PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2019
·
IF 4.384
Huawei Wang,Zijuan Lv,Yi Song,Ya-nan Wang,Daoyong Zhang,Yingjie Sun,Yiu Fai Tsang,Xiangliang Pan
Antimony(Sb(III)) contamination in wastewater has raised global concerns due to its high toxicity. The efficiency and mechanisms of Sb(III) adsorptive removal from wastewater with environmentally-friendly biogenic Mn oxide (BMO) materials as adsorbent were investigated, based on kinetic experiments and multispectroscopic analyses. Kinetic experiments showed that after 300 min of reaction, 97.79–100% of Sb(III) and 85.60–92.92% of total Sb were removed, indicating that BMO can quickly and effectively oxidize Sb(III) and sequester Sb(V) from water. The bacterial activity in BMO did not significantly affect Sb(III) removal, but a decrease in the release of Mn(II) into solution may provide new reactive sites for the re-oxidation of Sb(III). X-ray photoelectron spectrometer (XPS) high-resolution analysis suggested that Sb(V) was the only speciation remaining in the solid phase after the reaction of Sb(III) with BMO. X-ray diffraction (XRD) results further showed that the fast oxidation of Sb(III) by BMO led to the production of Mn(II) antimonate (Mn 2 Sb 2 O 7 ) precipitates. Successive extraction experiments confirmed that residual fraction (67.49–83.62%) and Mn oxide bound fraction (13.18–29.72%) were the dominant fractions of Sb(III) after 300 min of reaction, which were relatively stable and had low leaching risks. These findings indicated that BMO performed well in removing Sb(III) from wastewater.
研究领域:
环境科学
·
微生物学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Shaopeng Zhang,Jie Ding,Dayong Tian,Jing Wang,Jiale Zhang,Minghua Lu
China faces severe antimony pollution due to long-term, high-intensity mining and smelting operations. Long-term exposure to Sb(III) can lead to chronic respiratory problems. Adsorption method is used to remove Sb(III) because of its simplicity, economy and high efficiency. Therefore, a novel MIL-101(Fe)-Cl/SA hydrogel with oxidation-sorption bifunctionality was developed. 1602 cm −1 and 1025 cm −1 correspond to N H and S = O indicate N-chlorosulfonamide is bonded to MIL-101(Fe)-Cl/SA. MIL-101(Fe)-Cl/SA exhibited rough and wrinkled surfaces with numerous irregular particles by SEM. The presence of O (22 %) and Cl (2 %) confirmed the incorporation of N-chlorosulfonamide and SA into MIL-101(Fe)-Cl/SA by EDS and mappings. The adsorption capacities of MIL-101(Fe)-Cl/SA were 86 mg/g at 298 K and 123.21 mg/g at 328 K by Langmuir model. Kinetic and equilibrium correspond to pseudo-second-order and Langmuir model, respectively. Adsorption was spontaneous and endothermic by thermodynamic analysis. MIL-101(Fe)-Cl/SA exhibited enhanced selectivity in solution containing various ions. Moreover, MIL-101(Fe)-Cl/SA demonstrated potential for regeneration and reuse. The removal process primarily involved oxidation, electrostatic interaction, and complexation. In summary, the capability of MIL-101(Fe)-Cl/SA to adsorb and oxidize Sb(III) underscores its promising potential in mitigating the hazards associated with Sb(III).
研究领域:
环境科学
·
材料科学
·
废水处理
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产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2020
·
IF 4.605
Yaowu Cao,Qinghai Guo,Mengsi Liang,Weihao Sun
Antimony enrichment in aquatic environments is of great concern to international community. High-temperature geothermal waters usually contain excessive Sb, which are apt to contaminate the groundwaters or surface waters used as drinking waters in and around a hydrothermal area. However, Sb removal from geothermal water is rarely documented and the effect of high temperature on Sb removal has not received much attention. In this study, batch sorption experiments were conducted to investigate Sb removal from water by a hydroxyl-intercalated, mechanochemically synthesized Mg-Fe-LDH (i.e. Mg-Fe-OH-LDH) capable of avoiding secondary pollutions commonly related to other Mg-Fe-LDH intercalated by undesirable anions, such as Cl − and NO 3 − . The sorption capacities of Mg-Fe-OH-LDH for Sb(III) and Sb(V) were up to 48.7 and 30.0 mg/g, respectively. Notably, Mg-Fe-OH-LDH performed even better in removing aqueous Sb(V) at higher temperatures, superior to sorption of Sb by iron oxides that is generally exothermic and tends to be inhibited by increasing reaction temperature. The removal of Sb(V) existing as Sb(OH) 6 − by Mg-Fe-OH-LDH was attributable to its exchange with interlayer hydroxyl, and therefore could be impaired to some degree by coexisting anions with stronger electronegativity or smaller ionic radii . In contrast, anion exchange didn't contribute so much to Sb(III) sorption, because the main Sb(III) species at pH < 10 is neutral Sb(OH) 3 . XPS analyses confirmed that inner-sphere complexation between sorbed Sb(III) and Fe on Mg-Fe-OH-LDH layers was formed, which was hardly affected by competitive anions. Mg-Fe-OH-LDH is promising to be practically applied in removing both Sb(III) and Sb(V) from contaminated natural waters, wastewaters, or geothermal waters potentially acting as a pollution source .
研究领域:
环境科学
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水处理
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地球化学
·
材料科学
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产品关联
DOI
高影响因子
ACS Nano
·
2021
·
IF 15.881
Jingjie Wu,Xianli Li,Xin Lian,Binbin Su,Junhong Pang,Ming-De Li,Zhiguo Xia,Jin Z. Zhang,Binbin Luo,Xiao-Chun Huang
Antimony-based metal halide hybrids have attracted enormous attention due to the stereoactive 5s2 electron pair that drives intense triplet broadband emission. However, energy/charge transfer has been rarely achieved for Sb3+-doped materials. Herein, Sb3+ ions are homogeneously doped into 2D [NH3(CH2)4NH3]CdBr4 perovskite (Cd-PVK) using a wet-chemical method. Compared to the weak singlet exciton emission of Cd-PVK at 380 nm, 0.01% Sb3+-doped Cd-PVK exhibits intense triplet emission located at 640 nm with a near-unity quantum yield. Further increasing the doping concentration of Sb3+ completely quenches singlet exciton emission of Cd-PVK, concurrently with enhanced Sb3+ triplet emission. Delayed luminescence and femtosecond-transient absorption studies suggest that Sb3+ emission originates from exciton transfer (ET) from Cd-PVK host to Sb3+ dopant, while such ET cannot occur with Pb2+-doped Cd-PVK because of the mismatch of energy levels. In addition, density function theory calculations indicate that the introduced Sb3+ likely replace the Cd2+ ions along with the deprotonation of butanediammonium for charge balance, instead of generating Cd2+ vacancies. This work provides a deeper understanding of the ET of Sb3+-doped Cd-PVK and suggests an effective strategy to achieve efficient triplet Sb3+ emission beyond 0D Cl-based hybrids.
研究领域:
材料科学
·
光电学
·
化学
·
物理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2024
·
IF 5.8
Qi Cheng,Qingrui Li,Xiaoqin Li,Weizhen Liu,Zhang Lin,Liyuan Chai
Nanoscale zero-valent iron (nZVI) and modified nZVI have shown great removal capacities towards various heavy metals. However, the aging process of nZVI during the reaction is crucial for the long-term affinity and stability of heavy metals in the environment. In this study, the aging and iron oxide evolution of amorphous nZVI (A-nZVI) and nZVI during the reaction with Sb(III) were investigated and compared. The results indicated that after reacting with Sb(III), iron oxides in A-nZVI were mainly composed of γ-Fe2O3 (33.9%) and γ-FeOOH (29.8%), whereas α-Fe2O3 (24.9%) and α-FeOOH (31.8%) were dominant in the aged nZVI. The removal capacities for Sb(III) of γ-Fe2O3 (69.8 mg g−1) and γ-FeOOH (42.3 mg g−1) were both much higher than those of α-Fe2O3 (4.3 mg g−1) and α-FeOOH (8.4 mg g−1). Sb(III) was partially oxidized during the reaction, and DFT calculation showed that the adsorption energies of both Sb(III) and Sb(V) on γ-Fe2O3 and γ-FeOOH were higher than those on α-Fe2O3 and α-FeOOH. Furthermore, EXAFS analysis revealed that Sb formed an inner-sphere complex with the iron oxides in A-nZVI through the bidentate mononuclear edge-sharing structure (2E). Therefore, A-nZVI showed higher affinity and long-term stability toward Sb(III) remediation.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yuting Zhang,Jiaqi Wang,Xuesong Zhang,Wenxiu Qin,Youbin Si
Preliminary studies have demonstrated that light can facilitate the biogeochemical cycling of iron, influencing the valence state of heavy metals, solidifying them, and ultimately achieving detoxification effects. However, few studies have focused on the oxidation of Sb(III) in different iron minerals and the differences in mechanisms. This study explored the photooxidation of Sb(III) in the presence of various iron minerals (hematite, pyrite and goethite), focusing on how different iron minerals influenced the oxidation process and the mechanisms involved. Among the minerals tested, pyrite exhibited exceptional photooxidation performance, achieving an Sb(III) oxidation efficiency of 67.03% after 300 minutes. This superior photooxidation activity correlated with pyrite’s significant Fe(II) yield (11.70 μg/L). Our study demonstrated that light irradiation enhanced Sb(III) oxidation through three iron-based minerals. Light exposure drove the generation of Fe(II) within these minerals, initiating Fe(II)/Fe(III) redox cycling. This process promoted reactive oxygen species (ROS) generation, including hydroxyl radicals (•OH), superoxide radicals (O 2 •− ) and hydrogen peroxide (H 2 O 2 ), which collectively mediated Sb(III) oxidation to the less toxic Sb(V). In the photooxidation of Sb(III), •OH played a critical role in reactions involving hematite and pyrite, while O 2 •− dominated in goethite and pyrite systems. H 2 O 2 was found to have a pivotal role across all three iron mineral systems. Additionally, photogenerated holes ( h + ) significantly enhanced Sb(III) oxidation in the pyrite system. This research highlighted the impact of light on the biogeochemical cycling of iron and its role in facilitating the oxidation of Sb(III) through reactions that involve photo-generated electrons and free radicals.
研究领域:
环境科学
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地球化学
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光催化
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生物地球化学
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环境化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Nana Xiong,Peng Wan,Guocheng Zhu,Fubing Xie,Shengnan Xu,Chuanqu Zhu,Andrew S. Hursthouse
A series of environmental and health problems caused by the release of large quantities of antimony into the water environment have received wide social concern in a number of regions worldwide. Finding a feasible treatment technology is the best choice for the sustainable remediation of antimony pollution. A novel nano-modified chitosan (NMCS) was prepared by grafting iron oxide nanoparticles (Nano-Fe 3 O 4 ) and carboxylate metal organic frameworks (MOFs) denoted as MIL-100(Fe) onto chitosan. The NMCS before and after adsorption was characterized by analytical tools including Fourier transform infrared and X-ray photoelectron spectroscopy. Batch experiments with variable NMCS dose, solution pH, and competing anions were used to evaluate the most efficient way to remove Sb (III) from aqueous solutions. The results showed that removal efficiency increased with the increase of the NMCS concentration and solution pH, respectively. The maximum removal efficiency of Sb(III) was 96.8%, at pH 11 with 1.5 g/L of NMCS when treating a Sb(III) model solution of 10 mg/L, which is much higher than that with Nano-Fe 3 O 4 or MOFs. Compared with the efficient removal of Sb(III) under acid conditions, NMCS has a higher removal efficiency under alkaline conditions. The effect of common anions such as sulfate, carbonate, nitrate and chloride ions, on the removal of Sb(III), was minor. The removal of Sb(III) could be clearly described by pseudo-second order sorption kinetics and Freundlich isotherm, which suggested inner-sphere surface binding mechanisms. The presence of Sb (III) on NMCS was confirmed by an X-ray photoelectron spectroscopic analysis, and those functional groups binding to Sb (III) were identified using Fourier transform infrared analysis. The ability of NMCS to be regenerated was good and further enhanced by the possibility of magnetic recovery. Overall, the findings tested in this study showed that the NMCS developed can effectively remove Sb(III) from aqueous solutions and can be effectively recovered and reused.
研究领域:
环境科学
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水处理
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材料科学
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纳米技术
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Heng Li,Kaisheng Gong,Xiaoying Jin,Gary Owens,Zuliang Chen
Since antimony (Sb) is a toxic metalloid cost-effective method for the simultaneous removal of the two major Sb species from mining wastewater has attracted much attention. In this study, phytosynthesized iron nanoparticles ( n Fe) prepared using a eucalyptus leaf extract were successfully used to simultaneously remove Sb(III) and Sb(V) via an adsorption and oxidation mechanism with removal efficiencies of 100 and 97.7% for Sb(III) and Sb(V), respectively. Advanced analysis using X-ray photoelectron spectroscopy (XPS), ion chromatography-atomic fluorescence spectroscopy (IC-AFS), and electrochemical analysis confirmed that Sb(III) was oxidized to Sb(V) by Fe(III) on the n Fe surface while Scanning Electron Microscopy (SEM) and Energy Dispersive Spectroscopy (EDS) indicated that both Sb(III) and Sb(V) were adsorbed onto n Fe. Adsorption of both Sb(III) and Sb(V) best fit the Langmuir adsorption model with R 2 of 0.999 and 0.989, respectively and both followed pseudo-second-order kinetics with R 2 of 0.999 and 0.981, respectively. Furthermore, the adsorption rate of Sb(III) was faster than that of Sb(V) due to inner-sphere complex formation, and the Fe–O bonds in the asymmetric tetrahedron structure of Sb(III) were easier to break due to a lower energy barrier (0.863 eV). Consequently, a simultaneous removal mechanism of Sb(III) and Sb(V) was proposed. Finally, n Fe was used practically to remove Sb in mining wastewater with a removal efficiency of 93.5%, demonstrating that n Fe have significant potential to remove Sb in contaminated mining wastewaters.
研究领域:
环境科学
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纳米技术
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水处理
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Chunkai Huang,Zhiquan Xiang,Jincan Huang,Guangbing Liu,Xuemin Yu,Weijing Liu,Haijin Cao
Significant amounts of Sb(III) and Sb(V) are present in printing and dyeing wastewater (PDW), which leads to the detrimental effects on the environment if not treated properly. In this paper, the adsorptive removal of Sb(III) and Sb(V) by TiCl 4 derived flocs and the oxidation process were investigated. The results showed that TiCl 4 conducted superior coagulation performance on Sb(III) removal than Sb(V) in terms of dosage, pH range and immunity to interference. When the dosage was 50 mg/L and the final pH was 5.0, the concentration of Sb(III) and Sb(V) was reduced from 2000 μg/L to 100 μg/L and 180 μg/L, respectively. According to the Langmuir model, The adsorption for Sb(III) (74.27 mg/g) by TiCl 4 derived flocs was higher than Sb(V) (68.45 mg/g). The Sb(III) in the solution could partially inhibit the adsorption of Sb(V). It was also observed that the Sb(III) was oxidized to Sb(V), which was owing to the molecular oxygen during the coagulation and the flocs might act as catalyst. The actual printing and dyeing wastewater treatment experiments results showed that pre-reduction of Sb(V) to Sb(Ⅲ) could considerably improve the total Sb removal from 83 % to 98.8 %. The characterization results, such as zeta potential and x-ray photoelectron spectroscopy (XPS), indicated that the Sb(Ⅲ) removal was mainly achieved by chemisorption. The Sb(V) removal was mainly dependent on chemisorption and electrostatic adsorption, while the latter contributed more than former. The results of DFT calculations explained the reason for higher removal efficiencies of Sb(III) than Sb(V) in the TiCl 4 coagulation system. This study provides a new idea for the efficient removal of Sb(III) and Sb(V) using TiCl 4 in PDW to save the cost in engineering practice.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2018
·Vol. 92
·期 3
·575-581
·
IF 0.549
Zhang Dan,Zhao Yue,Xu Hong-Bo
Sb(III)-imprinted organic-inorganic hybrid sorbent was prepared by hydrothermal-assisted surface imprinting technique and was characterized by Fourier transform infrared spectroscopy, scanning electron microscopy coupled to an energy dispersive spectrometer and N 2 adsorption/desorption isotherms. Hydrothermal-assisted process can improve the selectivity of the Sb(III)-imprinted hybrid sorbent for Sb(III) due to stable control of temperature and pressure. The Sb(III)-imprinted hybrid sorbent IIS indicated higher selectivity for Sb(III), had high static adsorption capacity of 37.3 mg g –1 for Sb(III), displayed stable adsorption capacity in pH range from 4 to 8, reached an rapid adsorption equilibrium within 30 min. According to the correlation coefficient ( r 2 > 0.99), the experimental data fitted better the pseudo-second-order kinetic model and Langmuir equilibrium isotherm.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Min Li,Weiqi Wang,Mengxiaojun Wu,Jingwen Lei,Xiaolu Lu,Hongmei Wang
In this study Paraccocus versutus XT0.6 was employed to address the mechanism of microbial dissolution and oxidation of stibnite. Results showed that with the growth of XT0.6, pH increased to 9.0 in both microbe-mineral contact (MM) and microbe-mineral non-contact groups (M[M]). Dissolved Sb(III) was released from stibnite, which was subsequently quickly oxidized to Sb(V) completely in MM and partially in M[M] groups. On the contrast, the final pH decreased to 6.5 and 4.9, respectviely, in system amended with extracellular secretion (EM) of XT0.6 and abiotic groups. Dissolution of stibnite and oxidation of Sb(III) were also observed in EM group, suggesting a potential contribution of extracellular enzyme in Sb(III) oxidation. The dissolution and oxidation rates were the highest in MM group, followed by those in M[M], EM and abiotic groups. To be noted, Sb(V) concentration decreased in MM group on the fifth day, which might indicate the formation of Sb(V)-bearing secondary mineral. Genome of XT0.6 consisted of two chromosomes and one plasmid, and most genes responsible for antimony oxidation and antimony resistance were located on the chromosomes. Proteomics analysis of the extracellular secretions indicated the up-regulated proteins were mainly related to electron-transfer, suggesting their potential role in Sb(III) oxidation.
研究领域:
微生物学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Qiao Li,Xinyue Ma,Chengsi Qi,Rui Li,Wei Zhang,Jiansheng Li,Jinyou Shen,Xiuyun Sun
Effective removal of Sb(III) and Sb(V) has long been an urgent task for protecting human health and environment. In this study, novel magnetic mesoporous Fe Mn binary oxides (MMFMs) were fabricated via calcinating the Mn encapsulated carboxymethyl cellulose-Fe(III) hydrogel, and the structure of MMFMs were closely related to the Fe:Mn ratio. Owing to the mesoporous structure together with synergistic effect of Fe Mn binary component, the MMFMs exhibited excellent mass transfer and adsorption ability to Sb(III) and Sb(V). MMFM 3 achieved a maximum Sb(III) and Sb(V) adsorption capacity of 281.5 and 204.6 mg/g, respectively. Co-existing anions of Cl − , NO 3 − and SO 4 2− exhibited marginal influence on the adsorption for both Sb(III) and Sb(V), except the PO 4 3− for Sb(III) and SiO 3 2− or PO 4 3− for Sb(V). X-ray photoelectron spectroscopic investigation revealed that high valence Mn(IV) was mainly responsible for the oxidation transformation of the highly toxic Sb(III) into less toxic Sb(V), while the FeO x content played major role for the adsorption of Sb(V). The generated inner-sphere Fe O Sb complex between Fe-OH groups and Sb(III/V) dominantly contributed to the removal of Sb(III/V). Overall, mesoporous structure, magnetic separation ability, excellent adsorption performance together with exceptional regeneration properties demonstrated the great potential of MMFMs for Sb(III/V) remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）