ENVIRONMENTAL RESEARCH
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2024
·
IF 7.7
Wenfei Ding,Zhaoyi Mo,Jia Qi,Mengying Wang,Junyu Zou,Kuo Wang,Daxiang Gong,Yongju Zhao,Hong Miao,Zhongquan Zhao
Cr(Ⅵ) residues in livestock and poultry wastewater are a rising concern for human health and biotic environments. For the removal of Cr(Ⅵ), its simultaneous reduction and adsorption represents a sustainable and efficient strategy. Herein, iron nodes on covalently bonded two-dimensional phthalocyanine organic polymer (PcOP-Fe) nanosheets with space-separated dual-active sites are developed for the simultaneous detection and removal of Cr(VI) from wastewater. In the FeN 4 structure of PcOP-Fe nanosheets, Fe acts as an electron capture center, effectively facilitating the accumulation of photogenerated electrons and transferring them to Cr(VI), thereby achieving its photocatalytic reduction. Meanwhile, pyrrolic nitrogen provides excellent adsorption sites, enabling the adsorption of Cr(III) or Cr(0). Fe accumulates the photogenerated electrons from pyrrole N and transfer them to Cr(Ⅵ). The formation of N-Cr(Ⅲ) bonds causes a space-separation between Cr(Ⅵ) and Cr(III). In addition, PcOP-Fe can be used for a Cr(Ⅵ) detection agent. The photoluminescence intensity decreases linearly with increasing Cr(Ⅵ) concentration from 80 μM to 2 mM, with a limit of detection of 0.18 μM. The PcOP-Fe nanosheets exhibit good Cr(Ⅵ) detection and reduction performance in livestock and poultry wastewater, suggesting their suitability for practical sensing applications. Thus, the PcOP-Fe nanosheets with space-separated dual-active sites are promising for the simultaneous detection and removal of Cr(Ⅵ) in water treatment processes.
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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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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zijun Xu,Ruoxin Ma,Chun Zhang,Jiao Chen,Jingbiao Fan,Qingdong Shi
Cr(VI) pollution in water caused by industrialization poses a serious threat to human health and ecosystems, necessitating a rapid reduction of Cr(VI) treatment method. Therefore, We have established a photocatalytic method for the rapid reduction of Cr(VI) by modifying TiO 2 with carbon dots (CPC-CDs) that possess a quaternary ammonium structure in the first time. The CPC-CDs widens the band gap of TiO 2 and increases the electrostatic interactions between CPC-CDs/TiO 2 and Cr(VI), thus improving the reduction efficiency. CPC-CDs/TiO 2 (0.1 g, 2 % CPC-CDs) exhibited excellent reduction performance and fully reduced Cr(VI) (50 mg/L) under neutral conditions within 150 min using a xenon lamp to simulate sunlight. Moreover, CPC-CDs/TiO 2 achieved more than 95 % reduction efficiency over a wide pH range (pH = 3, 5, 7, and 9) and showed excellent reduction of Cr(VI) at various concentrations (10, 20, 30, 40 and 50 mg/L). CPC-CDs/TiO 2 maintained high Cr(VI) reduction efficiency (93.57 %) after five cycles. Tests under real sunlight revealed that CPC-CDs/TiO 2 thoroughly reduced Cr(VI) (10 mg/L) within 30 min, and exhibited excellent structural stability under conditions with interfering ions. Furthermore, CPC-CDs/TiO 2 exhibited prominent antibacterial activity against Escherichia coli . In addition, free-radical trapping experiments verified that the superoxide radicals (• O 2 - ) was the main active species. This study aims to overcome the limitations of photocatalytic reduction under conditions of high concentration Cr(VI), neutral and alkaline environments, and natural sunlight, thereby providing technical support for the rapid reduction of Cr(VI).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bing Hou,Ling Wang,Xinyu Yang,Yuyou Li,Zhuohang Wu,Jingwen Pan,Lei Wang
Cerium-based adsorbent with the merits of variable valence and ample oxygen vacancies was applied for the removal of highly toxic hexavalent chromium (Cr(VI)). However, its cost controllability and recycling stability in practical applications remain to be further explored. Herein, a varieties of bimetallic cerium-based biochar adsorbents (CeFe@BC) were prepared by doping iron (Fe) and loading onto straw-based biochar, and the effects of the introduced Fe and biochar on adsorption performance of cerium-based adsorbent for Cr(VI) were studied. In comparison to pure cerium-based adsorbent (Ce@C), CeFe@BC had a stronger Cr(VI) adsorbability with the maximum adsorption capacity of 57.05 mg/g (25°C). Meanwhile, CeFe@BC had good regeneration stability and environmental friendliness. The adsorption capacity only decreased by 16.11 % after 7 adsorption–desorption cycles, with almost no metal leaching in different pH. Results showed that Fe doping and loading onto straw-based biochar could effectively promote Ce(III) and oxygen vacancy content in Ce@C. Electrochemical and density function theoretical calculations proved that Fe doping and loading onto straw-based biochar could promote the reduction of Ce@C impedance and the increase of current density. In conclusion, Fe doping and loading onto straw-based biochar effectively regulated the intrinsic properties of cerium adsorbent and further accelerated the electron transfer in adsorption. This study shows that bimetallic cerium-based adsorbent is a promising, efficient and stable environmental friendly adsorbent for Cr(VI) removal from wastewater.
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INDUSTRIAL CROPS AND PRODUCTS
·
2024
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IF 5.6
Jianshuo Miao,Quanling Zhao,Lijun Qian,Kehao Fan,Jialong Wen,Liuting Mo,Zhiyong Qin
Wastewater with chromium is a common heavy metal pollution in industrial pollution, affecting health of human seriously, while adsorption and photocatalysis are efficient for Cr(Ⅵ) removal. The multi-layer lignin core-shell structure materials were prepared with kraft lignin/polydopamine core-shell structure material, using non-covalent bonding to induce the in-situ induction of TiO 2 . The hydroxyl group of kraft lignin and the amino group of polydopamine provided abundant adsorption active sites with adsorption capacity being 299 mg/g at pH of 2. The adsorption process conformed to the Freundlich isotherm model and the pseudo-second-order kinetic model. The removal rate of Cr(Ⅵ) reached more than 99.9 % within 10 min under simulated solar light with influence of adsorption and photocatalysis. The multi-layer lignin core-shell structure materials presented excellent antibacterial activity, with the inhibition rate against S.aureus and E.coli being 40 % under dark conditions and 99 % under simulated solar light because h + or ·OH producing by TiO 2 . The antibacterial multi-layer lignin core-shell structure materials showed good universality in water pollution treatment.
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Journal of Environmental Chemical Engineering
·
2025
·
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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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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SENSORS
·
2025
·Vol. 25
·期 10
·3228
·
IF 3.5
Lihua Zhang,Jiang Li,Juan Wang,Xu Yan,Jinping Song,Feng Feng
HighlightsWhat is the main findings?ATG-functionalized AuNPs were prepared as a colorimetric chemosensor with ultra-sensitivity for the simultaneous detection of MOX/CIP and Cr(III).What are the implications of the main findings?ATG-AuNPs sensor color transitions from wine-red to gray-blue indicated successful detection.The detection limits for MOX/CIP and Cr(III) are 1.57 µM, 1.30 µM, and 57.1 nM, respectively.The presented method was used to detect multiple analytes in lake and tap water samples.Water pollution by antibiotics and heavy metals threatens the ecological environment and human health globally, yet there is no rapid method to detect multiple antibiotics and metal ions simultaneously. A simple, fast, and ultra-sensitive colorimetric chemosensor for the simultaneous detection of moxifloxacin (MOX), ciprofloxacin (CIP), and Cr(III) based on the aggregation of ammonium thioglycolate (ATG)-functionalized gold nanoparticles (ATG-AuNPs) was developed. Following the addition of MOX, CIP, and Cr(III), a color change in the solution was observed from wine-red to blue-grey. The UV–Vis signal of the ATG-AuNPs system blended with MOX, CIP, and Cr(III) in the range of 0~200 µM, 0~100 µM, and 0~5 µM was assessed and measured with detection limits (LODs) of 1.57 µM, 1.30 µM, and 57.1 nM calculated by 3σ/S, respectively. Therefore, this system has the potential to act as an effective colorimetric chemosensor for simultaneously detecting MOX, CIP, and Cr(III) in complex environmental systems.
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LANGMUIR
·
2025
·
IF 3.9
Changhua Li,Wei Liu,Yuquan Jing,Hao Yang,Qiuping Tang,Yongxu Cui,Chao Zhang,Wei Ren,Jing Zhang,Yi He
Metal–organic framework materials with large specific surface areas are ideal choices for storing corrosion inhibitors in organic coatings. Existing reports focus on materials such as ZIF-8 and ZIF-67, which release corrosion inhibitors by disintegrating themselves upon external stimuli. This release mechanism may lead to the formation of holes within the coating, providing channels for penetration into corrosive media. In this study, NH2-MIL 101 (Cr), which is stable under acidic/alkaline conditions, was grown on Ti3C2Tx surface via a hydrothermal method. Its porous structure was utilized to load environmentally friendly MoO42– corrosion inhibitors, and a stimulus-responsive TEOS shell was wrapped as a valve to control the release of the corrosion inhibitors. The synthesis of the Ti3C2Tx-MIL 101-MoO42–-TEOS (TMIT) composite material was verified by FT-IR spectroscopy and XPS, respectively. The TMIT-epoxy (TMITP) composite coating was prepared through a solid–liquid mixing method. The surface-active groups of NH2-MIL 101 (Cr) (−NH2) enhanced the interfacial strength with the resin and the crosslinking density, significantly increasing the tensile strength and adhesion strength of the composite coating. Due to the improved interfacial strength, the low-frequency impedance value remained at 4.14 × 108 Ω cm2 after 6 cycles of accelerated cyclic electrochemical tests (−4.0 V, 30 min), which greatly shortening the evaluation period of the coating performance. Additionally, the stimulus-responsive release mechanism of the TMIT filler endowed the coating with self-healing effects, achieving corrosion inhibition in damaged areas. Notably, the acid/alkali stability of NH2-MIL 101 (Cr) ensured that few holes would form within the coating after the release of corrosion inhibitors, preventing the penetration of corrosive media. This study utilized the pores of NH2-MIL 101 (Cr) to load corrosion inhibitors and prepare self-healing composite coatings, achieving intelligent release and enhancing the corrosion resistance of coatings, thus broadening the application strategy of MOF materials in corrosion protection coatings.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Guona Bai,Xu Wu,Mengqun Li,Zihao Zhao,Mengqing Wang,Xinyu Wang,Jiangang Gao,Zongrui Zhang
To address the synergistic removal of Congo Red (CR) and hexavalent chromium (Cr(VI)) from industrial wastewater, this study proposed an “electrospinning-surface modification” strategy. Using poly(vinyl alcohol-co-ethylene) (PVA-co-PE) as the substrate, a dual-functional composite nanofibrous membrane adsorbent (PVA-co-PE/chitosan (CS)/polydopamine (PDA)) was constructed via CS grafting and PDA coating. The structural and physicochemical properties of the PVA-co-PE/CS/PDA NF membranes were characterized by elemental mapping, spectroscopic analyses, and morphological observation, while batch experiments were conducted to investigate the adsorption behavior and key influencing factors. Results showed that the composite membrane exhibited maximum adsorption capacities of 716.9 mg/g for CR and 264.4 mg/g for Cr(VI), with the adsorption process conforming to the Langmuir monolayer adsorption model and pseudo-second-order kinetic model (dominated by chemical adsorption). After four adsorption–desorption cycles, the membrane retained adsorption capacities of 609.3 mg/g for CR and 224.5 mg/g for Cr(VI), demonstrating excellent cyclic stability. With advantages of simple preparation, strong recyclability, and negligible secondary pollution, the proposed composite membrane serves as a novel, efficient adsorbent for the synergistic advanced treatment of organic dyes and heavy metal ions in complex industrial and holds substantial engineering application value.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Beibei Zhao,Jingchun Tang,Honghong Lyu,Feng Liu,Lan Wang
Low molecular weight organic acids with low cost and environmentally friendly characteristics can enhance the electron transfer between materials and contaminants. In this study, oxalic acid (OA), citric acid (CA), and ethylenediaminetetraacetic acid (EDTA) were selected to strengthen ball milled natural FeS 2 /biochar composite (FeS 2 /biochar) for aqueous Cr(VI) removal. 100% of Cr(VI) was removed when 5 mM of OA and 0.25 g·L −1 FeS 2 /biochar were used together. In contrast, the removal rate of Cr(VI) by the individual FeS 2 /biochar and OA was 57.9% and 6.3%, respectively. The experimental and characterization results suggested that OA was adsorbed on the surface of FeS 2 /biochar through the conjugated structure of pine biochar, thereby enhancing the dissolution rate of Fe(II) and S(-II) in the FeS 2 /biochar composite, and facilitating the conversion of Fe(II), S(-II), and Cr(VI) to Fe(III), SO 4 2- , and Cr(III), respectively. In addition, the complexation of OA with Fe(III) and Cr(III) reduced the formation of Fe(OH) 3 and Cr(OH) 3 , exposing more surface active site of FeS 2 /biochar for the reduction of Cr(VI). As an electron donor , the addition of OA enhanced the electron transfer process of FeS 2 /biochar to Cr(VI) on the one hand, and on the other hand promoted the redox cycle of Fe(II) through the electron transfer between OA and Fe ions . FeS 2 /biochar showed better stability even after 5 cycles (in 5 mM OA system). The present study demonstrated the promise of low molecular weight organic acids in strengthening materials for environmental remediation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Mao Gao,Fan Tang,Yongchao Zhao,Yixuan Chu,Yan Yang,Guangming Tian,Yanlong Wang,Huaqing Liu
The characteristics of soil pore structure response to electric field strength and their effects on the migration of hexavalent chromium during electrokinetic remediation remain unclear. This paper investigates the effects of soil actual voltage and pore redistribution on hexavalent chromium removal under various voltage gradients during electrokinetic remediation. The electric field across the soil was the dominant factor that affected the soil properties, pore structure, and transportation of hexavalent chromium. The removal efficiency of dissolved hexavalent chromium was significantly enhanced from 36.1 % to 80.5 % as the theoretical voltage gradients increased from 0.5 V·cm −1 to 3 V·cm −1 due to the highest voltage proportion (52.7 %) of the soil chamber at 3 V·cm −1 , while it only increased to 82.0 % at 4 V·cm −1 . The optimal actual electric field strength of 1.00–1.50 V·cm −1 across the soil matrix facilitated the efficient electromigration of hexavalent chromium. The electric field force exerted a direct (0.70) or indirect action intensity (1.55) on soil pore structure by altering soil chemical properties. Soil mesopores and ultra-micropores transformed into micropores through collapsing, shrinking, ion migration, weakening electrostatic repulsion, and enhancing adhesive bonding among particles with increasing electric field. The distribution and structure of soil pores were more homogenous under optimal electric field conditions, thereby improving the migration path of hexavalent chromium. Soil mesopores facilitated hexavalent chromium removal and the formed micropores were opposite. These findings have significant scientific and practical implications for applying the in-situ electrokinetic techniques in the remediation of metal-contaminated soils.
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