SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Ziyi Deng,Xiaohan Li,Gaosheng Zhang,Guicong Xiao,Yuan Xie,Ru Nie,Shenglin Mai,Jianyou Long,Ziqing Xiao,Ping Zhang,Huosheng Li
Hypochlorite (ClO − )-based chlorination has shown effectiveness in oxidizing and purifying ammonium nitrogen (NH 4 + -N) and thallium (Tl) individually. However, the co-removal of these contaminants remains understudied. Addressing this gap, our study investigated the behaviors and mechanisms of NaClO-based breakpoint chlorination in oxidizing and removing both Tl and NH 4 + -N. The interaction among thallous ions (Tl + ), NH 4 + -N and NaClO in wastewater created a synergistic oxidation effect, which led to high removal efficiencies, exceeding 97 % for both Tl and NH 4 + -N, achieved with a NaClO concentration of 7 mmol/L, across a pH range of 6 to 10 in less than 5 min. Notably, the presence of Tl + , rather than Tl 3+ or Tl 2 O 3 , significantly enhanced the conversion of hypochlorite alongside NH 4 + -N. This coupled process generated chloramines and nitroxyl, along with oxygen-independent hydroxyl radicals formation, which further transformed into chloride radicals, dichlorine radical anions, and chlorine oxide radicals. Introducing these highly reactive species into the binary-pollutant system marked a substantial improvement over single-pollutant systems, yielding significantly higher removal efficiencies. These findings shed new light on the role of Tl in breakpoint chlorination for wastewater containing both Tl and NH 4 + -N.
研究领域:
环境科学
·
污水处理
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产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Qitong Xue,Jiaying Xing,Jianjun Chen,Jinxing Mi,Jianqiang Shi,Yao Wang,Junhua Li,Zhiming Liu
V 2 O 5 /TiO 2 has been wide used in the selective catalytic reduction of NO x by NH 3 (NH 3 -SCR). However, the poisoning mechanism of thallium (Tl) on the catalytic performance of commercial V 2 O 5 /TiO 2 catalyst has remained unclear. Herein, we have systematically investigated the poisoning effect of Tl based on the different characterizations and DFT calculations. It was found that the strong interaction between V and Tl exists, resulting in the transformation of V from monomeric VO x to polymeric and crystalline VO x , the formation of V-O-Tl species, a decrease in the active V 5+ sites, and the inhibition of the adsorption and activation of NH 3 on both Brønsted and Lewis acid sites. Mechanistic studies further confirmed that inactive nitrate intermediate species gradually accumulated over V 2 O 5 /TiO 2 catalyst surface due to the presence of Tl. A combination of factors ultimately led to the deactivation of the V 2 O 5 /TiO 2 catalyst. This study unveils the poisoning mechanism of Tl on V-based catalysts and shed light on the design of Tl-tolerant NH 3 -SCR catalysts.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Jianbo Jiang,Jichang Wen,Ruijia Yang,Haixia Yang,Shikai Yang
Long-term mining activities in the mercury-thallium mining area of Lanmuchang, southwestern China, resulting in contamination of surrounding soils with complex toxic elements such as Tl, As, Sb, Hg, and Cd. While manure aids in pollution control and soil fertilization, its impact on Tl bioavailability in soil remains incompletely understood. This study explored the physiological changes and Tl accumulation in Capsicum annuum under combined pollution stress and application of livestock and poultry manure near the Lanmuchang mining area. The results showed that chicken manure promoted Tl accumulation in Capsicum annuum , whereas pig and cattle manure inhibited it, with pig manure exhibiting the strongest inhibitory effect. Both pig and cattle manure reduced the transpiration rate of Capsicum annuum , which decreased the driving force for Tl transport to the plant's upper parts. Additionally, manure increased organic acid secretion in Capsicum annuum roots and decreased soil Eh. This led to a reduction in Tl 3+ to the more stable Tl + , which decreased the content of exchangeable Tl form and its activity. Pig manure significantly reduced Tl content in stems, leaves, and fruits by increasing the area of the Casparian bands in Capsicum annuum roots, which hindered Tl accumulation. In contrast, chicken manure had the opposite effect. The findings of this study provide important theoretical support for scientifically guiding agricultural production safety in areas contaminated with the heavy metal Tl.
研究领域:
环境科学
·
植物生理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Lixian Zhong,Peidi Luo,Yaoyao Wu,Kai Yang,Can Zhang,Ruihao Peng,Chuanhao Li,Xianping Luo
Thallium (Tl), an unconventional and highly toxic metal, is increasingly recognized as a significant contaminant in wastewater. One promising strategy to enhance Tl removal is the electrocatalytic oxidation of Tl(I), yet the contribution of chloride ions—prevalent in wastewater from metallurgical and smelting industries—has often been overlooked in such processes. Herein, this study introduces a novel chlorine-mediated electrochemical oxidation system, coupled with a coagulation process, designed to efficiently treat thallium-contaminated saline wastewater. The dimensionally stable anode (Ti/TiO 2 -RuO 2 -IrO 2 , DSA) demonstrates exceptional electrocatalytic chlorine evolution and efficient oxidation of Tl(I), with a kinetic rate constant of 0.131 min −1 , which is 21.8 times faster than that of a carbon cloth anode (0.006 min −1 ) in the presence of Cl − ions. Under optimized conditions of 5 mM Cl − ions at pH 3.0, over 98.3 % of Tl(I) was removed within 30 min. After coagulation treatment, the total Tl removal efficiency reached 98.5 %, in stark contrast to the mere 18.0 % achieved without the pre-electro-oxidation step. Mechanistic analysis revealed that the reactive chlorine species (Cl•) plays a more significant role in the oxidation of thallium (Tl) compared to the hydroxyl radicals. Notably, the system exhibits excellent recyclability (up to 35 cycles) and stable performance in the presence of various competing ions and actual wastewater, even under unsteady-state continuous-flow conditions. These findings offer valuable insights into chlorine-mediated electrocatalytic oxidation coupling with coagulation processes for thallium removal, providing guidance for practical applications in purifying thallium-contaminated industrial wastewater.
研究领域:
环境科学
·
化学工程
·
水处理技术
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产品关联
DOI
高影响因子
PeerJ
·
2019
·
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
·
化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Chao Wang,Min Chen,Huimin Hu,Junwei Huang,Ting Jiang,Lei Peng,Qing Shi,Qiwu Zhang
The deep treatment of monovalent thallium (Tl + ) and the study of Tl + incorporation mechanism are of great value for water safety. However, current research objectives have focused on how to oxidize or precipitate Tl + , while neglecting to investigate the underlying mechanisms of the direct immobilization and stable storage state of Tl + . Therefore, the present study examines in detail how Tl + is directly incorporated and stably stored by silicate minerals. In this study, an idea is proposed to enhance the purification of Tl-containing wastewater by using mechanically activated mica to stabilize Tl + in the silicate structure in the form of lattice residue state. Elucidation of the removal mechanism was first performed with focus on Tl + exchange with interlayer K + and H(H 2 O) + inside the silicate mineral based on the quantitative data and a series of characterizations such as XRD, XPS, FTIR, SEM-EDS and TG. As adsorbents for Tl-containing wastewater, both activated phlogopite and biotite for the purification of target wastewater demonstrated excellent performances at a dose of 2 g/L and a reaction time of 240 min, reaching quantitatively down to 23.88 μg/L and nearly 0 μg/L respectively, from an initial Tl + concentration of 1203 μg/L, so that the effluent concentrations would meet the requirements of US EPA and Chinese discharge standards for industrial wastewater and drinking water. In addition, density functional theory (DFT) calculation was used to quantify the adsorption energy of Tl + being solidified in the interlayer structure to further give insight into the mechanism of Tl + immobilization by silicate mineral.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Lijuan Huang,Longyan Xiang,Yan Zhang,Yongan Wang,Zhiyong Nie
The simultaneous detection of K + and Tl + can serve as a toxicological diagnostic tool for thallium poisoning. Colorimetric-reaction-based nanoprobes have emerged as promising sensors for the rapid and ultrasensitive detection of molecular species in simple systems. However, the development of viable screening tools for multicomponent analysis in complex systems remains challenging owing to interference from coexisting materials in the media. Herein, a simple chemical sensor array based on the peroxidase-like activity of gold nanoparticles modified with single-stranded DNA (AuNPs-ssDNA) and chemometrics was developed for the simultaneous detection of K + and Tl + in aqueous solutions and serum. The use of a K + adapter conferred high selectivity to the developed method. Optimized AuNPs-ssDNAs were used to construct a sensor array, which together with chemometrics provided fingerprints that can facilitate the simultaneous analysis of multiple components. The developed colorimetric reaction in combination with the chemometrics assay was directly used as a biosensor array, which exhibited detection limits of 107.33 nM for K + and 19.26 nM for Tl + . The developed method could potentially serve as a diagnostic technique for investigating thallium poisoning and toxicology.
研究领域:
分析化学
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毒理学
·
环境科学
·
纳米技术
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Anyang Tang,Weilun Qian,Junfeng Kong,Wenyu Feng,Huazhen Cao,Huibin Zhang,Guoqu Zheng
A highly effective, stable, and recyclable adsorbent based on titanium dioxide nanofibers (TNFs) was fabricated via a one-step hydrothermal synthesis. The application of TNFs for the deep removal of thallium (Tl) from ammonium perrhenate (NH 4 ReO 4 ) solutions was investigated. The effect of different factors, including hydrothermal temperature and time (120–170 °C, 4–10 h), adsorbent surface area (3–12 cm 2 ), initial concentration of Tl(III) (2–10 mg/L) and pH (2–10) on the removal performance, was analyzed using batch adsorption experiments. Kinetic analysis revealed that the removal process followed a pseudo-first-order model. The adsorption data of TNFs were analyzed using Freundlich and Langmuir isotherms, with the Langmuir isotherm showing the best fit and indicating a theoretical maximum adsorption capacity of 767.2 mg m −2 . Thermodynamic studies demonstrated the adsorption process was characterized by physisorption, being spontaneous, and exothermic. Under optimized conditions, TNFs demonstrated successful removal of Tl(III) from NH 4 ReO 4 solutions with limited adsorption of rhenium (Re) and arsenic (As) ions. Acidity and reusability tests confirmed the significant stability and excellent recoverability of TNFs. The proposed TNFs serve as an effective, and stable adsorbent with a high affinity for Tl(III), offering a viable and efficient approach for the purification of NH 4 ReO 4 solutions.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Chao Wang,Ting Jiang,Junwei Huang,Min Chen,Huimin Hu,Lei Peng,Lei Wu,Zeng Chaocheng,Qiwu Zhang
The remediation of high-concentration thallium (Tl + ) contaminated wastewater is a critical environmental concern. Current research emphasizes the effectiveness of adsorption and oxidation methods for Tl + treatment, yet challenges persist in enhancing their performance. This study explores the feasibility of emergency Tl + wastewater treatment and elucidates the mechanisms of Tl + incorporation into mineral structures, with a focus on the struvite mineral as a framework for Tl + integration via NH 4 + ion exchange. To assess the efficacy and mechanisms of Tl + immobilization, we utilized comprehensive analytical techniques, including X-ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), Fourier-Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopy (SEM-EDS), Thermogravimetric Analysis (TG), and Density Functional Theory (DFT) calculations. The findings reveal that struvite adsorbs Tl + onto its surface, followed by an ion exchange process between monovalent cations (NH 4 + /K + ) within the structure and Tl + . Ultimately, Tl + is incorporated in the form of a (NH 4 ,Tl)MgPO 4 solid solution within the structure, achieving a remarkable maximum incorporation capacity of 320.56 mg/g, which significantly surpasses the capacity of typical adsorbents. The findings demonstrate significant Tl + incorporation, validating the approach for emergency wastewater treatment and suggesting the potential of mineralogy in environmental remediation. This research contributes to advancing heavy metal wastewater treatment strategies, offering a foundation for further investigation.
研究领域:
环境科学
·
矿物学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qiang Ma,Fan Li,Xianglong Zhang,Bowen Yang,Yingjie Zhang,Qingyuan Wang,Qihong Wu,Jin Huang,Jiming Hao
With the rapid development of ore refining, coal power plants, and mining, aqueous thallium pollution in natural waters has been reported over the past few decades. However, few thallium control technologies have been put into practice. In this study, a modified MOF adsorbent, MnO 2 @HKUST-1(MOH), was fabricated. Its chemical component shift, thermal stability, and microstructure changes during thallium adsorption were analyzed using TGA, XRD, XPS, and TEM-EDS techniques. The results showed a promising Tl + removal rate of over 90 %, and an adsorption capacity of 178.8 mg/g was obtained at a pH of 5 and a temperature of 293 K. The dynamic behavior of Tl + adsorption on MOH was simulated using power rate law expression (PRL), pseudo-first-order model (PFO), and pseudo-second-order model (PSO), which revealed a superior selection of Tl + among other competing heavy metal ions (Cr 3+ , Fe 3+ , Ca 2+ , Zn 2+ , and Cu 2+ ). The Tl + removal mechanism was further studied, which was mainly forced by surface adsorption/desorption. Based on its efficient Tl + removal rate, high adsorption capacity, promising regeneration property, and economical price, the MOH adsorbent has the potential to be a feasible option for smelting, ore refining, packaging, and testing wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2022
·Vol. 9
·期 9
·3385-3396
·
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
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）