Surfaces and Interfaces
·
2024
·
IF 5.7
Kuo Yang,Yun Yang,Yifan Jiang,Bingjie Ye,Luowei Li,Wenju Liu,Tong Yan,Wei Li,Shixi Liu
s In this study, a flower-shaped Bi 2 S 3 /g-C 3 N 4 heterostructure was synthesized via a hydrothermal method and utilized as a visible-light-driven photocatalyst for the removal of hexavalent chromium (Cr 6+ ) and Rhodamine B (RhB). Employing an interface electronic engineering strategy with heterostructure nanosheets, the thickness of the nanosheets was adjusted by varying the molecular weight of the structure guiding agent, polyethylene glycol (Mn = 400, 2000 or 4000). Under visible light irradiation for 18 and 60 minutes, the removal efficiencies of Cr 6+ and RhB reached 95.0 % and 99.9 %, respectively, with corresponding rate constants being 8.64-fold and 9.67-fold higher than pure Bi 2 S 3 . The enhanced photocatalytic efficiency may be attributed to the intermediate adsorption states and increased active sites enhancing light absorption and charge separation. Furthermore, species capture studies revealed that electrons (e - ) and superoxide radicals (·O 2 - ) played crucial roles in the reduction of chromium (VI), while holes (h + ) were the primary active species involved in RhB degradation. Density-functional theory (DFT) calculation demonstrated charge redistribution and electron accumulation can be more obviously observed at Bi 2 S 3 /g-C 3 N 4 than Bi 2 S 3 , which proved that g-C 3 N 4 doping effectively improved the electrons transfer efficiency over the Bi 2 S 3 /g-C 3 N 4 surface, thereby enhancing the photocatalytic activity.
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ACS ES&T Water
·
2024
·
IF 4.8
Zhi Ye,Yunpeng Liu,Jiang Xu,Nan Xu,Juncai Dong,Haijun Chen,Dongrui Li,Lei Peng,Yuxi Gao,Jiating Zhao
The efficiency and stability of in situ remediation of Cr(VI) contamination in underground water and soil are still challenging. In this study, a green tea (GT) synthesized nano-zerovalent iron (nZVI) nanocomposite supported by diatomite (DE) (nZVI@GT/DE) via tea polyphenols was designed. The synergetic effect of DE support and tea polyphenols wrapping increased the Fe(II) component in nZVI@GT/DE and its transportability. Compared to nZVI@GT/Mont (supported by Mont with sandwich structure), nZVI@GT/DE exhibited a notably higher capacity (>100 mg g–1) for immobilizing Cr(VI) and a more pronounced ability to release iron ions in solution (corrosion parameter: K ≈ 1.046). This was attributed to the combined effect of the unwrapping process of tea polyphenols coverage and the distinctive columnar porous structure of DE, which increased the exposure of α-Fe0 core for enhanced Cr(VI) reduction during their cotransport in the water-saturated soil system. X-ray absorption fine structure and X-ray photoelectron spectroscopy analyses confirmed that nZVI@GT/DE released more Fe(II) ions to reduce Cr(VI) to bidentate binuclear Cr(OH)3 (vs FeOCr2O3) complexes. This study unraveled the molecular mechanism and highlighted the Cr speciation transformation and physiochemical property changes of nZVI@GT/DE during their cotransporting when applied in situ remediation in complex subsurface of Cr(VI)-contaminated groundwater and soil system.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Guang Tian,Falin He,Xiangxiang Li,Shaoyang Hu,Xingchen Zhao,Shuqi Guo,Tingting Wang,Hao Wang,Wansong Zong,Rutao Liu
Chromium (Cr) poses a high ecological risk, however the toxic mechanisms of Cr in different valence states to soil organisms at cellular and molecular levels are not exactly. In this study, the Eisenia fetida coelomocytes and Cu/Zn-superoxide dismutase (Cu/Zn-SOD) were chosen as the target subjects to investigate the effects and mechanisms of cellular toxicity induced by Cr(VI) and Cr(III). Results indicated that Cr(VI) and Cr(III) significantly reduced the coelomocytes viability. The level of reactive oxygen species (ROS) was markedly increased after Cr(VI) exposure, which finally reduced antioxidant defense abilities, and induced lipid peroxidation and cellular membrane damage in earthworm coelomocytes. However, Cr(III) induced lower levels of oxidative stress and cellular damage with respect to Cr(VI). From a molecular perspective, the binding of both Cr(VI) and Cr(III) with Cu/Zn-SOD resulted in protein backbone loosening and reduced β-Sheet content. The Cu/Zn-SOD showed fluorescence enhancement with Cr(III), whereas Cr(VI) had no obvious effect. The activity of Cu/Zn-SOD continued to decrease with the exposure of Cr. Molecular docking indicated that Cr(III) interacted more readily with the active center of Cu/Zn-SOD. Our results illustrate that oxidative stress induced by Cr(VI) and Cr(III) plays an important role in the cytotoxic differences of Eisenia fetida coelomocytes and the binding of Cr with Cu/Zn-SOD can also affect the normal structures and functions of antioxidant defense-associated protein.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xiang-Zheng Cui,Yu Peng,Shuo Chen,Hong Jiang
Hexavalent chromium (Cr(VI)), a highly toxic and mobile contaminant commonly found in industrial wastewater, poses substantial environmental and health risks, and its reduction to the less harmful trivalent form (Cr(III)) is a critical remediation strategy. While copper nanoparticles (Cu NPs) offer a cost-effective alternative to expensive precious metal catalysts, their tendency to agglomerate limits their catalytic efficiency. To address this, we synthesized a Cu-MMT/CS (montmorillonite/chitosan) composite catalyst via a straightforward two-step pyrolysis method, leveraging the chelating ability of chitosan and the layered structure of montmorillonite to disperse Cu NPs. The optimized Cu-MMT/CS catalyst achieved exceptional performance, removing more than 98 % of Cr(VI) within 6 min via formic acid (FA) as a reductant, and maintained its high efficiency even in the presence of common environmental anions such as Cl - 、NO 3 - 、SO 4 2- 、CO 3 2- 、H 2 PO 4 - . The uniformly dispersed Cu nanoparticles serve as the active sites for the catalytic reaction, while the high degree of graphitization of the carrier (MMT/CS structure) and the low charge transfer resistance facilitate charge transfer between the catalyst and FA, promoting the decomposition of FA to produce active hydrogen, which in turn enhances the ability to reduce Cr(VI). This study offers a cost-effective, environmentally friendly solution for Cr(VI) reduction, advancing the design of sustainable nonprecious metal-based catalysts for wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2017
·
IF 6.065
Shunxing Li,Jiabai Cai,Xueqing Wu,Biwen Liu,Qiaoying Chen,Yuehai Li,Fengying Zheng
An solar-light-driven and bifunctional photocatalyst was designed for photo-reduction of Cr(VI) and selective photo-oxidation of benzyl alcohol into benzaldehyde in the presence of water under ambient conditions. Double-shelled and sandwiched TiO 2 @Pt@CeO 2 hollow spheres were prepared by using functionalized polystyrene spheres, sol-gel, hydrothermal reaction, and calcination. The Pt nanoparticles (NPs) were controllably loaded between the TiO 2 shell and CeO 2 shell. Under solar-light irradiation, the photo-reduction rate of Cr(VI) (μmol h −1 ) was in the order of TiO 2 @Pt@CeO 2 (1.901) > TiO 2 @CeO 2 (1.424) > TiO 2 (1.040) > CeO 2 (0.992). Among the above-mentioned photocatalysts, the conversion rate of benzyl alcohol for TiO 2 @Pt@CeO 2 was also the best. These results were attributed to the combination of TiO 2 and CeO 2 as photocatalyst and oxygen buffer, the double-shelled and sandwiched nanostructure, and the addition of Pt NPs as cocatalyst and electron trap site, which could store and shuttle photo-generated electrons, reduce the recombination of the electron-hole, and then enhance photo-generation of active radicals. This conclusion was verified by the electron paramagnetic resonance (EPR) spectroscopy. Considering the versatile combination of photocatalyst, oxygen buffer and cocatalyst, this work could provide new insights into the design of high-performance bifunctional photocatalysts for heavy metal removal and selective synthesis.
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CHEMOSPHERE
·
2024
·
IF 8.1
Xinying Zhang,Yuling Zhang,Dong Li,Jili Wang,Yang Ding,Yiliang Wang,Liuyuan Feng,Yuliang Hu
In this study, we examined the aging characteristics of polyethylene (PE) and polylactic acid (PLA) microplastics (MPs), examining the adsorption behaviors and mechanisms concerning Cd(II) and Cr(VI) under both single and binary systems. The results revealed that aging treatment changed the physicochemical properties of MPs. The aging mechanisms of PLA and PE MPs were shown to be similar by the 2D-FTIR-COS study. These mechanisms involve the formation of oxygen-containing functional groups through the combination of carbon chain breakdown and oxygen. Aged MPs had a greater ability to adsorb metal ions than pristine MPs, with PLA MPs outperforming PE MPs. After 30 days of aging, Cd(II) adsorption increased by 40.61 % and 25.49 % for PE and PLA MPs, respectively, while Cr(VI) adsorption increased by 37.50 % and 69.29 %, respectively. The adsorption ability of PE and PLA MPs with Cd(II) or Cr(VI) under binary systems was less than that under single systems, with Cd(II) exhibiting more adsorption competitiveness than Cr(VI). Humic acid (HA), ionic species and strength , solution pH, and adsorption of Cd(II) and Cr(VI) were found to be significantly correlated. Further investigation into the adsorption mechanisms of Cd(II) and Cr(VI) on PE and PLA MPs revealed that pore-filling, electrostatic interactions , complexation, and hydrogen bonding play important roles in the adsorption process . The study's conclusions are crucial for assessing the risk associated with concurrent contamination by metal ions and microplastics.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Haoruo Xu,Chenxi Huang,Weili Yu,Ningjie Fang,Yinghao Chu,Jinhui Li
The combined pollution toxicity of hexavalent chromium heavy metal (Cr(VI)) and antibiotics (such as ofloxacin, OFL) is much higher than that of a single pollutant, posing a serious challenge to the ecological environment. Photocatalytic technology can achieve the removal of both single pollutants and composite pollutants. It is urgent to develop catalysts with high carrier separation efficiency and photocatalytic degradation performance. In this work, we successfully prepared m-PDI/BiOI heterojunction catalysts (mPB-3) with tight contact interfaces using the continuous ion layer adsorption and reaction method, and applied them to the synergistic removal of OFL and Cr(VI). The results showed that mPB-3 exhibited a bidirectional enhancement effect. The degradation rate of OFL reached more than 99.5 % within 40 min, the corresponding reduction efficiency of Cr(Ⅵ) reached 63.7 % at pH = 9. Furthermore, the influence of different environmental factors on the degradation process have also been clarified, indicating that mPB-3 has good stability and adaptability. The system characterization results confirmed that a S-scheme heterojunction has been formed. This can accelerate the rapid migration of electrons from m-PDI to BiOI, achieving efficient charge separation, and ultimately enhancing the photocatalytic activity. Finally, the degradation intermediate products and degradation mechanism were analyzed. This study provides a feasible solution for the design of efficient photocatalytic materials and their application in the combined pollution treatment of OFL and Cr(VI). Environmental implication Cr(VI) and OFL coexisting in water bodies pose significant ecological risks due to their enhanced combined toxicity. Traditional treatment techniques often struggle to effectively address such complex pollution systems. This study demonstrates that the m-PDI/BiOI heterojunction photocatalyst can efficiently synergistically remove both contaminants under environmentally relevant conditions (e.g., pH = 9), providing a practical strategy to mitigate composite pollution challenges. The S-scheme charge separation mechanism offers insights for designing advanced catalysts to tackle emerging multi-pollutant threats in aquatic ecosystems, supporting sustainable water treatment solutions.
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WATER AIR AND SOIL POLLUTION
·
2025
·Vol. 236
·期 10
·1-20
·
IF 3
Hu Wei,Zhang Jun
This study investigated the adsorption characteristics of Cr(VI) and methyl orange (MO) onto polyethyleneimine (PEI) cryogels. The morphology and physicochemical properties of this prepared adsorbent were characterized with various techniques. Its adsorption behaviors towards MO and Cr(VI) were systematically investigated. In single-component systems, PEI cryogels exhibited significant adsorption capacities for Cr(VI) (875 mg/g) and MO (1777 mg/g), respectively. In binary systems, the cryogels demonstrated a stronger affinity for Cr(VI) than for MO. Column adsorption studies in single-component systems explored the effects of bed height, flow rate, and inlet concentration using breakthrough curves, with the modified dose–response model proving effective in describing these curves. Moreover, repeated dynamic adsorption experiments highlighted that the cryogels exhibited exceptional reusability. Results from column adsorption in binary systems indicated that the presence of MO did not significantly affect the adsorption of Cr(VI), while the presence of Cr(VI) enhanced the affinity of the cryogels for MO adsorption. The adsorption mechanism of PEI cryogels towards Cr(VI) primarily involved electrostatic attraction and reduction, whereas for MO, it predominantly entailed electrostatic attraction and hydrogen bonding. These findings collectively emphasize the significant potential of PEI cryogels for treating dyeing wastewater.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiao Dan Sun,Zhangxin Duan,Jingjing Song,Hanxing Yang,Kai Yan,Zhenhua Tian,Dangge Gao,Jianzhong Ma
Carcinogen Cr(VI) is reduced efficiently into Cr(III) by a photocatalyst, but the produced Cr(III) is difficult to transfer from the photocatalytic active site. The “two birds with one stone” strategy is proposed to realize the in situ growth of ZnIn2S4 nanoplates on SBA-15 and the creation of separated active sites, in which ZnO loading on the porous SBA-15 nanorod was used as a zinc source. Obtained samples ZnIn2S4/SBA-15 (ZIS/SBA) showed the redshift of the absorption band and better separation of photoinduced carriers than pristine ZnIn2S4, due to its smaller size and S defect. All of the Cr(VI) was reduced to Cr(III) by the ZIS/SBA sample during the photocatalytic process, which was 2 times higher than pristine ZnIn2S4. Moreover, 92.8% of Cr(III) was adsorbed simultaneously during photocatalysis due to the electrostatic interaction from SBA-15. In addition, the ZIS/SBA sample showed good recycling stability after 5 times cycles, providing a new strategy for the in situ growth of ZnIn2S4 on the surface of porous materials and a novel way for the simultaneous removal of Cr(VI) and Cr(III) during photocatalysis.
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Desalination and Water Treatment
·
2024
·
IF 1
Jianlei Gao,Zixu Zhao,Yixin Yan,Mengyuan Feng,Yu Wang,Jing Wang
ABSTRACT Hexavalent chromium [Cr(VI)] pollution has attracted intense interest in research on heavy metal pollution removal. Here, quartz sand chitosan zero-valent iron (QS-CTS@ZVI) was prepared as a permeable reactive barrier (PRB) medium material by using PRB permeable reaction wall technology and modified CTS-loaded ZVI-coated quartz sand. Characterization analyses were performed with scanning electron microscope, X-ray diffraction, Fourier-transform infrared spectroscopy and thermogravimetry-differential scanning calorimetry. The effects of the reaction time, reaction temperature, initial solution pH, initial Cr(VI) concentration, adsorbent dosage, interfering ions and adsorption cycle on the adsorption of Cr(VI) and total Cr on QS-CTS@ZVI were examined. Then, the adsorption of Cr(VI) by QS-CTS@ZVI was investigated. The results showed that for a ZVI:CTS ratio of 1:1 (m:m), a QS:ZVI ratio of 1:2 (m:m), a pH of 3, t = 5 h, an initial Cr(VI) concentration of 200 mg/L, a QS-CTS@ZVI dosage of 3.5 g/L, and T = 25°C, the efficiencies of Cr(VI) and total Cr removal by QS-CTS@ZVI were 91.6% and 90.9%, respectively. The adsorption efficiency of QS-CTS@ZVI for Cr(VI) was approximately 80% after three reuses. The coexistence of SO 4 2- in water can significantly inhibit the Cr(VI) adsorption and removal process. The process of adsorption of Cr(VI) by QS-CTS@ZVI conformed to the pseudo-second-order kinetic equation and the Langmuir adsorption isotherm model.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Xiaoshu Lv,Xiaofeng Qin,Kaifeng Wang,Yiyin Peng,Peng Wang,Guangming Jiang
The scaled application of nanoscale zero-valent iron nanoparticles (nZVI or Fe° NPs) in environmental remediation is challenged by easy surface passivation and particle aggregation. To improve this situation and enhance their performance in Cr(VI) removal from water phase, we present one novel strategy to hybridize nZVI with layered double hydroxide (LDH) decorated reduced graphene oxide (rGO). The as-prepared ternary (Fe@LDH/rGO) composites possess better dispersibility, improved hydrophilicity and more positive surfaces that allows higher removal efficiency and capacity for Cr(VI) oxyanions. Composition proportion are optimized and influences of surroundings (solution pH, Cr(VI) concentration and temperature) are evaluated. Also, we demonstrate that Fe@LDH/rGO can be reused with suitable post-treatments, which combines alkaline solution desorption and NaBH 4 revivification possess. Cr desorption and Fe leaching ratio during regeneration should be critical indicators that determine the recovery efficiency. Synergistic effect within this ternary system not only contributes to its superiorities in stability, but also continuous iron corrosion via the formation of micro Fe-C batteries, where rGO acts as cathode and alternative electron conductor. The present work suggests great potentials of Fe@LDH/rGO composites in groundwater remediation.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Chongfei Yu,Pengyan Yang,Luna Tie,Siyu Yang,Shuying Dong,Jingyu Sun,Jianhui Sun
Herein, we demonstrate the design and fabrication of β-Bi 2 O 3 @ Bi 2 S 3 hollow microspheres with sheet-like hierarchical nanostructures targeting an advanced visible-light-responsive photocatalytic system. In comparison with pure Bi 2 S 3 and β-Bi 2 O 3 , the as-obtained β-Bi 2 O 3 @Bi 2 S 3 heterojunction photocatalyst exhibits a markedly enhanced sunlight photocatalytic activity towards the photo-degradation of rhodamine B. Following, the property of the β-Bi 2 O 3 @Bi 2 S 3 on the Cr 6+ photocatalytic reduction was then evaluated. Operating conditions such as β-Bi 2 O 3 @Bi 2 S 3 mass, tartaric acid concentration, and initial Cr 6+ concentration were analyzed. The results showed that a suitable reduction condition was selected as, β-Bi 2 O 3 @Bi 2 S 3 dosage 25 mg, initial concentration 20 mg·L −1 and molar ratio of Cr 6+ /tartaric acid 1:20. The outstanding photocatalytic performances of the hybrid photocatalyst are mainly attributed to the reduced recombination rates of photo-generated electrons/holes, enhanced light harvesting, increased active sites as well as the improved photo/chemical stability. Moreover, the photocatalytic mechanism of β-Bi 2 O 3 @Bi 2 S 3 for oxidation of RhB and reduction of Cr 6+ was investigated in detail. The enhanced photocatalytic activity and excellent chemical stability render the thus-fabricated heterostructure a promising candidate to remediate aquatic contaminants and meet the demands of future photocatalytic materials.
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