based on PMS.
研究领域:
环境化学
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催化科学
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材料化学
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环境污染控制
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高级氧化过程
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xuefeng Liu,Shijie You,Nanqi Ren,Hao Zhou,Jinna Zhang
This study reports the development of complete solar-driven dual-photoelectrode fuel cell (PFC) based on WO 3 photoanode and Cu 2 O photocathode with peroxymonosulfate (PMS) serving as cathodic electron acceptor . As indicated by photoelectrochemical measurements, the PMS was able to improve thermodynamic properties of photocathode, achieving an increased open circuit potential from 0.42 V to 0.65 V vs standard hydrogen electrode (SHE). Under simulated sunlight irradiation (~100 mW cm −2 ), the maximum power density of 0.12 mW cm −2 could be obtained at current density of 0.34 mA cm −2 , which was 8.57 times of that produced by PFC without PMS (0.014 mW cm −2 ). Correspondingly, adding PMS (1.0 mM) increased overall removal efficiency of 4-chlorophenol (4-CP) from 39.8% to 96.8%, accounting for the first-order kinetic constant ( k =0.056 min −1 ) being 6.67 times of that in the absence of PMS ( k =0.0084 min −1 ). Radical quenching and electron spin-resonance (ESR) results suggested the contribution of free radicals (•OH and SO 4 •- ) and non-radical pathway associated with direct activation of PMS by Cu 2 O photocathode. Fourier transformed infrared (FTIR) analysis confirmed the strong non-radical interaction between Cu 2 O photocathode and PMS, resulting in 4-CP removal via activation of PMS by surface complex on Cu 2 O. The proof-in-concept complete solar-driven dual-photoelectrode fuel cell may offer an effective manner to realize water purification and power generation, making wastewater treatment more economical and more sustainable.
研究领域:
环境科学
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光催化
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能源材料
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电化学
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水处理技术
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可持续能源
✓ 已验证
DOI
高影响因子
NANO
·
2024
·
IF 1
Sai Wang,En-Ni Wu,Liang Meng,Zhen-Jun Wang,Tuan-Tuan Wang
To improve the activation efficiency of PMS to efficiently degrade antibiotic sulfadiazine (SD), herein, a Co@MoS 2 catalyst was prepared by a one-step hydrothermal process. The unique petal-like structure of MoS 2 enables the transition metal Co to achieve high dispersion and avoid agglomeration. Mo(IV) and unsaturated S accelerate the electron transfer between Co 2 + and Co 3 + to improve the cycling efficiency and thus realize the efficient activation of PMS. The results of active substance quenching experiment and ESR analysis show that the main active substance for the efficient degradation of SD by Co@MoS 2 is the non-radical 1 O 2 , while the other three radicals ⋅ O − 2 , ⋅OH and SO • − 4 contribute significantly to the efficient degradation of SD. And after 5 cycles, the degradation could still be as high as 90%. The strong consolidation of Co on the petal-shaped sheet of MoS 2 ensures the stability of Co@MoS 2 catalyst.
研究领域:
环境科学
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催化
·
纳米技术
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xin Mao,Zhaoyan Deng,Yiming Liu,Haiyang Xie,Qian He,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Ultra-small metal clusters have emerged as one of the most promising alternatives to heterogeneous Fenton-like catalysts. Despite the high atom utilization and structural stability of catalysts with ultra-small clusters and single-atom sites, there is still challenging for the synthesis of these catalysts due to their facile aggregation. Herein, we successfully fabricated a catalyst (Fe-NC-900) with single-atom sites and ultra-small clusters by a ball milling method combined with subsequent pyrolysis process. Fe-NC-900 showed high efficiency and superior stability in the activation of peroxymonosulfate (PMS) for catalytic oxidation of refractory organic compounds. Chemical quenching experiments, electron paramagnetic resonance (EPR), in-situ Raman spectra, and electrochemical analysis indicated that the 1 O 2 oxidation was the main non-radical pathway rather than the high-valent iron oxidation and electron transfer mechanism for the degradation of RhB in the Fe-NC-900/PMS system. This work provides useful insights into the design and synthesis of the catalysts with single atoms and ultra-small clusters for practical applications in Fenton-like catalytic processes.
研究领域:
环境催化
·
材料化学
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纳米环境技术
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高级氧化过程
·
污染物降解
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chen Zhang,Haohao Wu,Fangqin Cheng,Jianfeng Li
Nonradical advanced oxidation has a distinctive excellent selectivity and reactivity. The fine-tuned O/N basic functional groups play a distinguishing role in the occurrence of nonradical pathways. However, it remains debatable regarding the principal basic species and their contribution. Consequently, identification of preferred basic sites and the correlation with the triggered activation mechanism need to be further clarified. In this study, the hydrothermal and thermal annealing method were adopted to construct heterogeneous basic sites on three-dimensional graphene (3D GN), and the activity of peroxydisulfate (PDS) activation was systematically assessed by humic acid(HA)abatement. Herein, the significantly improved catalytic capability (up to 80 %) of 3D GN-NH 3 ⋅H 2 O was acquired, more than 2 times compared to that of 3D GN-NH 3 . The added I D/I G value of 3D GN-NH 3 ⋅H 2 O from 1.05 of 3D GN to 1.08 indicated that it is less graphitized and has more structural defects. Notably, the hydrothermal modification of NH 3 ⋅H 2 O enhanced both the basic oxygen and nitrogen groups (C = O/pyrrolic-N, pyridine-N). A positive correlation was displayed between the integrated basic sites ratio (34.2–71.7 %) and reaction rate (0.169–0.442 min −1 ) based on quantitative calculation. Moreover, the increased content of basic sites and defective sites on 3D GN-NH 3 ⋅H 2 O was responsible for the hydrophobic interaction and 1 O 2 generated in nonradical pathways. The most reactive basic site is the pyrrolic-N which was illustrated by density functional theory (DFT) calculations. Furthermore, a possibly involved nonradical activation mechanism of 3D GNs/PDS was explored. The challenges and prospects of PDS advanced oxidation activated by carbon catalyst are evaluated. This work provides insights into a facile protocol for engineering a carbon catalyst to drive efficient PDS activation in the remediation of water environmental pollutants.
研究领域:
环境化学
·
材料科学
·
催化化学
·
水污染治理
·
碳材料
·
高级氧化技术
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2024
·Vol. 46
·期 2
·1-19
·
IF 3.2
Yu Weiwei,Li Yueqi,Shu Minghui,Liu Cong,Liang Yue,Mao Yufeng,Tan JiangLin,Liu Yang,Ai Ting
Tetracycline becomes a crucial measure for managing and treating communicable diseases in both human and animal sectors due to its beneficial antibacterial properties and cost-effectiveness. However, it is important not to trivialize the associated concerns of environmental contamination following the antibiotic's application. In this study, cobalt ferrate (CoFe 2 O 4 ) nanoparticles were loaded into chitosan (CS), which can avoid the agglomeration problem caused by high surface energy and thus improve the catalytic performance of cobalt ferrate. And it can avoid the problem of secondary contamination caused by the massive leaching of metal ions. The resulting product was used as a catalyst to activate peroxymonosulfate (PMS) for the degradation of tetracycline (TC). To determine the potential effects on TC degradation, various factors such as PMS dosing, catalyst dosing, TC concentration, initial solution pH, temperature, and inorganic anions (Cl − , H 2 PO 4 − and HCO 3 − ) were investigated. The CS/CoFe 2 O 4 /PMS system exhibited superior performance compared to the CoFe 2 O 4 -catalyzed PMS system alone, achieving a 92.75% TC removal within 120 min. The catalyst displayed high stability during the recycling process, with the efficiency observed after five uses remaining at a stable 73.1%, and only minor leaching of dissolved metal ions from the catalyst. This confirms the high stability of the catalyst. The activation mechanism study showed that there are free radical and non-free radical pathways in the reaction system to degrade TC together, and SO 4 •− and 1 O 2 are the primary reactive oxygen radicals involved in the reaction, allowing for effective treatment of contaminated water by TC.
研究领域:
环境科学
·
材料科学
·
催化
·
纳米技术
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）