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MATERIALS CHEMISTRY AND PHYSICS · 2023 · IF 4.6

Adsorption of La3+ onto trifluoroacetic acid modified UiO-66-COOH: Adsorption mechanism and application

Lin Yang,Tingjiao Liu,Zheng Li,Changqing Liu,Feifeng Wang,Chunshan Wu

The application of metal organic frameworks (MOFs) for the recovery of low concentrations of rare-earth elements (REEs) has attracted increasing attention due to the precious value of REEs resources. In this study, UiO-66-COOH was modified by trifluoroacetic acid (TFA) to not only promote material crystallization and the pore structure verified by XRD and SEM characterization, but successfully enhance its adsorption capacity and achieve perfect selectivity for Lanthanum ion (La 3+ ). The adsorption capacity for UiO-66-COOH-24TFA was increased by 58% compared to unmodified material. The adsorption mechanism and application were comprehensively investigated. By adsorption kinetics , isotherm and thermodynamic studies, it was found that the adsorption process mainly exhibited monolayer adsorption with spontaneous endothermic-chemisorption characteristics, and –COOH of the modified materials (UiO-66-COOH-24TFA) played an important role, which was confirmed by XPS. Moreover, UiO-66-COOH-24TFA was applied to REEs actual wastewater by successive six-stage adsorption process , where the overall recovery rate on La 3+ reached 94.1% under the coexisting conditions of multiple ions. The application of this acid modified material in the field of the separation and recovery of REEs is of great promise.

CAS / MDL: 528-44-9
研究领域: 材料科学 · 环境科学
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Nitrogen rich hollow carbon spheres with well-developed mesoporous: An efficient adsorbent for tetracycline removal

Yanyang Liu,Qingliang You,Xiaofang Yang,Guiying Liao,Dongsheng Wang

In this study, we developed a simple and green method to fabricate the N-doped mesoporous hollow carbon (NMHC) materials by one step carbonization of coating the melamine‐formaldehyde (MF) resin sphere with dopamine (DA). The characterization results indicated that the NMHC had large specific surface areas (302.38–399.54 m 2 /g), well-developed mesoporous structure (0.390–0.414 cm 3 /g) and high nitrogen content (7.71–10.15 wt%). The as-prepared NMHC exhibited excellent adsorption performance towards tetracycline (TC), and the maximum adsorption amount on the NMHC-700 was 481.70 mg/g at 298 K, which increases of 19.46% and 9.36% than that of NMHC-600 (403.22 mg/g) and NMHC-800 (440.44 mg/g), respectively. The adsorption process obeyed the pseudo-second-order kinetic model and Langmuir adsorption isotherm model. The NMHC exhibited outstanding reusability for TC after five cycles. And the NMHC adsorbents would be considered as a broad-spectrum adsorbent to remove other organic pollutants . Moreover, it was also found that the NMHC still maintained excellent adsorption capability towards TC in actual wastewater. Thus, this work not only displayed a mild method to prepare the NMHC for the removal of antibiotics, but also demonstrated the practical application prospect of the NMHC.

CAS / MDL: 51-61-6 60-54-8
研究领域: 环境科学 · 材料科学
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2019 ·Vol. 30 ·期 16 ·15754-15765 · IF 2.195

Photocatalytic performance of Ag/AgBr modified TiO2: critical impacts and wastewater sample study

Sun Jialin,Huang Dejia,Liu Rui,Dai Jingtao,Chen Jian

To improve the visible-light photocatalytic performance of TiO 2 for practical application, Ag/AgBr modified TiO 2 was fabricated in ionic liquid–water medium via a facile hydrothermal-reduction method. The visible-light catalytic activity of as-prepared Ag/AgBr/TiO 2 was measured using tetracycline (TC) as the target pollutant. Characterizations by various techniques (SEM–EDS, XRD, XPS and DRS) and the quenching experiments with scavengers for possible active species (h + , • O 2 − and ·OH) were executed to probe the mechanism underlying the photocatalytic performance. Critical impacts from the catalyst and solution chemistry were evaluated in the mediums of TC solution, simulated wastewater and real wastewater sample. The results suggested that: (1) benefitting from the visible-light sensitive Ag/AgBr and high specific surface area TiO 2 , Ag/AgBr/TiO 2 exhibits fair stability and remarkable visible-light photocatalytic activity; (2) under optimized conditions, Ag/AgBr/TiO 2 provides higher visible-light catalytic activity than Ag/AgBr and TiO 2 ; (3) the coexisting inorganic ions with high concentration in the simulated wastewater sample depress TC photo-degradation, and the impacts varies with the species of inorganic ions; (4) COD removal rate about 65.5% in real wastewater sample proves that Ag/AgBr/TiO 2 can mineralize TC promptly and almost completely.

研究领域: 环境科学 · 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Ti4O7-C3N4 anode with a low charge transfer resistance value for degradation of imidacloprid in actual wastewater

Shuting Guo,Qiongfang Zhuo,Gang Huang,Liying Lan,Tongyin Zhu,Wenlong Wang,Zehong Yang,Jiasheng Fang,Yongfu Qiu,Bo Yang

Imidacloprid (IMD) is a kind of neonicotinoid insecticide, which is widely used in the agricultural production. There are few reports on electrocatalytic degradation of IMD with the low concentration. In this study Ti 4 O 7 -C 3 N 4 electrode was employed for the first time to electrocatalytically degrade low concentration IMD. Compared with pure Ti 4 O 7 electrode, the oxygen evolution potential was increased from 1.84 V to 2.50 V, the charge transfer resistance (R ct ) was reduced by 66.05 %, and the oxygen vacancies were increased by 2.5 times compared to the original Ti 4 O 7 . Especially, the R ct for Ti 4 O 7 (5.45 Ω·cm 2 ) was only 1/7 of that for boron-doped diamond (BDD) (38.89 Ω·cm 2 ). IMD degradation ratio was up to 98 % in only 1.256 min (75.360 s) using a Ti 4 O 7 -C 3 N 4 . When SongShan Lake water, Wanjiang water, and secondary effluent were treated, the degradation radios of IMD were 70.30 %, 72.33 % and 81.12 %, respectively. In the presence of Cl − coexisting ions, no disinfection by-product of ClO 4 − was detected, which is an advantage for Ti 4 O 7 -C 3 N 4 compared with BDD. The first and 48th degradation ratios were 99 % and 97 %, respectively, indicating the good stability of Ti 4 O 7 -C 3 N 4 . The development of Ti 4 O 7 -C 3 N 4 provides a stable, low energy consumptions and no secondary pollution anode for the treatment of actual wastewater.

CAS / MDL: 108-78-1
研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2024 · IF 8.1

Sustainable H2O2 production in a floating dual-cathode electro-Fenton system for efficient decontamination of organic pollutants

Zhicheng Wang,Chen Wang,Xiaohui Wu,Wen-Da Oh,Mingjie Huang,Tao Zhou

Electrochemical advanced oxidation processes (EAOPs) based on natural air diffusion electrode (NADE) promise efficient and affordable advanced oxidation water purification , but the sustainable operation of such reaction systems remains challenging due to severe cathode electrowetting. Herein, a novel floating cathode (FC) composed of a stable hydrophobic three-phase interface was established by designing a flexible catalytic layer of FC. This innovative electrode configuration could effectively prolong the service life of the cathode by mitigating the interference of H 2 bubbles from the hydrogen evolution reaction (HER), and the H 2 O 2 production rate reached 37.59 mg h −1 ·cm −2 and realize a long-term stable operation for 10 h. Additionally, an FC/carbon felt (CF) dual-cathode electro-Fenton system was constructed for in situ sulfamethoxazole (SMX) degradation. Efficient H 2 O 2 production on FC and Fe(III) reduction on CF were synchronously achieved, attaining excellent degradation efficiency for both SMX (ca. 100%) with 2.5 mg L −1 of Fe(Ⅱ) injection. For real wastewater , the COD removal of the FC/CF dual-cathode electro-Fenton system was stabilized at exceeding 75%. The practical application potential of the FC/CF dual-cathode electro-Fenton system was also demonstrated for the treatment of actual landfill leachate in continuous flow mode. This work provides a valuable path for constructing a sustainable dual-cathode electro-Fenton system for actual wastewater treatment .

CAS / MDL: 31175-20-9 14481-26-6
研究领域: 环境科学 · 电化学工程 · 水处理技术
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AICHE JOURNAL · 2023 · IF 3.7

Ionic liquid-induced deep grafting of polyelectrolyte to reform polyamide layer for antifouling nanofiltration membrane

Lulu Liu,Yuxuan Liu,Yinhua Wan,Weijie Song,Hongwei Lu,Jianquan Luo

Surface grafting has been widely used to tune hydrophilicity and chargeability of nanofiltration membranes for reducing membrane fouling potential. However, surface grafting typically leads to a significant pore narrowing and resultant permeability loss, and monocharged surface still struggles to resist mixed foulants with different charges. Herein, ionic liquid (IL)-ethanol (EtOH) solution containing polyethyleneimine (PEI) is used to rearrange the nascent polyamide layer. The high affinity of IL to the PA layer and the low diffusion steric hindrance of EtOH contribute to the polyamide swelling and PEI deep grafting, during which the “self-regulation” effect (larger pores would be filled with more PEI molecules) narrows the pore size distribution and enhances hydrophilicity. The nearly charge-neutral and smooth separation layer shows impressive antifouling capacity to hydrophobic macromolecules and mixed charged molecules, along with long-term operating stability for real wastewater treatment. This study emphasizes the importance of solvent properties on the membrane grafting behavior.

研究领域: 材料科学 · 环境工程 · 膜技术 · 化学工程
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Journal of Materials Chemistry C · 2025 · IF 5.1

Interfacial charge-transfer in CoAl-LDH/CoOx for photocatalytic dye degradation and UV/H2O2 assisted real-wastewater treatment

Tariq Ali,Yiwei Li,Bingjie Fang,Saleem Raza,Yeyuan Xiao

Photocatalysis can decolorize dye-laden wastewaters using light, but practical catalysts often suffer from narrow absorption, charge recombination, and stability limits. Here we synthesize a carbonate-intercalated cobalt–aluminum layered double hydroxide hosting cobalt-oxide nanocluster (CoAl-LDH/CoOx) via a one-pot hydrothermal route and evaluate its performance for dye decolorization and UV/H2O2 treatment of real textile wastewater. Under UV irradiation, CoAl-LDH/CoOx accelerates discoloration of methyl orange (MO) and Congo red (CR), following pseudo-first-order kinetics (e.g., MO: ∼98% removal at 5 mg L−1 in 100 min; CR: ∼100% at 100 mg L−1 in 100 min; kapp up to 0.14 min−1). On real textile wastewater (ADMI0 = 608.1), UV/H2O2 with 0.5 g L−1 catalyst achieved ∼80% American Dye Manufacturer's Institute (ADMI) removal in 120 min at 48.96 mM H2O2; outdoor sunlight tests removed 82.5% (raw influent) and 50.8% (biologically treated effluent) over 20 h. Scavenger tests and EPR spin-trapping implicate h+ and ˙O2− as dominant species under UV, with ˙OH contributing when H2O2 is present. Five-cycle tests indicate stable activity. The one-pot CoAl-LDH/CoOx heterostructure provides a robust, recyclable platform for interfacial charge-transfer-assisted photocatalysis on realistic effluents and motivates follow-up on mineralization and leaching.

CAS / MDL: 7784-27-2
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Enhanced removal of hydrophobic endocrine disrupting compounds from wastewater by nanofiltration membranes intercalated with hydrophilic MoS2 nanosheets: Role of surface properties and internal nanochannels

Ruobin Dai,Hongyi Han,Tianlin Wang,Xuesong Li,Zhiwei Wang

The presence of endocrine disrupting compounds (EDCs) in water and wastewater poses potential risks on aquatic environment and human health. Conventional polyamide (PA) nanofiltration (NF) membrane showed poor rejection against EDCs due to unfavorable hydrophobic interaction. In this study, we introduced MoS 2 nanosheets (NS) to PA NF membrane by pre-deposition before the interfacial polymerization process, creating hydrophilic surface and nanochannels in the PA rejection layer to enhance removal of hydrophobic EDCs from wastewater. Results showed that the MoS 2 NS intercalated membrane simultaneously enhanced water permeance and EDCs rejection, with water/EDC selectivity nearly 6 times larger compared to the control. The enhanced EDC rejection was primarily attributed to the suppressed hydrophobic interaction between membrane surface and hydrophobic EDCs, as well as the selective effect by the MoS 2 NS-induced nanochannels. Further calculation based on the solution-diffusion theory indicated that for MoS 2 NS intercalated membranes the selective nanochannels played a more important role than the hydrophilic surface in impeding the transport of EDCs across the PA layer. The feasibility of the MoS 2 NS intercalated PA membrane for EDC removal was also verified using EDC-contaminated real wastewater . The results of this work highlight the potential of using the designed NF membranes for efficient removal of targeted organic micropollutants from water and wastewater.

研究领域: 环境工程 · 膜科学 · 水处理 · 纳米技术
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Environmental Science-Nano · 2024 ·Vol. 11 ·期 7 ·3092-3103 · IF 5.8

Highly coordinated Fe–N5 sites effectively promoted peroxymonosulfate activation for degradation of 4-chlorophenol

Manoj Kumar Panjwani,Feiyu Gao,Ting He,Pan Gao,Feng Xiao,Shaoxia Yang

M–Nx single-atom catalysts (SACs) with a high coordination number (x > 4) are effective catalysts for eliminating organic pollutants, while the origin of SACs with high activity still remains elusive. In this work, we successfully synthesized an Fe–N5 SAC with axial N coordination, which exhibited exceptional catalytic performance by peroxymonosulfate (PMS) activation for degrading 4-chlorophenol (4-CP) in a wide pH range (4.0–10.0). The rate constant of Fe–N5 (2.99 min−1) was 6.36 times higher than that of Fe–N4, and the turnover frequency (TOF) of Fe–N5 was found to be 4–149 times higher than those of state-of-the-art SACs and nanocatalysts reported in the literature for 4-CP degradation by PMS activation. Moreover, Fe–N5 was not significantly affected by coexisting substances (HA, HCO3−, SO42−, H2PO4−, NO3−, and Cl−) and had satisfactory degradation efficiency for various chlorophenols. Electron paramagnetic resonance (EPR), quenching experiments, and radical probe experiments demonstrated that 1O2 played a key role in the Fe–N5/PMS system for 4-CP degradation. Density functional theory calculations confirmed that a narrower gap between the Fe-3d band center and Fermi level enhanced the electron transfer in Fe–N5, which resulted in promoted PMS activation. In addition, the Fe–N5/PMS system showed good potential for application in real wastewater. The above findings offer important implications for the future of coordination chemistry in designing M–Nx–C SACs (x > 4), highlighting their practical applications in environmental remediation.

研究领域: 环境化学 · 催化 · 材料科学 · 环境工程
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A novel UV based advanced oxidation process with electrochemical co-generation of chlorine and H2O2 for carbamazepine abatement: Better performance, lower energy consumption and less DBPs formation

Haoran Yin,Qizhan Zhang,Yi Su,Yunping Tang,Minghua Zhou

To promote the performance of traditional UV/chlorine and UV/H 2 O 2 processes, the novel UV based advanced oxidation process with electrochemical co-generation of chlorine and H 2 O 2 (UV/E-Cl&H 2 O 2 ) was for the first time used for degradation of carbamazepine (CBZ), a refractory antiepileptic drug with resistance to photodegradation and microbial degradation . Compared with UV/E-Cl and UV/E-H 2 O 2 processes, the apparent first-order rate constant of CBZ degradation by UV/E-Cl&H 2 O 2 process increased by 3.87 and 5.84 times respectively with a lower energy consumption (1.12 kWh/m 3 -log). Meanwhile, the disinfection by-products (DBPs) formation by the novel process was 21.4% less than that by UV/E-Cl process. Under the optimal condition of initial pH 7, applied current 600 mA and 15 mM NaCl, the UV/E-Cl&H 2 O 2 process could almost completely eliminate CBZ within 4 min and obtain 57.8% TOC removal in 1 h. The mechanism of UV/E-Cl&H 2 O 2 was investigated through processes comparison, quenching experiments, EPR analysis and determination of OH concentration. The generated radicals (i.e., OH and reactive chlorine species), especially OH, played a major role in CBZ removal. Besides, the possible degradation pathways of CBZ were proposed and the stability of UV/E-Cl&H 2 O 2 process for CBZ removal was certified based on ten consecutive runs. The degradation of typical pollutants (sulfamethazine, rhodamine B, methylene blue , atrazine and phenol) and treatments in three kinds of real wastewater confirmed the wide application feasibility of the novel process. In summary, this study provides a novel efficient and energy-saving process for removing organic pollutants with promising perspectives..

研究领域: 环境科学 · 水处理 · 化学工程 · 高级氧化过程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 30 ·期 13 ·35683-35697 · IF 5.19

Activation of peroxymonosulfate by catalysts derived from water treatment plant sludge for the simultaneous removal of Disperse Blue 56 and phosphates

Tang Xing,Jin Hongyi,Zou Jing,Liu Shupo,Li Fei,Zhou Zhenming

In this study, calcined water treatment plant sludge (C-WTPS) was used as a catalyst for peroxymonosulfate (PMS) activation to simultaneously remove Disperse Blue 56 (DB56) and phosphates. Firstly, the performance of the C-WTPS/PMS system was examined for the degradation of DB56. The results showed that 96.7% of DB56 (400 mg L −1 ) was removed within 60 min in the presence of 4.8 g L −1 PMS and 0.8 g L −1 C-WTPS at pH 3 and 50 °C. Hydroxyl radicals (·OH), sulfate radicals (SO 4· − ), and singlet oxygen ( 1 O 2 ) were generated during the oxidation process, and 1 O 2 was the main active species. The relatively high surface area, proper Fe content, and abundant ketone groups on the catalyst surface were responsible for PMS activation. Furthermore, the possible degradation pathways of DB56 were proposed based on the gas chromatography–mass spectrometry (GC–MS) results. Secondly, the simultaneous removal of DB56 and phosphates by the C-WTPS/PMS system was investigated. Due to the different removal mechanisms, the effects of the initial phosphate concentration and water matrix species on the removal of DB56 and phosphates showed different trends. Reusability tests results showed that C-WTPS had relatively high stability. In addition, the C-WTPS/PMS system exhibited a high decolorization ratio and phosphate removal efficiency in real wastewater tests. This article offers a value-added approach for reusing WTPS as a catalyst for treating organic contaminants and phosphates.

研究领域: 环境科学 · 水处理 · 催化 · 污染物去除
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Efficient peroxymonosulfate activation by nanoscale zerovalent iron for removal of sulfadiazine and sulfadiazine resistance bacteria: Sulfidated modification or not

Ying Liu,Jingfeng Gao,Qian Wang,Hao Chen,Yi Zhang,Xiaoyu Fu

Whether it’s necessary to extra chemical synthesis steps to modify nZVI in peroxymonosulfate (PMS) activation process are worth to further investigation. The 56 mg/L nZVI/153.65 mg/L PMS and 56 mg/L sulfidated nZVI (S-nZVI) (S/Fe molar ratio = 1:5)/153.65 mg/L PMS) processes could effectively attain 97.7% (with k obs of 3.7817 min −1 ) and 97.0% (with k obs of 3.4966 min −1 ) of the degradation of 20 mg/L sulfadiazine (SDZ) in 1 min, respectively. The nZVI/PMS system could quickly achieve 85.5% degradation of 20 mg/L SDZ in 1 min and effectively inactivate 99.99% of coexisting Pseudomonas . HLS-6 (5.81-log) in 30 min. Electron paramagnetic resonance tests and radical quenching experiments determined SO 4 •− , HO•, 1 O 2 and O 2 •− were responsible for SDZ degradation. The nZVI/PMS system could still achieve the satisfactory degradation efficiency of SDZ under the influence of humic acid (exceeded 96.1%), common anions (exceeded 67.3%), synthetic wastewater effluent (exceeded 90.7%) and real wastewater effluent (exceeded 78.7%). The high degradation efficiency of tetracycline (exceeded 98.9%) and five common disinfectants (exceeded 96.3%) confirmed the applicability of the two systems for pollutants removal. It’s no necessary to extra chemical synthesis steps to modify nZVI for PMS activation to remove both chemical and biological pollutants.

研究领域: 环境科学 · 化学工程 · 水处理
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