JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Gao Feiyue,Zhou Chuncai,Cao Yachuan,Yu Yue,Li Yunfei,Liu Guijian
As a highly toxic rare metal, the removal of thallium (Tl) from wastewater has been widely investigated, and adsorption is considered one of the most promising treatment technologies for Tl-containing contaminated water because of its cost-effectiveness, convenience, and high efficacy. In this work, coal tar residue (CTR)-based porous carbon was synthesized through K 2 FeO 4 activation, and applied in adsorbing Tl(I). K 2 FeO 4 could synergistically produce porosity and load iron oxide on the produced porous carbon surface because of the catalytic cracking and oxidative etching during the activation of CTR. The adsorbent was synthesized at 800 ℃ with a mass ratio of K 2 FeO 4 /CTR being 3 (PC 3–800 ) showed optimal Tl(I) adsorption performance. The removal efficiency and distribution coefficient of PC 3–800 were above 95 % and 10 4 mL/g, respectively, in a wide pH range (4−10). Furthermore, the selection and reusability of PC 3–800 were favorable. The adsorption was a spontaneous, exothermic, and entropy increase process. The adsorption process was dominated by electrostatic attraction, surface complexation, and surface oxidation . The results suggested that removing Tl(I) from contaminated water via CTR-based porous carbon was feasible.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
PeerJ
·
2019
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IF 2.353
Weilong Zhang,Yang Wu,Jin Wang,Juan Liu,Haifeng Lu,Shuijing Zhai,Qiaohui Zhong,Siyu Liu,Wanying Zhong,Chunling Huang,Xiaoxiang Yu,Wenhui Zhang,Yongheng Chen
Rutile nano-titanium dioxide (RNTD) characterized by loose particles with diameter in 20–50 nm has a very large surface area for adsorption of Tl, a typical trace metal that has severe toxicity. The increasing application of RNTD and widespread discharge of Tl-bearing effluents from various industrial activities would increase the risk of their co-exposure in aquatic environments. The adsorption behavior of Tl(I) (a prevalent form of Tl in nature) on RNTD was studied as a function of solution pH, temperature, and ion strength. Adsorption isotherms, kinetics, and thermodynamics for Tl(I) were also investigated. The adsorption of Tl(I) on RNTD started at very low pH values and increased abruptly, then maintained at high level with increasing pH >9. Uptake of Tl(I) was very fast on RNTD in the first 15 min then slowed down. The adsorption of Tl(I) on RNTD was an exothermic process; and the adsorption isotherm of Tl(I) followed the Langmuir model, with the maximum adsorption amount of 51.2 mg/g at room temperature. The kinetics of Tl adsorption can be described by a pseudo-second-order equation. FT-IR spectroscopy revealed that -OH and -TiOO-H play an important role in the adsorption. All these results indicate that RNTD has a fast adsorption rate and excellent adsorption amount for Tl(I), which can thus alter the transport, bioavailability and fate of Tl(I) in aqueous environment.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
Environmental Science-Nano
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2022
·Vol. 9
·期 9
·3385-3396
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IF 9.473
Yu Luo,Zonglin Weng,Yuanfang Lin,Bin Han,Xinwen Ou,Yang Zhou,Jin Jiang
Thallium (Tl) is an extremely toxic trace element with high bioaccumulation. Selective and ultrafast Tl+ removal from water is critical to the safety of water resources but remains a grand challenge. Here, by intercalating KOH into multilayered Ti3C2Tx MXene, an efficient adsorbent with coordination/cation exchangeable sites (KOH@Ti3C2Tx) has been developed for Tl+ removal. Almost 99.6% of Tl+ could be removed over optimal KOH@Ti3C2Tx in just 10 s, and the maximal uptake capacity was up to 238.1 mg g−1, which is 3.8-fold larger than that of the pristine Ti3C2Tx (61.4 mg g−1). Moreover, benefitting from a wider working pH window and excellent selectivity, KOH@Ti3C2Tx could quickly remove almost all Tl+ from actual wastewater, demonstrating great potential for water purification. Control experiments and calculations jointly demonstrated that the boosted performance can be attributed to the synergistic effect of the abundant hydroxyl groups and exchangeable K+ sites, in which the hydroxyl groups can capture Tl+via coordination while the K+/Tl+ cation exchange contributes to selectivity and fast uptake kinetics. This work highlights the interaction mechanism of active sites and metal ions, providing fundamental guidance to the selective and rapid removal of heavy metals from water, especially in emergency disposal of heavy metal pollution accidents.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Jiangyan Lu,Zhu Xiong,Mahmud Sakil,Yuhang Cheng,Kaige Dong,Dongdong Qin,Wei Zhang,Li Yu,Gaosheng Zhang,Shuaifei Zhao
Developing highly efficient adsorbents for the removal of trace thallium(I) (Tl + ) is crucial for addressing environmental challenges. In this study, we successfully synthesized cubic Prussian blue (PB) loading on filter papers using an intermediate layer (dopamine/polyethyleneimine) via in-situ methods. The as-prepared PB-modified FP demonstrated outstanding anti-interference properties and light-enhanced adsorption performance for Tl + (0.5 mg/L) under ultraviolet (UV) irradiation, exhibiting twice the effectiveness compared to dark conditions, even in acidic and coexisting ionic environments. This indicated its suitability for treating complex Tl + -contaminated water. Notably, the removal efficiency for trace Tl + was almost 100%, with a maximum experimental adsorption capacity of 86.2 mg/g after 1-h photo-promoted adsorption under 365 nm UV. Characterization results supported a proposed photo-driven redox mechanism that elucidated the interaction between Tl + and PB-modified FP. Specifically, the accelerated Fe(III) to Fe(II) redox reaction facilitated Tl + accommodation on the surface and/or lattice of PB, enhancing Tl + adsorption by compensating for missed positive charges. This study provides valuable insights into utilizing PB-based materials to enhance the photo-enhanced Tl + adsorption capacity in a cost-effective, easy-to-synthesize, and environmentally friendly manner.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Chengxue Ma,Haijun Cheng,Ruixing Huang,Yijie Zou,Qiang He,Xiaoliu Huangfu,Jun Ma
The oxidation of thallium [Tl(I)] to Tl(III) by chlorine (HOCl) is an important process changing its removal performance in water treatment. However, the role of bromide (Br–), a common constituent in natural water, in the oxidation behavior of Tl(I) during chlorination remains unknown. Our results demonstrated that Br– was cycled and acted as a catalyst to enhance the kinetics of Tl(I) oxidation by HOCl over the pH range of 5.0–9.5. Different Tl(I) species (i.e., Tl+ and TlOH(aq)) and reactive bromine species (i.e., HOBr/BrO–, BrCl, Br2O, and BrOCl) were kinetically relevant to the enhanced oxidation of Tl(I). The oxidation by free bromine species became the dominant pathway even at a low Br– level of 50 μg/L for a chlorine dose of 2 mg of Cl2/L. It was found that the reactions of Tl+/BrCl, Tl+/BrOCl, and TlOH(aq)/HOBr dominated the kinetics of Tl(I) oxidation at pH < 6.0, pH 6.0–8.0, and pH > 8.0, respectively. The species-specific rate constants for Tl+ reacting with individual bromine species were determined and decreased in the order: BrCl > Br2 > BrOCl > Br2O > HOBr. Overall, the presented results refine our knowledge regarding the species-specific reactivity of TI(I) with bromine species and will be useful for further prediction of thallium mobility in chlorinated waters containing bromide.
研究领域:
环境科学
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水处理化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Muhammad Haris,Muhammad Usman,Fang Su,Wang Lei,Atif Saleem,Yasir Hamid,JunKang Guo,Yongtao Li
Tailoring the pathways to synthesize efficient biochars for pollutant adsorption has received extensive attention. Here, we synthesized highly efficient exfoliated biochar having thin layered nanosheets in its structure from agricultural wastes (wheat straw) by an innovative method involving biomass pre-treatment, nitrogen pyrolysis, and a flash heat exfoliation for thallium(I) removal from contaminated waters. Exfoliated biochar with nanosheets in its structure (EBNs) exhibited an open porous structure with a BET surface area 421.24 m 2 g −1 and pore size 3.98 nm, much higher than the 3.81 m 2 g −1 and 2.05 nm, respectively, of pristine wheat-straw biochar (PB). Using these materials for the adsorption of T1(I) revealed that the EBNs had a maximum adsorption capacity of 382.38 mg g −1 at pH 7.0, over 9 times higher than the PB. The adsorption kinetics and isotherm data were better fitted by pseudo-second order and Langmuir models. Moreover, EBNs retained its selective adsorption capacity for T1(I) in the presence of competing ions (Ca 2+ , Mg 2+ , K + , Cu 2+ , Zn 2+ ) and organic materials (humic acid, fulvic acid). Also, high regeneration ability (>93%) of EBNs was noted for five consecutive adsorption–desorption cycles. The efficiency of EBNs was also tested in river water (sampled from Bahe river, Xi’an, West China) spiked with T1(I) where it removed ∼ 90% of T1(I). These findings highlight the potential of EBNs for practical water treatment applications by developing the biochar nanosheets from agricultural wastes and provide insights into a new strategy to develop cost-effective carbon-based nanomaterials for wastewater treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Fa Fang,Nuo Li,Xian Zhang,Juan Liu,Jingzi Beiyuan,Jielong Cao,Jin Wang,Yanyi Liu,Gang Song,Tangfu Xiao
Due to extreme toxicity of the element of thallium (Tl), increasing aqueous Tl pollution incidents have aroused growing concerns. As the prevalent and stable form, i.e. , monovalent Tl, the highly efficient removal methodologies of Tl(I) from (waste)water remains limited and challenging. In this study, an advanced oxidation method, the feasibility of using zero valent iron (Fe 0 ) coupled with persulfate (PS) to treat Tl(I)-containing synthetic wastewater was investigated. Its influence parameters, including reaction time, initial Tl concentration, dosages of PS and Fe 0 , initial and coagulation pH, temperature, coexisting ions and organic matter (NO 3 − , SO 4 2− , Cl − and HA) were examined. The results revealed that the system can be applied to a wide range of pH and temperature and the reaction equilibrium can be reached in about 30 min. Favorable Tl(I) removal rate (>98%) was observed in the synthetic wastewater with medium and relatively high Tl(I) concentration (≤0.250 mM). The analyses of characterization results including electron spin resonance spectrometer and X-ray photoelectron spectroscopy indicated that ·OH played a vital role in the removal of Tl(I), which was oxidized and removed by co-precipitation. Fe 0 can be served as a stable source of Fe 2+ to efficiently catalyze PS. The remaining Fe 0 can be easily separated because of its magnetism, assuring the promising reusability of the reactant. The study aims to provide references for treatment of real Tl polluted wastewater.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Hailong Zhang,Jianying Qi,Fang Liu,Zhangxin Wang,Xiaoming Ma,Di He
Thallium (Tl) often enters the environment via mineral exploitation and utilization. The main restriction of Tl removal is the interference of high concentrations of coexisting ions in wastewater, therefore, enhancing the selectivity for Tl is essential to its treatment. Magnetic Prussian blue particles (Fe 3 O 4 @PB), an ion-sieving material with an open structure, were synthesized through a “one-pot” method at room temperature for the highly selective removal of Tl + . The removal percentage of Tl + was over 92% even when the concentration of coexisting ions (e.g. Zn 2+ , Cd 2+ , Cu 2+ , and Pb 2+ ) were 10,000 times higher than the initial concentration of Tl + . The maximal experimental removal capacity was 528 mg Tl/g Fe 3 O 4 @PB, and the removal percentage remained steady at pH 3–10. The high selectivity of Fe 3 O 4 @PB for Tl + is attributed to the fact that hydrated Tl + has a smaller hydrated diameter and a lower hydration free energy than other coexisting ions, while the rapid adsorption kinetics of Tl + results from the negative surface charge and the network of nanocapillaries of the Fe 3 O 4 @PB. Overall, a new low-cost material that is easy to synthesize and has superior Tl + removal capacity with extremely high selectivity for Tl + was obtained for effective magnetic removal of thallium from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Gao Feiyue,Zhou Chuncai,Cao Yachuan,Yang Ke,Li Zhiguo,Li Xin,Liu Guijian
Thallium (Tl) is a typical hypertoxic heavy metal, its accumulation in the water environment can have serious impacts on ecosystems and human health. In this study, a composite material (PC@MnO 2 ) was designed for removing Tl(I) by grafting MnO 2 onto coal tar residue-based porous carbon (PC) via hydrothermal impregnation. δ-MnO 2 with nano flower-like structure was verified to be evenly distributed on PC surface through material characterizations. The adsorption performance was markedly elevated after loading MnO 2 on PC, and the optimal adsorbent (PC@MnO 2 -75) was prepared by hydrothermal process from KMnO 4 (75 mg) using PC (100 mg) as a reducing agent. The adsorption of Tl(I) onto PC@MnO 2 -75 has achieved equilibrium in 90 min, slightly affected by solution pH (4−12), and exhibited an outstanding adsorptive selectivity in the presence of high concentrations of K + , Na + , Ca 2+ , Mg 2+ , Cl - , CO 3 2- , humic acid, and fulvic acid. The pseudo second order kinetic and Freundlich isotherm models were preferably described as the adsorptive characteristics. And the Tl(I) removal was a spontaneous exothermic adsorptive process. Density functional theory (DFT) results manifested that Mn doping enhanced electron transfer rate during adsorption. The highly efficient removal of Tl(I) on PC@MnO 2 -75 was achieved via electrostatic interaction, complexation, and oxidation-adsorption. The porous carbon derived from coal tar residue was engineered into PC@MnO 2 composites for efficient Tl(I) removal, which was in line with the environmental protection concept of sustainable development and green production.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Yu Gong,Yujie Wang,Jing Yang,Yongxin Bing,Zifei Sun,Yongming Ju,Xiaochen Lin,Houhu Zhang,Zitao Lin,Weixin Li
Recently, thallium (Tl) contamination at trace levels has gained worldwide attention, particularly in the remote ore-smelting regions of China. To effectively eliminate the residual target Tl(I) ions, one of the best strategies is to develop novel adsorbents with high selectivity. In this study, we selected silicate mineral waste (SMW) and chitosan (CTS) to synthesize a low-cost composite adsorbent for the removal of trace Tl(I). The results show that a mass ratio for SMW to CTS was optimized as 3:1 (denoted as SMW@CTS), and the preferred SMW@CTS exhibited a 37% higher removal efficiency compared to pure CTS beads (19%), underscoring the critical role of SMW in enhancing trace-level adsorption of Tl(I). Under the optimal conditions of 25 °C, pH = 5, and 6 g/L dosage, SMW@CTS achieved a Tl(I) removal efficiency of approx. 89% for an initial concentration of 100 μg/L. Moreover, the thermodynamics for the adsorption of Tl(I) onto SMW@CTS were investigated, and the structural characteristics of SMW@CTS were also characterized in detail. Furthermore, the mechanism for the high selectivity of Tl(I) onto SMW@CTS has been explored in the presence of humic acid and a series of competing ions. These findings highlight the novel SMW@CTS as a promising candidate for eliminating trace-level Tl(I) contamination from co-existing substances.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zhu Xiong,Yuhang Cheng,Kaige Dong,Mahmud Sakil,Zhu Wang,Liguo Zhang,Tangfu Xiao,Gaosheng Zhang,Shuaifei Zhao
Super trace thallium(I) (Tl + ) is still highly toxic and its removal from surface water is challenging. Here, we developed a new adsorptive membrane by immobilizing bimetal (cobalt and iron) Prussian blue analogues (Co@Fe-PBAs) on a polytetrafluoroethylene microporous membrane (Co@Fe-PBAs-M). The prepared membrane displayed precise adsorption of trace Tl + (50 μg/L) from complex water. A variety of interfering factors, such as water pH, competitive adsorption of positive ions (Na + and K + ) and negative ions (CO 3 2– and PO 4 3- ), natural organic matters (e.g., fulvic acid and bovine serum albumin) were evaluated during Tl removal. The composite membrane showed high removal efficiency (over 80 %) during long-term dynamic membrane separation of surface water containing super trace Tl + (<2.0 μg/L), breaking through the adsorption limitation in ultralow concentration of Tl + . The unique bimetal electron transfer of Co@Fe-PBAs-M reinforced the adsorptive performance to Tl + through dual ion exchange and intercalation. In the treatment of real Pearl River water containing 0.5 μg/L of Tl + , our membrane effectively reduced the Tl + concentration to 0.04 μg/L during 6-h continuous separation, which was far below the required level for drinking water (i.e., 0.1 μg/L). This work offers a promising solution for safe drinking water by remedying ultralow Tl + contaminated surface water.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Chengxue Ma,Xiaoliu Huangfu,Yijie Zou,Ruixing Huang,Qiang He,Jun Ma
The oxidation of thallium(I) (Tl (I)) to Tl (III) is referred to as an efficient means for Tl removal. Bromide (Br‾) inevitably occurs in nearly all water sources at concentrations of 0.01–67 mg/L (0.14–960 μM). The effect of Br‾ remains largely unclear but likely of critical importance on the redox fate and thus the removal potential of Tl (I) during typical oxidation treatment processes. Here, we investigate the kinetics and tackle the mechanism of Tl (I) oxidation by permanganate (KMnO 4 ) under the influence of Br‾. The results demonstrated that Br‾ at environmental levels exhibited significant catalytic effect on Tl (I) oxidation kinetics by KMnO 4 at acidic pH of 4.0–7.0, while no significant effect of Br‾ was observed for Tl(I) oxidation under alkaline conditions of pH 8.0 and 9.0. It was found that the enhanced oxidation kinetics under acidic conditions was driven by the combined effect of and autocatalysis mediated by MnO 2 and a fast oxidation kinetics served by in-situ formed bromine species. Through quantifying the relative contributions of those bromine species to the homogenous oxidation of Tl(I), HOBr, Br 2 and Br 2 O were found to play roles in catalyzing the oxidation of Tl(I) by KMnO 4 . The results discussed herein highlight the critical role of Br‾ on the Tl(I) complex oxidation process by KMnO 4 and may have implications for evaluating the redox cycle and removal potential of Tl in bromide-containing water treatment .
研究领域:
环境科学
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化学动力学
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）