Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·123082
·
IF 7.5
Zhe Xu,Jiantong Zhou,Chengfeng Liu,Weilan Zhen,Taicheng An
The peroxodisulfate (PDS)-based oxidation systems are promising for Cu(II) complex decomplexation owing to its capacity to harness the self-enhanced decomplexation (SED) effect of Cu(II) complexes. This phenomenon was conventionally attributed to liquid-phase autocatalysis via Fenton-like reactions between daughter Cu(II) species and PDS. However, this frequently adopted hypothesis is inconsistent with the actual catalytic activity of Cu(II) species and has been challenged by our preliminary results. Herein, we revisit the decomplexation of copper(II)-ethylenediaminetetraacetate (Cu(II)-EDTA) in UV/PDS system, with particular emphasis on correcting the catalytic behaviors of Cu species and clarifying the indispensable role of UV-irradiation in SED effect. Both acidic and alkaline conditions exhibit significant SED effect, but we reveal a pH-dependent SED mechanism that is fundamentally different from the prevailing liquid-phase autocatalysis mechanism. Under acidic conditions, Cu(II) complexes exhibit enhanced catalytic capacity with decreasing ligand coordination strength, primarily stemming from the activation of PDS by Cu(I) species produced via the irradiation-induced intramolecular charge transfer; In alkaline environments, only liberated Cu(II) substantially contribute to SED effect via spontaneous hydrolysis, forming nanostructured CuO after aging, which activates PDS through heterogeneous Fenton-like processes. While acidic conditions demonstrate faster decomplexation, alkaline-generated solid products facilitate multi-cycle treatment efficiency and alkaline conditions also exhibits stronger resistance to chloride. This work corrects the misinterpretation of SED mechanism in UV/PDS/Cu(II)-EDTA system, and provides a fundamental and accurate mechanistic basis for the efficient treatment of copper-containing organic wastewater by PDS-based processes.
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Separations
·
2026
·Vol. 13
·期 5
·130
·
IF 3.5
Yanlin Wu,Lanhua Luo,Yuan Li,Shanghua Shi,Xiaoning Wang,Wenbo Dong,Gilles Mailhot
Over the past 20 years, the iron-activated persulfate systems have been widely used for removing pharmaceuticals and personal care products (PPCPs) from water. However, slow Fe(III)/Fe(II) redox cycling and precipitation of iron, unless in very acidic conditions, were the main limitations. Thus, two ligand-assisted Fe(III)/persulfate systems, Fe(III)-acetohydroxamic acid (AHA)/peroxydisulfate (PDS) and Fe(III)-nitrilotriacetic acid (NTA)/peroxymonosulfate (PMS), were comparatively investigated for the degradation of atenolol (ATL) in this study. The experimental results showed that the Fe(III)-NTA/PMS system worked much better than the AHA system. However, the cost of PMS is higher than that of PDS, which should be considered. The primary advantage of the NTA system was its ability to overcome the pH limitations. It worked well over a wide pH range (3.0–10.0), whereas the AHA system could only be used in a narrower pH window (pH 2.4 to 6.5). The investigation of radicals that contributed to ATL degradation revealed that sulfate radicals (SO4•−) were dominant in the NTA system, while hydroxyl radicals (•OH) and SO4•−were the primary and secondary radicals in the AHA system. These results provided useful insight into the comparative behavior of two ligand-assisted Fe(III)/persulfate systems for ATL degradation, with the Fe(III)-NTA/PMS system showing clear potential under neutral or near-neutral conditions, while Fe(III)-AHA/PDS may still represent a lower-cost option under acidic conditions.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yongchao Wang,Fancheng Meng,Yahui Liu,Yongqi Guo,Shuai Zhao,Desheng Chen,Lina Wang,Tao Qi
The chemical similarity between vanadium and chromium poses significant challenges for the selective extraction of V(IV) from Cr(III)-containing solutions to prepare high-purity vanadyl sulfate electrolyte. In this study, with EHEHPA employed as the extractant and the extraction equilibrium pH maintained at 2.5, the introduction of 1.00 mol/L sodium acetate into the solution effectively suppressed the extraction of Cr(III) while preserving the efficient extraction of vanadium achieving a separation factor of 29482. This introduction of acetate ion not only significantly enhanced the separation of vanadium and chromium but also effectively mitigated the precipitation of sodium salts at lower temperatures. Furthermore, after pretreatment of the water-leaching solution of sodium-roasted vanadium slag, extraction was carried out under the sodium acetate concentration of 1.00 mol/L, and the vanadyl sulfate electrolyte containing 2.12 mol/L of vanadium and only 2.17 mg/L of chromium was obtained after stripping. At low sodium acetate concentrations (≤ 0.05 mol/L), Cr(III) predominantly exists as [Cr(H 2 O) 6 ] 3+ , while at higher sodium acetate concentrations (e.g., 1.00 mol/L), Cr(III) primarily exists as [Cr(CH 3 COO) 2 (H 2 O) 4 ] + . Density functional theory calculations show that acetate ion readily complexes with Cr(III), forming a stable water-soluble complex. This complexation inhibits the extraction of Cr(III) by EHEHPA and enables efficient separation of vanadium and chromium.
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CHEMOSPHERE
·
2023
·
IF 8.8
Dingxi Zhang,Yuping Xiang,Guangliang Liu,Lina Liang,Lufeng Chen,Jianbo Shi,Yongguang Yin,Yong Cai,Guibin Jiang
Methylmercury (MeHg), derived from industrial processes and microbial methylation , is still a worldwide environmental concern. A rapid and efficient strategy is necessary for MeHg degradation in waste and environmental waters. Here, we provide a new method with ligand-enhanced Fenton-like reaction to rapidly degrade MeHg under neutral pH. Three common chelating ligands were selected (nitriloacetic acid (NTA), citrate, and ethylenediaminetetraacetic disodium (EDTA)) to promote the Fenton-like reaction and degradation of MeHg. Results showed that MeHg can be rapidly degraded, with the following efficiency sequence: EDTA > NTA > citrate. Scavenger addition demonstrated that hydroxyl radical ( ▪ OH), superoxide radical (O 2 ▪– ), and ferryl (Fe Ⅳ O 2+ ) were involved in MeHg degradation, and their relative contributions highly depended on ligand type. Degradation product and total Hg analysis suggested that Hg(Ⅱ) and Hg 0 were generated with the demethylation of MeHg. Further, environmental factors, including initial pH, organic complexation (natural organic matter and cysteine), and inorganic ions (chloride and bicarbonate) on MeHg degradation, were investigated in NTA-enhanced system. Finally, rapid MeHg degradation was validated for MeHg-spiked waste and environmental waters. This study provided a simple and efficient strategy for MeHg remediation in contaminated waters , which is also helpful for understanding its degradation in the natural environment.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Xuefeng Zhang,Yujie Zhang,Qin Yang,Yingchun Yang,Xuping Sun
Sulfate radical-based advanced oxidation processes (AOPs) are highly reliable for the elimination of recalcitrant contaminants by increasing degradability and reducing toxicity. Here, MnFe 2 O 4 nanowires (MnFe 2 O 4 NWs), composed of abundant MnFe 2 O 4 nanoparticles immobilized on one-dimensional carbon nanowires derived from annealed MnFe-Nitrilotriacetic acid (MnFe-NTA) precursor was successfully synthesized. The MnFe 2 O 4 NWs, which could provide more active sites, were then utilized to activate peroxymonosulfate (PMS) for oxidizing the target pollutant Moxifloxacin (MOX) in an aqueous solution. The MnFe 2 O 4 NWs/PMS system acquired 91.9% removal of MOX and achieved 55.1% chemical oxygen demand (COD) degradation efficiency in 30 min. The results exhibited that the increased catalyst doses and PMS concentration lead to ascending MOX removal rate, which decreased with the participation of co-existing ions. Besides, there is a close relationship between original pH and MOX degradation efficiency. It was found that SO 4 ⋅– , ⋅OH, 1 O 2 , and O 2 ⋅– were involved in the MOX degradation by quenching experiments and electron paramagnetic resonance (EPR) detection. More importantly, the stable magnetism of MnFe 2 O 4 NWs contributed to its convenient recycling. Finally, a reliable mechanism for activating PMS was proposed based on the aforementioned results and previous researches, which could exhibit a novel horizon in effluent treatment.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Xiaohong Zhou,Wenfeng Zhou,Wei Zhuang,Chenjie Zhu,Hanjie Ying,Hongman Zhang
Cytidine 5′-monophosphate (5′-CMP) is an essential nucleotide for additives. In this study, enhanced production of 5′-CMP was realized by the transformation of cytidine using co-immobilized di-enzymes, uridine-cytidine kinase (UCK) and acetate kinase (AcK). The immobilization yield of the enzyme had a clear correlation with the surface charges as zeta potential ( ξ ). Among them, ε -polylysine-functionalized sepharose (SA-EPL, ξ = 9.31 mV) showed high immobilization yield (78.8%), which was 4.9-fold than that of nitrilotriacetic acid functionalized sepharose (SA-NTA, ξ = −12.6 mV). The residual activity of affinity co-immobilized enzyme (EPL-Ni/ [email protected] ) was higher than 70.6% after recycled 10 times. Thus, this study provides an effective approach for the production of 5′-CMP with the advantages of low adenosine 5′-triphosphate (ATP) consumption, reduced side reactions, and improved reusability by co-immobilized UCK and AcK on the functionalized Sepharose.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ruoyun Lin,Fangjie Lv,Hao Zhang,Yang Li,Jiangang Lu,Jiansheng Li
Efficient removal of multiple pollutants from discharged antibiotic wastewater effluents by a single processing unit is highly desirable, yet challenging. In this study, intrinsically synergizing Fenton oxidation and in-situ coagulation were achieved in the tannic acid (TA)/Fe(III)/H 2 O 2 process, demonstrating the simultaneous removal of multiple pollutants over a wide pH range. Under the optimal conditions (TA/Fe(III)/H 2 O 2 = 25 mg/L/0.1 mM/0.5 mM), 95.43 % of SMR and 98.41 % of turbidity were simultaneously removed at pH = 7. Moreover, the applicability of this process was validated by treating a spiked actual secondary effluent. Compared with polymer ferric sulphate coagulation and conventional Fe(II)/H 2 O 2 Fenton, TA/Fe(III)/H 2 O 2 process exhibited significantly enhanced removal performance in terms of SMR, COD, UV 254 and turbidity without any pH adjustment. The mechanism analysis revealed that the introduction of TA can not only promote the iron redox cycle for the production of ∙OH, but also neutralize the charge for the generation of the porous flocs. Due to the bridging of TA, the synergy of Fenton oxidation and in-situ coagulation was achieved in a single processing unit. Finally, the synergy mechanism proposed that a four-step process sequentially proceeded during the treatment. This study may provide new insights into the simultaneous removal of multiple pollutants in the advanced treatment of refractory industrial wastewater.
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Batteries & Supercaps
·
2022
·Vol. 5
·期 11
·e202200335
·
IF 6.043
Yue Zhang,Tiancun Liu,Yaling Ji,Jianhua You,Chen Cai,Yi Wen,Zhujun Yao,Yefeng Yang
Graphical A functional artifical layer containing with plentiful polar oxygen sites and regular channels is constructed to alleviate the generation of Zn dendrites, corrosion and side reactions for stable and long-life Zn metal anode. Particularly, the functional sites and open structure are able to induce uniform Zn deposition. Aqueous zinc (Zn)-ion batteries (AZIBs) have attracted much attention for the high safety, economy and nontoxic property, but further practical applications are still hindered due to the severe interfacial corrosion and annoying dendrite growth. Herein, a functional protective layer (FPL) containing abundant oxygen sites and regular channels is proposed as the surface coating to stabilize the Zn-metal anode. Specifically, transferred free water molecules and mitigated Zn-ions can be attracted by these polar oxygen sites, beneficially reliving corrosion behavior, reducing side reactions and inducing uniform Zn deposition. Furthermore, the cross-linked structure with opening channels of FPL benefits electrolyte to quickly arrive the electrode surface and maintain the superior movement of Zn-ions. As a result, a superior cycling performance with high stability of 450 h at 5 mA cm −2 and excellent rate behavior have been endowed by Zn electrode loading FPL. In the exploration of practical utilization, full battery consisting of Zn@FPL anode and cathode adopting commercial MnO 2 powder also exhibits an outstanding capacity retention of 98.9 % after 300 cycles at 0.5 A g −1 . The proposed strategy of constructing a protective layer with functional sites and opening structure shows a good guiding significance for protecting Zn-metal anode.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yan Xiao,Liangliang Xiong,Yin Xu,Hui Zhang
In recent years, visible light assisted advanced oxidation processes (AOPs) are appealing in the elimination of pollutants. Herein, an innovative and eco-friendly visible light enhanced Fe 3+ -nitrilotriacetic acid system for the activation of peroxydisulfate (Vis/Fe 3+ -NTA/PDS) was proposed for the removal of bisphenol A (BPA). Fe 3+ -NTA could be dissociated through ligand-to-metal charge transfer (LMCT) to realize the generation of Fe 2+ for the continuous activation of PDS to remove BPA. The use of 0.10 mM Fe 3+ , 0.10 mM NTA and 1.00 mM PDS led to 97.5% decay of 0.05 mM BPA and 66.3% of TOC removal in 30 min with the illumination of visible light at initial pH 3.0. The sulfate and hydroxyl radicals were proved to be the dominant species leading to BPA removal by means of radical scavenging experiments, radical probes and electron paramagnetic resonance (EPR) technique. The effects of various operating parameters, natural water constituents as well as different water matrices on BPA abatement were explored. The intermediate products of BPA degradation were identified and a possible transformation pathway was proposed. Briefly, this research provides an attractive strategy for the remediation of refractory wastewater using NTA assisted with visible light in the homogeneous Fe 3+ /PDS system.
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DESALINATION
·
2022
·
IF 11.211
Ruonan Gu,Zhen Yu,Yi Sun,Yuqing Su,Wei Wu,Shaoan Cheng
Zero liquid discharge (ZLD) of high-salinity brine has attracted increasing attention recently. Interfacial solar crystallizers , which employ solar-driven water evaporation for salts crystallization from the near-saturation brine to achieve ZLD, are promising in ZLD due to low energy consumption and cost. However, many interfacial solar crystallizers were only used to treat high-salinity NaCl solution in the past while probably failing when treating high-salinity concentrated seawater. Here we explored the failure mechanism of the solar crystallizers in the high-salinity concentrated seawater and proposed a novel strategy to stably treat high-salinity concentrated seawater by combining a solar crystallizer with antiscalant (Nitrilotriacetic acid, NTA), taking Janus 3D solar crystallizer (Janus-3DSC) as an example. Janus-3DSC exhibited a stable average evaporation rate of 2.29 ± 0.36 kg m −2 h −1 under 1.5 sun in the 20.0 wt% concentrated simulated seawater containing NTA. The large-size Janus-3DSC could treat 20.0 wt% concentrated natural seawater containing NTA outdoors with a salt recovery rate of 11.27 kg m −2 day −1 and an evaporation rate of 18.63 kg m −2 day −1 . We believe that this work would provide a novel and effective way to achieve effective and eco-friendly ZLD of high-salinity concentrated seawater, even other high-salinity brine.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2022
·
IF 3.428
Yunfeng Lei,Xuezhong Zhang,Xiangyu Meng,Zhifei Wang
The removal of methylene blue (MB) with the magnetic separation in water treatment is of increasing attentions due to its high solubility and chemical stability, which poses a great challenge on the ecological environment and human health. Herein, with assistance of simplified modification strategies, multi-carboxyl functionalized Fe 3 O 4 @SiO 2 magnetic nanoparticles (mCMNPs) have been developed with a novel insight into the grafting densities effects on the adsorption process. The results of UV–Vis spectrometry obviously showed that the increased carboxyl content on the surface of CMNPs resulted in the significant improvement in the removal process of MB. Among different types of CMNPs, mCMNPs were chosen for the separation of MB owing to possessing the highest surface carboxyl densities 0.2363 mmol/g and exhibiting the highest removal efficiency of 96.18%. Several important factors including solution pH, initial MB concentration and sorption time were optimized to achieve the best removal efficiency. Desired adsorption capacity for MB (34.75 mg/g) was achieved using mCMNPs with the pH 10, sorption time of 100 min and initial MB concentration of 50 mg/L. The sorption isotherms and sorption kinetics can be well in agreement with the Langmuir model and pseudo-second-order kinetic model, respectively. Most importantly, the synthesized mCMNPs still exhibited high removal efficiency (63%) after 5 cycle numbers. As adsorbents, it is noted that the prepared mCMNPs possessed the excellent regeneration ability and recyclability and could be a promising adsorbent for the removal of MB in water treatment.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Jiali Gu,Xiyao Huang,Yanxuan Ma,Xuekai Sun
Metabolites affect the binding mechanism between parent drug and transport protein. The effects of the metabolite nicotinamide (NTA) on the interaction mechanism of the antihyperlipidemic drug nicotinic acid (NA) with bovine serum albumin (BSA) were investigated through fluorescence spectroscopy, UV–Vis spectroscopy and FT-IR spectroscopy along with molecular docking. The fluorescence quenching results revealed that the NA/NTA bound to BSA in 1:1 stoichiometry with binding constants of K b (NA-BSA) = 2.19 × 10 3 L·mol −1 and K b (NTA-BSA) = 5.82 × 10 3 L·mol −1 , respectively. The results of thermodynamic experiment (Δ H , Δ S and Δ G ) showed that NA bound spontaneously with BSA through entropy driven hydrophobic interaction. The binding of NA/NTA caused conformational changes in BSA molecule, as proved by FT-IR spectroscopy, UV–Vis spectroscopy and synchronous fluorescence spectroscopy. The site marker experiment and molecular docking suggested that NA/NTA located in site I of BSA. The presence of metabolites did not significantly change the effect of sodium on the conformation of BSA, but increased the binding constant of NA and BSA.
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