CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Mingchun Bi,Yuning Liang,Weimeng Chi,Hongya Liu,Ying Chen
Nano zero-valent iron (nZVI) is extensively employed in the realm of wastewater treatment. However, conventional synthesis methods involve inherent risks of nZVI oxidation and aggregation, resulting in challenging recovery and potential waste generation. To address these concerns and improve stability, nano zero-valent nickel (nZVNi) was employed as a modifier for nZVI. The modified nZVNi/nZVI was successfully blended with polydopamine (PDA)-modified polyvinylidene fluoride (PVDF) powder, enabling the preparation of a novel hydrophilic composite membrane termed nZVNi/nZVI-PDA@PVDF (NFPP). PDA played a crucial role in effectively immobilizing nZVI particles and preventing their oxidation and aggregation. Scanning electron microscopy was used to confirm the consistent dispersion of nZVNi/nZVI particles both on the surface of the membrane and within its pores. Moreover, the NFPP membrane exhibited excellent performance in removing Cr(VI), with a maximum adsorption capacity of 75.65 mg/g. The presence of PDA endowed the NFPP membrane with a plentiful supply of hydroxyl and amino groups, enhancing its hydrophilicity, antioxidation properties, and loading capacity for nZVNi/nZVI. Additionally, the NFPP membrane demonstrated remarkable resistance to interference under different pH and ionic conditions. The removal of Cr(VI) by the NFPP membrane followed a pseudo-second-order kinetics and Langmuir isotherm adsorption model. Furthermore, the NFPP membrane retained good performance and stability in Cr(VI) removal even after undergoing five cycles. This study indicates that the highly efficient NFPP composite material holds promising potential for application as a functional material in heavy metal wastewater treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Tiantian Li,Zhining Huang,Mengfan Hu,Yuen Hu,Ke Quan,Man Zhou,Yao chen,Shaoju Fu
Heavy metal wastewater pollution has been a globally important and serious issue for the industrial manufacturing center. Herein, we developed a novel CAP@Ui0-66-NH 2 @PPy nanocomposite fibrous membrane, by combining the in-situ growth and oxidative polymerization technical routes, which possessed a high specific surface area and abundant amino-active sites to remove Cr (Ⅵ). Systematic characterization showed that the porous structure and in situ growth of MOF provided sites for polymerization of charged polypyrrole (PPy), resulting in the large specific surface area (78.837 m 2 /g) of CAP2@Ui0-66-NH 2 @10 %PPy. The maximum adsorption capacity was as high as 312.70 mg/g at 298 K, which was significantly better than that of CAP (CA and PVP electrostatic spinning and then washing off the PVP) nanomembranes. The adsorption process was consistent with the proposed secondary kinetic and Langmuir model, and the high adsorption capacity was maintained after five rounds of cyclic adsorptions. Through XPS analysis, the abundant amino groups on the surface of the adsorbent material were protonated, caused the electrostatic attraction and ion-exchange interaction with the anion Cr(Ⅵ). These protonated amino groups were able to reduce the toxic Cr (Ⅵ) to non-toxic Cr (Ⅲ), which was immobilized on the surface of the material through chelation. The MOF lattice achieved in-situ growth on porous CA nanofibrous membranes, which significantly enhances the mass-transfer dynamics and the membrane cycling stability, the amine-based functionalization of the UI0-66-NH 2 improved the coordination activity and increased the adsorption efficiency, and polypyrrole (PPy) conductive layer promoted the directional migration of Cr (VI) and effectively suppressed the interference of competing ions. In sum, the prepared CAP@Ui0-66-NH 2 @PPy hybrid fibrous membranes showing great potentially applicable for heavy-metal wastewater treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Chundi Zhou,Minghao Sui,Yali Guo,Songhang Du
Efficiently removing hexavalent chromium (Cr(VI)) using iron-based adsorbents under neutral pH conditions continues to pose a challenge. In this study, we constructed nano zero-valent iron (nZVI) supported by carboxylated multi-walled carbon nanotubes (OCNT) composites with iron-based dual active sites through the nitrilotriacetic acid modification (FOC-NA). The acid dissolution experiment, high-resolution transmission electron microscopy (HRTEM), thermogravimetric analyzer (TGA), X-ray photoelectron spectroscopy (XPS), and Raman analysis proved these active sites consisted of iron-carboxylate complex (−COOFe(II)) and OCNT-confined nZVI (Fe 0 -in-OCNT). The existence of iron-based dual active sites enhanced electron transfer efficiency in Cr(VI) removal under neutral pH conditions. This leaded to a superior adsorption capacity for Cr(VI), as evidenced by a maximum adsorption capacity of 141.29 mg·g −1 at a pH of 6.5. Meanwhile, the formation of a Cr-containing product (−COOFe-O-Cr) on the surface of FOC-NA substantially hindered the re-release of chromium into the environment. Furthermore, this study proposed the significant involvement of active hydrogen atoms (H*) in the reduction of Cr(VI), as confirmed by quenching experiments and analyses using electron spin resonance (EPR), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). The formation pathway and energy barrier of H* and the −COOFe-O-Cr complex were analyzed by density functional theory (DFT) calculations. This study provided insights for the rational design of iron-based adsorbents with dual active sites to facilitate the activation of H* for Cr(VI) reduction under neutral pH conditions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuyu He,Shaohua Chen,Liwen Zhang,Shanyi Tan,Huizi Wen,Luyao Xi,Xiangru Zuo,Dongyun Du
Dissimilatory iron-reducing bacteria (DIRB) offer an eco-friendly approach to address nanoscale zero-valent iron (nZVI) surface passivation problem, yet their efficacy is limited by the slow direct extracellular electron transfer (EET) between DIRB and Fe(III) oxide passivation layers (Fe( III )OPL). This study demonstrates that natural dissolved humic substances (DHS)-mediated electron shuttling unlocking nZVI reactivity in Shewanella oneidensis MR-1 (MR-1) system for enhance Cr(VI) removal. Seven DHSs from diverse sources were evaluated, revealing that Cr(VI) removal rate constants ( k obs ) correlate strongly with DHS's quinone content (C=O) and electron transfer capacity (ETC), quantified as k obs = 1.66 C C = O − 9.39 ( P < 0.0007) and k obs = 19.37 ETC + 0.74 ( P < 0.0005). DHS-mediated systems achieve 2.0–12.1-fold higher k obs than nZVI/MR-1 alone. The enhancement mechanism of DHS-mediated Cr(VI) removal by nZVI/MR-1 is that DHS effectively facilitates Fe( III )OPL dissolution on the nZVI surface via electron shuttling, maintaining nZVI reactivity and amplifying Fe(II) generation by 1.65-fold. Moreover, DHS stimulates MR-1 to secrete more extracellular polymeric substances (EPS), enhancing Cr(VI) adsorption and reduction. This work elucidates DHS's dual role in maintaining nZVI activity and amplifying Cr(VI) removal by nZVI/MR-1, while establishing a predictive framework linking DHS molecular traits parameters to Cr(VI) removal kinetic, offering sustainable strategies for heavy metal-contaminated water bodies remediation by integrating biogeochemical and material engineering principles.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Jie Zhang,Ting Hu,Shen Tang,Yanhong Li,Huanlong Liu
This study elucidates the mechanism by which hexavalent chromium [Cr(VI)] synergistically promotes malathion biodegradation in Shewanella oneidensis MR-1. Exposure to 5 mg/L Cr(VI) significantly enhanced the malathion degradation rate by 2.3-fold, achieving 96.79 % removal within 72 h under optimized conditions (5 % inoculum, pH 6). Analysis of cell membrane parameters combined with microscopic observation techniques indicated that Cr(VI) induced biofilm densification and membrane lipid peroxidation. Metabolomic profiling identified three critical Cr(VI)-activated pathways: (1)tryptophan-mediated redox homeostasis, (2)sulfur assimilation for antioxidant substances biosynthesis, and (3)cofactor biosynthesis for electron transport optimization. These metabolic adaptations increased membrane permeability and accelerated reactive oxygen species diffusion. The findings highlight Cr(VI) as a metabolic modulator that reprograms microbial catabolism via redox signaling, providing a mechanistic basis for developing biocatalysis strategies in multi-pollutant environments.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zhonglei Xu,Xuejiao Zhang,Xinying Li,Hao Zha,Jun Chen
Chromium (Cr(VI)) and phosphate contaminants in wastewater pose severe threats to ecosystems and human health. To address this challenge, we engineered a novel molecular-scale organic-inorganic hybrid material (Lys-HZO) through facile integration of lysine (Lys) with hydrated zirconium oxide (HZO). The uniform anchoring of Lys within the HZO framework significantly enhances the material’s hydrophilicity, improving the accessibility of adsorption sites both internally and externally, thus overcoming the structural limitations of traditional HZO materials. The amino and hydroxyl groups in the material create a synergistic effect through multiple mechanisms, including electrostatic attraction, ligand exchange, and redox interactions, which collectively drive the adsorption process. Batch adsorption experiments showed that the material’s adsorption capacities for Cr(VI) and phosphate were 15 and 10 times higher, respectively, than those of pure HZO. Kinetic and isothermal adsorption analyses confirmed that adsorption is primarily governed by chemisorption, while thermodynamic studies indicated the adsorption process’s spontaneous and endothermic nature. In cyclic fixed-bed column experiments under competitive ion conditions, Lys-HZO demonstrated high adsorption capacity, treating 2532 bed volumes (BV) of phosphate-containing wastewater (3 mg P/L) and 726 BV of Cr(VI)-contaminated effluent (3 mg Cr(VI)/L). The treated effluent concentrations remained below regulatory limits: < 0.5 mg P/L and < 0.2 mg Cr(VI)/L, respectively. The innovative design strategy of "molecular-scale hybridization and site synergistic activation" proposed in this study not only fully unlocks the adsorption potential of HZO materials, but also provides novel insights for developing amino acid-functionalized metal oxide hybrid materials in the field of water treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Li Song,Chunping Su,Hui Li,Huiping Zhao,Rong Chen
To achieve an effective and straightforward method for Cr(VI) removal from industrial wastewater, a composite Bi 2 S 3 /PDA/PEI material (BSPP) was successfully prepared through in-situ polymerization of polydopamine (PDA) followed by chemical grafting with polyethylenimine (PEI) on the surface of Bi 2 S 3 materials for round-the-clock highly efficient Cr(VI) removal from actual industrial electroplating wastewater. Under dark conditions, the maximum adsorption capacity of Cr(VI) by BSPP reaches 780.75 mg/g. Interestingly, when exposed to light, the maximum Cr(VI) removal capacity was further increased to 1333.21 mg/g. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma optical emission spectrometry (ICP-OES) analyses indicate that BSPP not only reduces Cr(VI) to Cr(III) under light condition, but also facilitates the significant decrease of total chromium content. Notably, under natural sunlight exposure outdoors, BSPP is capable of completely eliminating Cr(VI) from both plating cleaning solutions and waste plating solutions. More importantly, BSPP maintains its original Cr(VI) removal efficiency after nine cycles within plating cleaning solutions and six cycles within waste plating solutions. Large-scale testing results indicate that BSPP can effectively treat substantial volumes of electroplating wastewater to comply with national Cr(VI) discharge standards. These findings suggest that BSPP represents a promising material for continuous 24-hour Cr(VI) treatment in industrial electroplating wastewater.
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高影响因子
Frontiers of Chemical Science and Engineering
·
2020
·Vol. 15
·期 3
·538-551
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IF 3.552
Deng Xiaoyan,Wang Luxing,Xiu Qihui,Wang Ying,Han Hong,Dai Dongmei,Xu Yongji,Gao Hongtao,Liu Xien
In this work, an adsorbent, which we call MnPT, was prepared by combining MnO 2 , polyethylenimine and tannic acid, and exhibited efficient performance for Cu(II) and Cr(VI) removal from aqueous solution. The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation. The maximum adsorption capacities of MnPT for Cu(II) and Cr(VI) were 121.5 and 790.2 mg·g −1 , respectively. The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(II) and Cr(VI) co-adsorption on MnPT. Electrostatic force, solvation action, adsorbate-adsorbate lateral interaction, and complexation were involved in the spontaneous adsorption process. Physical electrostatic action was dominant in the initial stage, whereas chemical action was the driving force leading to adsorption equilibrium. It should be noted that after adsorption on the surface of MnPT, Cr(VI) reacted with some reducing functional groups (hydroxylamine-NH 2 ) and was converted into Cr(III). The adsorption capacity declined by 12% after recycling five times. Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents. This MnPT nanocomposite has been proven to be a low-cost, efficient, and promising adsorbent for removing heavy metal ions from wastewater.
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高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Qiang Qu,Ling Qiu,Ming-Zhuo Li,Guo-Tao Sun,He-Yu Chen,Xiao-Hui Guo
Magnetic biochar was successfully prepared from the waste Zanthoxylum branch and applied for Cr (VI) removal from wastewater. Modification parameters including concentration of iron-containing solution, ratio of Fe (III)/Fe (II), and pyrolysis temperatures were systematically investigated. There was a synergistic effect of synthesis conditions on the porous structure and the form distribution of iron. Based on the adsorption experiments, 900MZB8–1 displayed the best Cr (VI) removal performance (42.68 mg/g). The fitting result confirmed that the Cr (VI) removal reaction was the homogeneous chemisorption , and the predicted maximum removal capacity could reach at 215.44 mg/g. Moreover, the XPS analysis indicated that 79 % of Cr (VI) on adsorbent surface was transformed to Cr (III) by the cooperation of oxygen-containing functional groups and reductive iron. Meanwhile, 900MZB8–1 maintained the eminent removal efficiency of 80.65 % after four regeneration cycles. Additionally, the economic feasibility and practical performance indicated the rich-potential adsorbent for Cr (VI) removal.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Qiong Sun,Bing Han,Kaijing Li,Liyan Yu,Lifeng Dong
Photocatalytic fuel cell (PFC) is a novel energy conversion device that can effectively convert light into chemical energy and then electrical energy, accompanied with the pollutant purification treatment by photocatalytic technology. In this study, the synergetic photocatalytic degradation of organic dye in anode and the reduction of heavy metal Cr(VI) in cathode are carried out in an improved dual-chamber PFC device with TiO 2 and core–shell structured Ag@Fe 2 O 3 nanoparticles as photoanode and cathode materials , respectively. Among different materials, Ag@Fe 2 O 3 shows the highest catalytic activity to the reduction of Cr(VI) with an apparent kinetic constant of 0.058 min −1 , even much better than commercial Pt foil (0.027 min −1 ). From morphology and electrical characterizations, the excellent electrical conductivity of noble metal Ag and suitable conduction band positions between TiO 2 and Fe 2 O 3 lead to a rapid and directional transfer of photoinduced electrons, and the variable valence of Fe(II)/(III) in iron oxide facilitates continuous catalytic reduction of Cr(VI) to Cr(III). Moreover, the addition of H 2 O 2 into anode chamber can significantly accelerate the reactions and electricity output. The radical quenching tests prove that the existence of H 2 O 2 can efficiently increase the production of photoinduced carriers, and more oxidizing species (such as O 2 − and OH) can be produced from the reactions between H 2 O 2 and photoinduced holes or electrons.
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Cheng-Feng Liang,Song-Hai Wu,Yu-Le Wang,Zhi Xu,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,Xu Han
Thiosulfate (S 2 O 3 2− ) is an important ligand to complex metal cations, however, the reactivity of metal-thiosulfate complexes has barely been mentioned. In this study, the reactivity of the Cu(II)–S 2 O 3 2− system in the reduction of Cr(VI) was investigated. Kinetic results show that the reduction rates of Cr(VI) decrease with increasing pH values from 3.0 to 5.0, and 94.3% and 97.5% of 10 mg L −1 Cr(VI) was rapidly reduced within 1 min at pH 3.0 and within 30 min at pH 5.0, respectively at the molar ratio of Cu(II):S 2 O 3 2− of 0.05. We rule out the contributions of S species of tetrathionate (S 4 O 6 2− ) and sulfite (SO 3 2− ) to Cr(VI) reduction and point out that the produced Cu(I) in the Cu(II)–S 2 O 3 2− system is the key reductant that mediates the reduction of Cr(VI). We suggest that complexation between Cu(II) and S 2 O 3 2− with the formation of Cu II (S 2 O 3 ) 2 2− is the pre-requisite for the formation of Cu I (S 2 O 3 ) n 1−2n , which plays an important role in Cr(VI) reduction, accompanied by the re-oxidation of Cu(I) to Cu(II) by Cr(VI), achieving the rapid redox cycling of Cu(II)–Cu(I)–Cu(II). Such a redox cycle also mediates the denitrification process of NO 2 − to NH 3 /NH 4 + under weakly acidic conditions. This study enriches our understanding on the reducing reactivity of the Cu(II)–S 2 O 3 2− system and the importance of the Cu(II)–Cu(I)–Cu(II) redox cycle towards environmental oxidizing contaminants.
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PubMed
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Jiaxing Yu,Qi Fu,Huangsheng Yang,Junhui Wang,Gangfeng Ouyang,Zhengping Hao
Highly resistant organic pollutants and heavy metals (such as hexavalent chromium (Cr(VI)) usually coexist in industrial wastewater. However, efficient synergistic removal of them is still challenging in practical applications, due to low efficiency and high energy input required for this process. In this study, the metal-free multiwalled carbon nanotubes (MWCNTs) are demonstrated to simultaneously remove bisphenol A (BPA) and Cr(VI) without any external energy or chemical input. In this novel synergistic removal system, the catalytic performance is even higher than those of most of the reported metal-based catalysts in photo/electrocatalytic systems. The catalytic performances are negligibly affected by ions and humid acid, indicating applicability of the catalyst in actual wastewater. In addition, the MWCNT catalyst exhibits good recyclability after thermal treatment under inert atmosphere. Furthermore, the catalytic mechanism of this system has also been comprehensively investigated. This MWCNT-activated synergistic organic pollutants–Cr(VI) elimination system provides a novel and cost-effective strategy of “waste control by waste” for removing multiple industrial contaminants.
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