SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Guanglan Di,Yuwen Wei,Jiaowei Ding,Yu Zhang,Zefang Chen,Xuede Li,Xiangwei Wu,Xiaoli Zhao
Modulating excitonic effects enables the selective activation of O 2 to singlet oxygen ( 1 O 2 ) for efficient degradation of emerging contaminants (ECs) in complex environmental systems. However, the lack of mechanistic investigation in excitonic effect modulation hinders the efficient O 2 activation towards generating preferred reactive oxygen species (ROS). Taking 2D BiOCl as a prototype, we herein propose a facile aluminum (Al) doping method to enhance the inherent excitonic effects of defective BiOCl (BiOCl OV ) and tailor the O 2 activation pathway for 1 O 2 generation. The Al dopants and surface oxygen vacancies (OVs) cooperatively promote O 2 activation, where OVs mainly promote O 2 absorption while Al mainly promote O 2 activation. A new mechanism for 1 O 2 generation driven by a strong excitonic effect has been proposed via experiments and theoretical investigations. Benefiting from the Al-mediated trapping state for singlet exciton, the intersystem crossing is promoted from singlet excitons to triplet excitons because of a lower singlet–triplet energy gap, thereby leading to a selective activation of O 2 to 1 O 2 by resonance energy transfer between triplet excitons and surface absorbed O 2 . Consequently, Al-doped BiOCl OV exhibits a superior activity and stability toward typical ECs degradation in both simulated and real water matrices. This study elucidates the role of the excitonic effect in selectively activating O 2 to 1 O 2 , offering valuable insights for the optimization of exciton-based photocatalysis through atomic-scale design strategies.
研究领域:
环境科学
·
光催化材料
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Haidong Luo,Shuai Dong,Suhang Chen,Fengqi Zhao,Kangzhen Xu
Photocatalytic-Fenton synergistic degradation of pollutants in wastewater is considered a promising technology for environmental treatment. Herein, FeOOH quantum dots decorated La-doped Bi 4 O 5 I 2 hybrids were prepared using an in-situ deposition strategy and applied for the removal of 2,4-dinitrophenylhydrazine. The FeOOH-1/La 10 -Bi 4 O 5 I 2 sample exhibits the highest catalytic activity in degradation experiments, eliminating 93.8 % of 2,4-dinitrophenylhydrazine within 30 min at a reaction rate constant of 0.117 min −1 . In addition, the impacts of several operational parameters on the catalytic activity were comprehensively examined, including H 2 O 2 concentration, catalyst dosage, reaction solution pH and co-existing ions. In degradation process of 2,4-dinitrophenylhydrazine, the major reactive oxygen species are ·OH and ·O 2 – , with ·OH generated by Fenton reaction. Optical property characterization, cyclic voltammetry tests, and photoelectrochemical measurements confirmed that the FeOOH-1/La 10 -Bi 4 O 5 I 2 composite has excellent light absorption capacity, abundant active centers, and excellent carrier separation efficiency. Finally, the degradation mechanism of FeOOH-1/La 10 -Bi 4 O 5 I 2 composites for 2,4-dinitrophenylhydrazine is rationally discussed based on experimental and theoretical calculations. This study presents a fresh design idea for developing bismuth oxyhalide-based composites with high activity.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Daniel T. Oyekunle,Beibei Wu,Fang Luo,Jawad Ali,Zhuqi Chen
Co-anchored on N doped graphitized carbon material (Gc-N-Co) was synthesized using glucose and melamine as carbon and nitrogen source, respectively. The prepared Gc-N-Co demonstrate a higher removal efficiency and PMS (peroxymonosulfate) decomposition compared to other control catalyst of Gc-N and Gc-Co, implying a synergistic effect between the precursor materials. The high performance was attributed to the co-ordination between the pyridinic N and Co forming N-Co bonds on the catalyst surface capable of degrading a wide range of organic contaminants (ciprofloxacin, carbamazepine, sulfamethoxazole, and 4-chlorophenol). Surface-bound (SO 4 •− ) radical was established as the dominant mechanism of the reaction process based on the quenching experiments and EPR tests. The activation energy (E a ) of 26.4 kJ/mol further established that an intrinsic chemical reaction takes place on the catalyst surface rather than in solution. Also, the electrostatic attraction observed at neutral pH validates the surface interaction between the surface-bound SO 4 •- radical and the organic molecules. The negative influence of inorganic ions followed the order of SO 4 2- > Cl - > NO 3 - , and the positive effect of HCO 3 – was discussed. In addition, Gc-N-Co demonstrate excellent reusability in four consecutive cycles consolidating on the presence of the strong N-Co bonds.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Aimal Khan,Kaikai Zhang,A Taraqqi-A-Kamal,Xiaoguang Wang,Yong Chen,Yanrong Zhang
ε-MnO 2 effectively activates peroxymonosulfate (PMS) for the efficient degradation of emerging pollutants. ε-MnO 2 was synthesized by a facile thermal-treatment method and its long-term stability and efficiency for the elimination of emerging pollutants, including sulfamethoxazole (SMX), sulfachloropyridazine (SCP), sulfamethazine (SMT), ciprofloxacin (CIP), and azithromycin (AZI), from aqueous media were evaluated. ε-MnO 2 was found to activate PMS more efficiently than α-MnO 2 , β-MnO 2 , or δ-MnO 2 , owing to its high − OH-group content, unique structure, and high surface area. Sulfate (SO 4 •− ), hydroxyl (•OH), and superoxide (O 2 •− ) radicals, as well as singlet oxygen ( 1 O 2 ) were generated, with O 2 •− acting as the 1 O 2 precursor. The ε-MnO 2 /PMS system proved to be effective in the pH range of 3.5–9.0 and the rate of SMX degradation was not significantly affected by the presence of inorganic anions or natural organic matter. The proposed pathway for the activation of PMS by ε-MnO 2 includes inner-sphere interactions between ε-MnO 2 and PMS, and electron transfer to PMS via the MnIII ↔ MnIV redox cycle, which generates reactive oxygen species. These findings provide new insight into PMS activation by less-toxic metal oxides as catalysts and demonstrate that Mn-based materials can be used to effectively treat water matrices containing emerging pollutants.
研究领域:
环境科学
·
催化材料
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bingheng Liang,Xiaoya Gao,Qingcun Gu,Xuhao Liu,Teng Guo,Jiatian Wang,Wenjie Zhu,Yongming Luo
Increasing number of spent lithium-ion batteries (LIBs) presents opportunities and challenges for the recycling of cathode LiCoO 2 (LCO). Here, simultaneously selective leaching Li and fabricating cobalt oxide catalyst was developed by autocatalytic Peroxymonosulfate (PMS) advanced oxidation method at ambient temperature without strong acids. Where, superoxide radical ( O 2 · - ) was generated to break Li-O leaching 96.6 % of Li, and induced part conversion of Co 3+ to Co 2+ forming oxygen vacancies (O V ) in the remaining Co-containing product (NLCO). Compared with LCO (without delithiation), NLCO promoted greater electron transfer to activate PMS producing radical ( SO 4 · - and •OH) and non-radical ( 1 O 2 and Co(Ⅳ)=O) in the degradation of emerging pollutants (carbamazepine, CBZ). Hence, the NLCO/PMS system was effective in removing CBZ with resistance to pH variation and water matrix interference ( SO 4 2- , NO 3 - , and HA). COHP calculation results revealed the strong and almost unbreakable Co-O in NLCO, with significantly low Co leaching ensuring the excellent stability (100 % degradation activity maintained after 7th cycling) for removing pollutants in the liquid-phase reaction. Degradation pathways and toxicity analysis elucidated that the NLCO/PMS was a green and toxicity reduction process for removing CBZ. This study showcased a novel method for recovering Li from spent LCO and subsequently producing an environmental catalyst form spent LIBs.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Applied Materials Today
·
2020
·
IF 8.352
Ying Zhang,Jing Gao,Xin Xin,Lihui Wang,Heyu Li,Xiaobing Zheng,Yanjun Jiang
The successful combination of enzymes and photocatalysts in one pot is an elegant approach for the reactions with high efficiency. This combination usually requires both enzymes and photocatalysts with reasonable activity under the same condition. Herein, a photo-enzyme integrated catalyst by immobilizing laccase on clustered porous TiO 2 heterophase junction (HPJs) microsphere (denoted as mTiO 2 -CVs) is synthesized for the first time. The TiO 2 microsphere with ordered regular radial structure and controllable heterophase junction (anatase/rutile) composition is prepared by a pressure-driven hydrothermal assembly method. The ratio of rutile and anatase phase of mTiO 2 -CVs can be controlled by adjusting the amount of hydrochloric acid in the preparing process. The characterization results of mTiO 2 -CVs prove that the mTiO 2 -CVs has regular morphology, uniform mesoporous structure, larger specific surface area and narrower band gap, and can realize the effective utilization of visible light. After immobilizing laccase on mTiO 2 -CVs by adsorption method, the integrated catalyst (mTiO 2 -CVs2.5@lac) can be obtained. Compared with free laccase, mTiO 2 -CVs2.5, and commercial P25, mTiO 2 -CVs2.5@lac shows higher catalytic efficiency in the emerging contaminants degradation under visible light. Therefore, the photo-enzyme integrated catalyst presented in this study provides a promising platform for emerging organic pollutants degradation by combining the enzymes with photocatalysts
研究领域:
环境科学
·
催化
·
材料科学
·
生物技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhijie Liu,Xin Li,Hezhi Guo,Zekai Zhang,Yongchun Wang,Polun Pang,Yuting Gao,He Guo
This paper presents a novel type of Underwater Bubble Plasma-Divalent Copper Salt-Peroxymonosulfate (UBP-Cu(Ⅱ)-PMS) for the efficient degradation of emerging contaminants in water. The results demonstrate that Cu(Ⅱ)-PMS can be effectively activated during UBP treatment process, generating two highly reactive free radicals ( OH and · S O 4 _ ) that promote the degradation of high-concentration tetracycline hydrochloride (TC). A comparative analysis of UBP’s performance in activating persulfate (PS), PMS, and sulfite (S(IV)) for the synergistic degradation of TC revealed that PMS and UBP exhibited the strongest synergistic effect. When PMS is 0.5 g/L, the activation performance peaked, with the UBP-PMS system achieving an impressive 87.22 % degradation efficiency of TC within 20 min, which is 30.02 % higher than that of the single UBP system. Furthermore, upon introducing Cu(Ⅱ) into the UBP-PMS system, with PMS at 0.5 g/L and Cu(Ⅱ) at 0.05 g/L, the degradation efficiency of TC reached 95.73 %, and energy efficiency was measured at 1.5509 g·(kWh) −1 within 20 min, surpassing other treatment systems. Free radical trapping experiments indicated that the primary reactive species responsible for TC degradation in UBP-Cu(Ⅱ)-PMS co-catalytic strategy include OH, ONOOH/ · O 2 _ , · S O 4 _ and 1 O 2 . Fenton-like reaction enhances the concentration of OH in the solution, while oxygen-sulfur radical reaction produces · SO 4 \_ . The conversion between different valence states of Cu primarily involves electron transfer. Possible degradation pathways were proposed based on DFT calculations and LC-MS analysis during the synergistic treatment, and the toxicity of by-products generated during the degradation process was evaluated using T.E.S.T. software. Ultimately, a synergistic degradation mechanism for the UBP-Cu(Ⅱ)-PMS strategy was proposed. This study introduces a new activation strategy involving UBP-Cu(Ⅱ)-PMS and provides valuable insights into the degradation performance and mechanisms of emerging contaminants.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shiyu Zuo,Yan Wang,Jinquan Wan
Peroxymonosulfate (PMS) activation technology has important application value in treating emerging contaminant (ECs), but it still faces challenges in achieving efficient electron transfer and metal valence cycling. In this study, the interfacial electric field characteristics of FeNC catalysts were adjusted by introducing N C defects to affect the electron transfer process, thereby enhancing the catalytic performance of PMS. It is found that in the Fe N C structure, the shift of the charge generates an interfacial electric field, which can promote the directional transfer of electrons. Through quantitative structure–activity relationship (QSAR) analysis, it was confirmed that the defect played a decisive role in regulating the interfacial electric field and improving the catalytic reaction efficiency. The interfacial electric field-mediated superexchange interaction realizes the electron donor effect of organic pollutants and the effective electron transfer between the Fe site, accelerates the electron cycling of the Fe site, and realizes the rapid and stable catalysis of PMS. The increase of the occupancy state distribution of d orbitals near the Fermi level provides favorable conditions for electron transitions and catalytic activation of PMS. ECs can be converted into environmentally friendly, non-toxic and harmless substances through. This defect-controlled interface electric field strategy realizes rapid electron directional transfer, which provides a new solution for improving the catalytic efficiency of PMS and the safe treatment of ECs in water.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Shizong Wang,Jianlong Wang,Hong Xu
In this study, biochar-based Fe and Co homonuclear (DAC–Fe–Co) and heteronuclear (DAC-Fe/Co) diatomic catalysts were first prepared via controlling the ligands of Fe and Co, and used to activate peroxymonosulfate (PMS) for the degradation of emerging organic pollutants, such as sulfamethoxazole (SMX), bisphenol A, phenol, atrazine, and nitrobenzene. The results showed that acid pretreatment of biochar was necessary for biochar to synthesize atomic catalysts. The DAC-Fe/Co had higher contents of Fe and Co than DAC–Fe–Co, but lower catalytic activity, in which the SMX first-order kinetics rate constant for DAC–Fe–Co was 4.1 times higher than that for DAC-Fe/Co, achieving 0.32 min–1. DAC–Fe–Co and DAC-Fe/Co could activate PMS to produce similar reactive species, including radicals and nonradicals. But DAC–Fe–Co produced a higher concentration of radicals than DAC-Fe/Co. The density functional theory (DFT) calculation indicated that compared to DAC-Fe/Co, DAC–Fe–Co had a higher adsorption capacity for PMS (−7.90 eV) and lower energy barrier for the regeneration of Fe (−1.20 eV) and Co (−1.16 eV) active sites. The enhanced regeneration of Fe and Co active sites promoted the formation of radicals, which explained the faster SMX removal rate in the system of DAC–Fe–Co/PMS than DAC-Fe/Co/PMS. The DAC–Fe–Co/PMS system exhibited high resistance to inorganic anions and showed excellent catalytic stability in the cycling experiments. This study provides insight into the discrepant catalytic activity of homonuclear and heteronuclear diatomic catalysts for PMS activation to degrade emerging organic contaminants, and offers a new way to prepare the homonuclear diatomic catalyst.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Dongdong Fan,Meihua Hu,Songyuan Li,Pinghua Chen,Hualin Jiang,Xinman Tu,Xibao Li,Xubiao Luo
The efficient activation of peroxymonosulfate for degrading emerging contaminants has become a focal point in recent decades, emphasizing the development of novel materials and efficient strategies for high-performance degradation. This study explores a spatial confinement strategy, where TiO 2 is confined inside carbon nanotubes with Co 3 O 4 loading outside, is performed to prepare the nano-confined composite TiO 2 -in-CNT/Co 3 O 4 . Norfloxacin is chosen as the primary target pollutant, revealing a degradation rate exceeding 97 % within 30 min. The non-radical 1 O 2 species were confirmed to be generated in nano-confined catalyst, but not observed in the control non-confined catalyst. Additionally, the quantity of original radical active species significantly increases in nano-confined catalyst compared to non-confined catalyst. TiO 2 -in-CNT/Co 3 O 4 has excellent reusability and application universality. Wonderful stability is observed in real water and anti-ion interference experiments, highlighting its robust stability. Experimental and DFT calculation results also demonstrate that the spatial confinement strategy prevents nanoparticle aggregation, accelerates electron transfer efficiency, and promotes the cycling of Co 2+ /Co 3+ electron pairs. This work provides insights into the regulation of confined effects in activating PMS and offers a feasible strategy for the synergistic activation of PMS for water environment remediation through a radical and non-radical mixed mechanism.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Dongdong Fan,Jian Wen,Pinghua Chen,Xinman Tu,Xubiao Luo,Yonghui Deng,Guolong Zhu,Hualin Jiang
In-situ modulation of the synergistic effect of both radicals and non-radicals is crucial in the activation of peroxymonosulfate (PMS). In this study, we show a layer-structured carbon nitride with anchored cobalt single atoms was facilely synthesized (0.2Co-CN), followed by an investigation of the mechanism and performance in activating PMS for the removal of emerging contaminants (ECs) assisted by visible light. The results indicate that under visible-light excitation, the catalytic system achieved 97.1% degradation of Norfloxacin (NOR) within 60 min, representing a 3.3-fold increase in kinetics compared to conditions without light. Experimental characterization reveals that the anchored single-atom Cobalt is prone to adsorbing and concentrating PMS, thereby favoring the activation; This observation is further supported by density functional theory calculations. The degradation mechanism shifts from a pure radical pathway to a synergistic pathway involving both radical and non-radical, under in-situ light irradiation. This light-assisted modulation significantly increases both the variety and concentration of reactive oxygen species(ROS), leading to effectively enhanced catalytic performance. The catalyst exhibits robust functionality across a broad pH range without metal ion leaching, possesses unmoved interference resistance without compromising efficiency, demonstrates excellent reusability without significant fatigue, and shows applicability to various ECs and diverse real-world water bodies, paving the road to potential industrial level applications.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xing Zhang,Suhang Chen,Haidong Luo,Zhenhua Tang,Enzhou Liu,Zhao Qin,Kangzhen Xu
The rapid redox cycle of metal active sites and effective surface reactions are crucial factors to activate peroxymonosulfate (PMS) for environmental remediation. Herein, a novel F-g-C 3 N 4 /Mn x Co 3−x O 4 composite as high-efficient PMS activator was successfully constructed by a one-step hydrothermal method for the degradation of 1,1-diamino-2,2-dinitroethylene (FOX-7). It was discovered that F doping could narrow the band gap, and enhance the light absorption range and the separation of photogenerated electron-hole pairs. Among all samples, the catalytic activity of F-CN/MCO was higher than that of MCO and CN/MCO. This can be attributed to the unique materials morphology and the synergistic effect of photocatalytic and chemical catalytic driven PMS activation. Quenching experiments and electron paramagnetic resonance (EPR) proved that both radical and non-radical pathways are responsible for the degradation of FOX-7, and singlet oxygen ( 1 O 2 ) was identified as the predominant active species. Importantly, the synergy between Co 2+ /Co 3+ and Mn 2+ /Mn 3+ couples enhanced more electron transfer and better redox potential, thus greatly promoting the photocatalytic activation of PMS. This work provides a novel approach for designing efficient catalyst to promote the redox behavior of metal species in sulfate radical-based advanced oxidation processes.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）