WATER RESEARCH
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2025
·
IF 12.4
Yang Wang,Ziyuan Huang,Zhang Yan,Zhenchao Lei,Huanxin Ma,Chunhua Feng
Acid mine drainage (AMD) is characterized by high concentrations of Fe(II) and Fe(III), which can be harnessed for the in-situ formation of schwertmannite, enabling the efficient immobilization of toxic heavy metals. However, existing biological and chemical methods for schwertmannite synthesis face significant challenges, including low Fe(II) oxidation rates and particularly limited Fe(III) precipitation efficiency in acidic environments. In this study, we develop a visible light-assisted photo-electrochemical (PEC) system that effectively overcomes these barriers. By leveraging anodically evolved O 2 and cathodically generated OH − , we achieved facile Fe(II) oxidation at pH 3.0, and an impressive Fe(III) precipitation efficiency of 82.8 %, significantly exceeding the < 30 % efficiency reported by other methods. Mössbauer spectroscopy and X-ray diffraction confirmed that the generated minerals are high-purity schwertmannite. Experimental and theoretical analyses revealed that in the presence of cathodic alkalinity, Fe(III) undergoes further hydrolysis to form [(H₂O) 3 Fe(OH) 2 (SO 4 )] − species, which are thermodynamically capable of spontaneous polymerization and mineralization. Furthermore, the photoreduction of [(H₂O) 4 Fe(SO 4 ) 2 ] − within the PEC system, followed by subsequent oxidation, plays a crucial role in facilitating Fe(III) mineralization. The PEC system also effectively transformed As(III) to As(V) and Cr(VI) to Cr(III) in AMD, promoting their immobilization in the resultant schwertmannite.
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FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Ting Lu,Yucui Hou,Weize Wu,Muge Niu,Wei Li,Shuhang Ren
Carboxylic acids are considered as an important group of chemicals. Direct conversion of cellulose to formic acid (FA) by vanadium(V(V))-contained catalyst is of significant conceptual and practical interest. A second metal (from Mg(II), Ca(II), Al(III), Cr(III), Mo(VI), Mn(II), Cu(II), or Fe(III)) incorporated into V(V)-contained catalyst system was screened to further improve the oxidation of cellulose by O 2 to yield FA. Fe(III) exhibited the best performance and effects of reaction parameters on the conversion of cellulose in NaVO 3 -FeCl 3 -H 2 SO 4 aqueous solution were investigated. Cellulose could be rapidly converted, and the yield of FA (66.8%) was higher than that obtained by the single use of FeCl 3 (48.4%) or NaVO 3 (57.6%). The conversion of cellulose in another V(V)-contained catalyst system (H 5 PV 2 Mo 10 O 40 ) was explored to verify the universal enhancement of FeCl 3 . Influences of the second metal Fe(III) on the V(V)-contained catalyst system and mechanism of cellulose oxidation in the V(V)-Fe(III)-H 2 SO 4 system were studied. Compared with single use of V(V), the employment of Fe(III) alone is not active enough in the oxidative C C bond cleavage . V(V) other than Fe(III) is the main active species for selective oxidation of substrates. The incorporation of Fe(III) and V(V) shows both synergistic and competitive relationships. Both the synergistic and competitive effects are beneficial to increase FA yield, as they promote the oxidation of V(IV) to V(V), increase oxidative ability, and inhibit the overoxidation to by-product CO 2 . The catalyst system was reused four times without decline in activity.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Shiyu Pan,Deling Yuan,Jinhao Li,Zhibin Wang,Qingrui Zhang,Shoufeng Tang
The traditional Fenton application is limited by the disproportionation of hydrogen peroxide (H 2 O 2 ) and the tardy reduction of Fe(III). To conquer these issues, we construct an enhanced Fenton-like process using a composite of citric acid-carboxylated microcrystalline cellulose complexing with Fe(III) (CA-Fe(III)@MCC) to activate sodium perborate (SPB), which can effectively eliminate antibiotic sulfamethoxazole (SMX, 89.2%, 0.035 min -1 ). The CA-Fe(III)@MCC composite significantly enhances the circulation of Fe(III)/Fe(II), leading to the generation of hydroxyl radicals and perboric radicals with excellent structural stability and minimal Fe leaching during CA-Fe(III)@MCC/SPB process. Systematic investigations reveal that the introduced carboxyl groups not only anchor Fe(III) to prevent its deactivation and leaching, but also regulate the coordination environment and serve as electron shuttles, driving the formation of reactive species and reduction of Fe(III). This process presents a novel, environmentally friendly, and sustainable strategy for utilizing natural cellulose and its industrial biomass product in advanced oxidation processes .
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CRYSTENGCOMM
·
2025
·
IF 2.6
Han Fang,Jia-Peng Han,Bo Zhang,Deng-Bo Liu,Xing-Wang Li,Jing-Yu Li,Yutong He,Mei-Hui Yu
The heavy metal ion pollution has become one of the most serious environmental problems, which promotes the continuous exploration of new materials and methods to achieve efficient detection of heavy metal ions. Luminescent metal-organic frameworks (LMOFs) featuring the designable and functional structures and tunable luminescence properties exhibit excellent potential for the recognition and detection of heavy metal ions. Herein, a Cd(II)-based luminescence MOF {[Cd2(2F-bpdc)2(tib)]}n (NKM-103) (tib=1,3,5-tris(1-imidazolyl)benzene, 2F-H2bpdc= 3,3'-difluorobiphenyl-4,4'-dicarboxylic acid) has been designed and synthesized successfully. Derived from the characteristic of ligand with conjugated units, NKM-103 shows well fluorescence emission performance and potential as a sensor for detecting both Fe(III) cations and Cr(VI) anions (Cr2O72- and CrO42-) through turn-off effect. Moreover, NKM-103 for all three kinds of ions shows low detection limit and high selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Shishun Wang,Shuang Gai,Kui Cheng,Zhuqing Liu,Markus Antonietti,Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO 4 •- , and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
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WATER SCIENCE AND TECHNOLOGY
·
2024
·Vol. 89
·期 7
·1682-1700
·
IF 2.5
Zhang Longbin,Gao Jianxiong,Liu Yulong,Zhou Zhengyuan,Sheng Xianxian,Li Dexiao,Chen Yuantian,Lyu Shuguang
View large Download slide View large Download slide Close modal In this research, ascorbic acid (AA) was used to enhance Fe(II)/Fe(III)-activated permonosulfate (PMS) systems for the degradation of fluoranthene (FLT). AA enhanced the production of ROS in both PMS/Fe(II) and PMS/Fe(III) systems through chelation and reduction and thus improved the degradation performance of FLT. The optimal molar ratio in PMS/Fe(II)/AA/FLT and PMS/Fe(III)/AA/FLT processes were 2/2/4/1 and 5/10/5/1, respectively. In addition, the experimental results on the effect of FLT degradation under different groundwater matrixes indicated that PMS/Fe(III)/AA system was more adaptable to different water quality conditions than the PMS/Fe(II)/AA system. was the major reactive oxygen species (ROS) responsible for FLT removal through the probe and scavenging tests in both systems. Furthermore, the degradation intermediates of FLT were analyzed using gas chromatograph-mass spectrometry (GC-MS), and the probable degradation pathways of FLT degradation were proposed. In addition, the removal of FLT was also tested in actual groundwater and the results showed that by increasing the dose and pre-adjusting the solution pH, 88.8 and 100% of the FLT was removed for PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The above experimental results demonstrated that PMS/Fe(II)/AA and PMS/Fe(III)/AA processes have a great perspective in practice for the rehabilitation of FLT-polluted groundwater. The effect of AA on the circulation between Fe(II) and Fe(III) in the PMS system was investigated. SO 4 •− was the primary ROS in PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The effect of actual groundwater matrixes on FLT removal was investigated. The possible degradation pathways of FLT were proposed. Effective degradation of FLT in actual groundwater was achieved.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiahui Ma,Bin Jiang,Longfei Zhang,Feihong Chu,Na Yang,Yongli Sun,Luhong Zhang
Traditional textile wastewater treatment methods face significant challenges in achieving effective dye/salt separation with low energy consumption. In this study, a high-performance loose nanofiltration (LNF) membrane based on metal-polyphenol bio-adhesion was fabricated. By exchanging Fe 3+ onto Laponite (Lp) nanosheets, the coordination between tannic acid (TA) and Fe 3+ was controlled, optimizing the structure of the selective layer. Subsequently, PVP was introduced to regulate membrane structure owing to the hydrogen bonding between TA and PVP, thereby enhancing both separation performance and stability of the membrane. The optimized Fe@Lp/TA-PVP membrane exhibited favorable separation performance by modulating preparation conditions including the Fe 3+ exchanging on Lp nanosheets, PVP concentration, and coating time. The LNF membrane possessed high water permeability (167.7 L·m −2 ·h −1 ·bar −1 ) and favorable separating efficiency for dyes from salts. A high rejection of 99.9 % was achieved for Congo Red and Methyl Blue, while the rejection of Na 2 SO 4 and MgCl 2 remained low, at 8.93 % and 2.21 %, respectively. Besides, the membrane demonstrated desirable antifouling capability. Therefore, this work enriches the applications of metal-polyphenol coordination in water treatment, provides new insights into the design of LNF membranes.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Xuan Zhang,Xi Du,Yan Ke,Yu-Gao Zhang,Zhi-Kang Xu
Loose nanofiltration membranes (LNMs) have attracted increased attention in the field of sustainable management of the highly-saline textile wastewater. Remained challenges include achieving efficient dye/salt fractionation and alleviating high fouling propensity. Herein, functionalized-LNMs (F-LNMs) are developed by the co-deposition of polyethylenimine and tannic acid, followed by the assembly of ferric ions (Fe(III)) and organophosphonic acid (OPa) for antifouling surface construction. Plentiful OPa groups are immobilized onto the membrane surface via the high surface binding affinity and the strong coordination bonding of Fe(III) as ‘bridge’ linkers. The superior hydrophilicity and large steric hindrance of these OPa groups endow the F-LNMs with notably improved antifouling property against organic dye clusters. The optimized F-LNMs show significantly increased membrane permeance (10–30 L m −2 h −1 ·bar −1 ) in treating those simulated dye/salt aqueous solutions containing 1.0 g L −1 dye and 80.0 g L −1 Na 2 SO 4 . They also exhibit high salt permeation (>94%) and acceptable dye rejection (overall >93%) of Congo red, methyl blue and three hydrolyzed reactive dyes. Furthermore, the direct reuse of Na 2 SO 4 from the actual dyeing effluent is achieved by combining membrane separation and activated carbon adsorption, revealing the promising application prospects of F-LNMs in managing highly-saline textile wastewater.
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WATER RESEARCH
·
2019
·
IF 7.913
Yuan Yuan,Wei Zhao,Zicheng Liu,Chen Ling,Changqing Zhu,Fuqiang Liu,Aimin Li
The efficient recovery of heavy metals from complexed wastewater is an essential but challenging task. In this study, a novel low-Fe(III) driven UV/Air process (LFUA) was developed to break the strong complexation between ethylenediamine tetracetic acid (EDTA) and heavy metal ions (HMIs) and enable the enhanced recovery of HMIs via chelating resin adsorption (CRA). The inside mechanism of the LFUA process includes: 1) displacement of HMIs from HMI-EDTA complexes by Fe(III); 2) direct photolysis of Fe(III)-EDTA through a ligand-to-metal charge transition reaction (LMCT) and indirect photolysis of EDTA by HO 2 ·/O 2 · - . The iron dosage was orders of magnitude lower than that previously reported, due to the Fe(II)/Fe(III) redox cycle in the LFUA process. Fe(II) formed during the LMCT reaction of Fe(III)-EDTA was oxidized back to Fe(III) by O 2 and HO 2 ·, and the reformed Fe(III) was then recombined with EDTA to sustains the LMCT reaction. EDTA was completely removed in 20 min at a molar ratio of Fe(III)/EDTA = 0.05. In addition, following the LFUA process, the adsorption amounts of various HMIs onto D463 resin were at least two orders of magnitude higher than those reported using the direct adsorption process. Employing the integrated technique of LFUA + CRA enabled the efficient removal of up to 64.5 mg/L of Cu(II) from inlet wastewater, and residual Cu(II) was below 0.5 mg/L. The results of desorption experiments showed that over 90% of Cu(II) was recovered, and the desorption solution had a Cu concentration of 2.1 g/L and purity of 99%. Furthermore, the economic and practical feasibility of using the combined process of LFUA + CRA was analyzed to substantiate that the technique is highly efficient and clean (produces no harmful sludge). Therefore, it is an appropriate and practical process in removing HMIs-EDTA complexes and recovering HMIs from wastewater.
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HIGH PERFORMANCE POLYMERS
·
2024
·
IF 1.8
Weihua Zhong,Jinwang Bai,Yunjun Luo,Dianbo Zhang,Chen Liang,Xiangdong Chen
Poly(p-phenylene-2,6-benzobisoxazole) (PBO) fiber is currently one of the best-performing organic fibers; however, its low UV aging resistance limits its use. To improve the UV aging performance of PBO fibers, a novel PBO-Fe-PDA fiber was created by depositing a biomimetic structure of polydopamine (PDA) on the surface of PBO fibers with the transition metal ion Fe3+ as the active center. The surface morphology and elemental composition of PBO-Fe-PDA fibers were investigated. It was revealed that Fe3+ formed a coordination bond structure with the oxazole ring, and PDA was successfully loaded onto the surface of PBO-Fe fibers. After UV aging, the crystallinity and crystallographic orientation of PBO fibers significantly decrease, microcrystals inside the fibers slip, and the size of microvoids in the fibers rises. As a result, the strength of PBO fibers was significantly decreased after UV aging. The anti-UV aging capacity of PBO-Fe-PDA fibers, on the other hand, has been enhanced, as evidenced by a slight drop in crystallinity and crystallographic orientation and a significant decrease in the size growth of internal microvoids in the fibers after UV aging. The tensile strength retention of PBO-Fe-PDA fibers after UV aging increased by 93.13% when compared to PBO fibers without altering the fibers’ initial strength. The testing results show that this surface modification method is simple to employ and extends the service life of PBO fibers significantly.
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Water
·
2022
·Vol. 14
·期 19
·2946
·
IF 3.53
Chaomin Jia,Yijia Fan,Ruolan Jiang,Peidong Su,Shuai Liu,Xiaohui Zhang,Jianbing Wang
Excessive fluoride in mine water has become a major concern because it can cause detrimental effects to human health. Nevertheless, the removal efficiency of traditional adsorbents is far from satisfactory. Herein, La and Fe bimetallic supported zeolite was synthesized by co-precipitation method, for efficient defluoridation. The defluoridation performance of La-Fe zeolite was studied by a batch adsorption experiment and dynamic adsorption column test. Results indicated that the removal efficiency of F−was 99.04% under the optimal conditions (4 h, adsorbent dosage 8.0 g/L, agitation rate 200 rpm/min, temperature 298K and pH = 6 ± 1) that were determined through the batch adsorption experiments. CO32−and HCO3−can inhibit the defluorination effect of La-Fe zeolite. The adsorption of fluoride ions on La-Fe zeolite can be well described by the Langmuir adsorption model, and the maximum fluoride ion adsorption capacity is 2.64 mg/g. The test of dynamic adsorption column shows that the adsorption efficiency of F−by La-Fe zeolite on was higher than 85% for continuous adsorption of 9 h, indicating that La-Fe zeolite has good practical applications. The mechanism analysis indicated that the adsorption of fluoride ion by La-Fe modified zeolite involves both ion exchange and complexation, which belongs to the physicochemical process.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
·
2015
·
IF 3.615
Shuang Fan,Yi Luan,Jingjing Wang,Hongyi Gao,Xiaowei Zhang,Ge Wang
A novel ferric chloride immobilized poly(4-vinylpyridine) (P4VP) catalyst was developed via a coordination chemistry-based approach. The pyridine moiety of poly(4-vinylpyridine) spheres functioned as the nitrogen donor to bind iron ions, as well as to decrease the amount of pyridine used in the catalytic reaction system. The monodispersed catalyst was well dispersed in the organic solvent during the catalytic procedure, taking advantage of its nanomorphology and uniform size. The catalytic activity of various monodispersed catalysts based different mass fractions of the divinylbenzene (DVB) was investigated, meanwhile the capacities of supported Fe(III) in the various catalysts were also discussed. The P4VPDVB 10% -Fe(III) catalyst exhibited high catalytic activity in the benzylic oxidation of benzylic methylenes and secondary benzylic alcohols. It was easily separated from the reaction system and reused several times without obvious degradation of catalytic activity. Moreover, leaching tests suggested that the as-synthesized P4VPDVB 10% -Fe(III) catalyst was a true heterogeneous catalyst without significant metal leaching.
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