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
·
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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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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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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Nanoscale
·
2022
·Vol. 14
·期 7
·2676-2685
·
IF 8.307
Haolu Hu,Xiaoxia Kang,Zhenhua Shan,Xiaoxiao Yang,Wei Bing,Li Wu,Haiyan Ge,Haiwei Ji
The construction of multifunctional nano-enzymes is a feasible strategy for fighting multi-drug resistant (MDR) bacterial biofilm-associated infections. Extracellular DNA (eDNA) is an important functional part of biofilm formation, including the initial adherence of bacteria to subsequent development and eventual maturation. A nano-enzyme platform of graphene oxide-based nitrilotriacetic acid-cerium(IV) composite (GO-NTA-Ce) against bacterial biofilm infection has been developed. When located at the site of bacteria-associated infection, GO-NTA-Ce could inhibit the biofilm formation and effectively disperse the formed biofilm by degrading the eDNA. In addition to Ce-mediated deoxyribonuclease (DNase)-like activity, near-infrared laser irradiation of GO-NTA-Ce could produce local hyperthermia to kill the bacteria that lost the protection by the biofilm matrix. In addition, graphene is also a new green broad-spectrum antimicrobial material that can exert its antimicrobial effects through physical damage and chemical damage. In short, our GO-NTA-Ce nano-enzyme platform is capable of effectively eradicating drug-resistant bacterial biofilm infections through the triple action of DNase-like enzyme properties, photothermal therapy, and graphene-based antimicrobial activity, and the nano-composite has excellent potential for the treatment of MDR bacterial biofilm infections.
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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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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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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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Batteries & Supercaps
·
2021
·Vol. 5
·期 1
·e202100203
·
IF 7.093
Yaqian Dong,Yaohui Zhang,Nana Wang,Guifu Zou,Qiang Zhang,Shengquan Gan,Liang He,Zhongchao Bai
Graphical Materials for better SIB anode : The synergistic effects of the one-dimensional N-doped carbon and ultra-small Fe 7 S 8 particles in the reported pod-like Fe 7 S 8 @N−C nanocomposite, improve electrical conductivity and alleviate the volume expansion of the anode of SIB during cycling. One dimensional Fe 7 S 8 @N−C nanocomposite, consisting of Fe 7 S 8 nanoparticles homogeneously embedded in N-doped carbon nanowires, was synthesized by a facile hydrothermal-annealing process. As an anode material for sodium-ion batteries, the electrode exhibited capacities of 481 mA h g −1 after 1000 cycles at 5 A g −1 and 591 mA h g −1 at 200 mA g −1 with a retention ratio of 91 %. The excellent rate performance and cycling stability can be attributed to the synergistic effects of the one-dimensional N-doped carbon and ultra-small Fe 7 S 8 particles, which will improve electrical conductivity and alleviate the volume expansion of the electrode during cycling. This work will afford a great reference for further development of iron sulfides-based anode materials towards high-performance sodium-ion batteries.
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GREEN CHEMISTRY
·
2021
·Vol. 23
·期 19
·7594-7608
·
IF 10.182
Yuanyuan Wang,Linlin Zhang,Yongjian Niu,Dong Fang,Jiao Wang,Qingxiao Su,Cheng Wang
Clear structure–performance relationships are helpful for the design of efficient catalysts and the understanding of reaction mechanisms. The electrocatalytic nitrate reduction reaction (NO3RR) offers a sustainable route to ammonia (NH3) synthesis and nitrate mitigation. However, it suffers from poor nitrate adsorption, low NH3 selectivity and sluggish reaction kinetics. Herein, N-doped carbon nanosheets supported Fe3C nanoflakes featuring large surface areas (860.024 m2 g−1) were prepared. Their NO3RR performances showed volcano-like relationships with the Fe3+/Fe2+ ratios and d-band centers. At −0.5 V, the NH3 yield, faradaic efficiency, selectivity and current density reached 1.19 mmol h−1 mg−1, 96.7%, 79.0% and 85.6 mA cm−2, respectively, exceeding most reported results. Such exceptional performances mainly originated from the optimized electronic structures that boosted nitrate adsorption and reaction kinetics (Tafel slope: 56.7 mV dec−1). Mechanistic investigations revealed a NO3− → NO2− → NH3 reaction pathway with the chemical process following the fast electron transfer process as the rate-determining step.
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