RSC Advances
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2020
·Vol. 10
·期 72
·44470-44480
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IF 3.119
Shu-Xin Pan,Ting-Zheng Xie,Tang-Fu Xiao,Jie-Hui Xie
Thallium (Tl) is a highly toxic heavy metal, and its pollution and remediation in aquatic environments has attracted considerable attention. To reduce or remove Tl pollution in the environment, various strategies have been applied. Graphene oxide (GO) has abundant oxygen-containing functional groups, indicating its high application potential for pollution remediation via methods involving binding to metal ions or positively charged organic molecules or electrostatic interaction and coordination. However, the adsorption of Tl to GO occurs via physical adsorption, for which the adsorption efficiency is low. Therefore, herein, we report a new method to effectively remove Tl pollution in water. We combined GO with aza-crown ether, which enhanced the electronegativity and ability to bind metal ions. The functionalized graphene oxide (FGO) demonstrated high efficiency through a wide pH gradient of 5–10, with a dominant Tl(I) adsorption capacity (112.21 mg g−1) based on the Langmuir model (pH 9.0, adsorbent concentration of 0.8 g L−1). The adsorption of Tl(I) during removal fit a pseudo-second-order kinetic model well. The mechanisms of Tl removal involve physical and chemical adsorption. In summary, our study provides a new method for the detection and treatment of Tl-containing wastewater by using FGO.
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
LANGMUIR
·
2023
·
IF 3.9
Qiang Ma,Lijun Jiang,Bowen Yang,Bowen Xu,Qingyuan Wang,Qihong Wu,Ping Ning,Yingjie Zhang,Jin Huang,Jiming Hao
Gaseous thallium (Tl) pollution events, primarily caused by non-ferrous mineral refineries and fossil fuel combustion, have increased over the past few decades. To prevent gaseous Tl distribution from flue gas, MnO2/CeO2@HKUST-1 (MCH) was synthesized and found to achieve a gaseous Tl(I) removal level of up to 90% at 423 K, a weight hourly space velocity (WHSV) of 2000 h–1/mL with an Mn dose of 10%, maintained over 10 h. The best Mn/Ce ratio was found to be 9:1. To further investigate surface kinetic behavior, four commonly used kinetic models were applied, including the Eley–Rideal (ER) model, Langmuir–Hinshelwood (LH) model, Mars–van Krevelen (MVK) model, and pseudo-first-order (PFO) model. While the ER and LH models had the slightest deviation, the MVK model was the most reliable. The CatMAP software was also used to match the simulation deviation. This work demonstrated the Tl removal mechanism and provided insights into the accuracy of kinetic models on minor-radius heavy metal. Thus, this research may help promote the design of reactors, heavy metal removal rates, and flue gas purification technology selection.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tao Huang,Dongping Song,Xinxin Wang,Yuxing Wang,Nan Shang,Si Liu,Lulu Zhou,Yujie Yan
Thallium (Tl) is a highly toxic element and can accumulate in human body through food, water, or air and cause damage to multiple organs. In this study, the nonthermal plasma (NTP) was employed to irradiate the potassium dihydrogen phosphate (KH 2 PO 4 ) and sodium diethyldithiocarbamate trihydrate (SDDC) to solve the issues brought by their poor stability and insufficient chelation capabilities in soils to intensify their performance on immobilizing monovalent Tl contaminants in soils. Both an orthogonal design (OD) and a central composite design (CCD) were adopted to arrange the multi-parametrical modification and stabilization experiments. The leaching toxicities ranging from 5.11 to 52.37 µg/L of Tl + ions were obtained in the OD experiments. The changes in both NTP time and the molar ratios of KH 2 PO 4 to SDDC had a significant effect on the activation procedure. The leaching concentration ranging from 0.37 to 7.34 µg/L was achieved in the CCD stabilization experiments. NTP activation and the rearrangement of the stabilization conditions both were beneficial to the transformation of physicochemical states of Tl pollutants in soils, which proved the existence of chemical immobilization brought by the irradiated stabilizers (NTP-PK-SDDCs) to the Tl contaminants. The stabilization process was targeted between only Tl contaminants and NTP-PK-SDDCs in soils. The NTP irradiation enhanced the physicochemical characteristics of stabilizers, further intensifying the immobilization of Tl species in the soils. The enhancement mechanism was attributed to the free radicals-induced doping, oxidation, and polycondensation and the bombards of electrons, which strengthened the electrostation and chemisorption of NTP-PK-SDDCs towards Tl ions. The potential impact of this study includes the development of more effective and sustainable remediation methods for Tl-contaminated soils, contributing to environmental protection and human health.
研究领域:
环境科学
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化学
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Tao Huang,Dongping Song,Zhengfeng Hu,Yuxuan Feng,Jialin Cui,Mengyue Wu,Di Wu,Yinglan Luo,Yue Li,Yirong Jiang,Chaojun Tang,DanDan Wang
The urgent need for remediation of thallium (Tl)-contaminated soils arises from its widespread presence as a poisonous heavy metal (HM), coupled with numerous challenges such as high costs, long durations, secondary pollution risks, and technological limitations. In the study, a novel approach has been introduced to the remediation of Tl-contaminated soils using calcium sulphoaluminate cement. This innovation involves the employment of nonthermal plasma-irradiated polyvalent Ce-Mn (hydro)oxide-modified nanographene (NTP-P-Ce-Mn-NGs) to intensify the cementation and immobilization of Tl species. The chemical speciation of Tl contaminants influenced by the dosage of NTP-P-Ce-Mn-NGs in the cementation was measured to explore the potential enhancement mechanisms brought by NTP-P-Ce-Mn-NGs in the sulphoaluminate cementation. Comprehensive strategies were adopted to explore the reaction pathways. In orthogonal (OD) experiments, compressive strengths ranging from 22.14 to 56.78 MPa in sulphoaluminate-cemented cubes were achieved. Remarkably, when NTP-P-Ce-Mn-NGs were introduced, the leached Tl concentration was reduced to 0.21–21.46 µg/L. This significant reduction was attributed to the NTP-P-Ce-Mn-NGs-induced more uniform hydration reactions and a more holistic microstructure. The presence of diverse valent Ce and Mn species within the matrix was confirmed, revealing a reliable interaction between NTP-irradiated high-valent Mn and Ce with monovalent Tl ions. This interaction induced multiple redox reactions, immobilizing Tl contaminants within the matrix and the cementation encapsulation. This study represents a significant milestone in Tl pollution control, paving the way for more efficient and cost-effective soil remediation strategies.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tao Huang,Dongping Song,Qi Fang,Chaojun Yang,Di Wu,Shouze Li,Yinglan Luo,Yujie Yan,Zhengfeng Hu
Thallium (Tl) enrichment in soils can cause an immeasurable ecological disaster, disturbing ecological balance and threatening human health. In this study, nonthermal plasma (NTP) irradiation was employed to synthesize polyvalent Mn-based (hydro)oxide-functionalized nanosilica (NTP-P-Mn-nSi). Mixtures of alkali-activated geopolymers and NTP-P-Mn-nSi were subsequently prepared for the efficient solidification and stabilization (S/S) of Tl-containing soils. The synthesis of NTP-P-Mn-nSi and the geopolymerization of soils were both optimized to obtain maximum adsorption capacities and achieve excellent immobilization of the matrix. The influence of the initial pH and concentration of Tl + on NTP-P-Mn-nSi was investigated. The leaching concentration of Tl and the compressive strengths from the soil matrix were monitored. Comprehensive strategies were adopted for soils and solidified samples to investigate the vital role played by NTP-P-Mn-nSi in the geopolymers of soils. The pseudofirst-order, intraparticle, and Elovich models were suitable for evaluating the uptake dynamics of Tl + to NTP-P-Mn-nSi. Langmuir, Freundlich, and Tempkin were all appropriate in analysing the isotherms of heterogeneous adsorption. Four maximum monolayer adsorption capacities of NTP-P-Mn-nSi responding to Tl + ions reached 93.90, 123.00, 355.87, and 323.62 mg/g at initial pH values of 7, 9, 11, and 13, respectively. NTP-P-Mn-nSi in the geopolymer explicitly inhibited leaching and intensified the immobilization of Tl ions in the matrix with the lowest leaching concentration of 0.16 µg/L Tl from the matrix being achieved. The increase in NTP-P-Mn-nSi dosage accelerated the growth rates of nucleation, enhanced the formation of alkali-activated gelation, induced the formation of flocculent surfaces and three-dimensional structures, and intensified the elemental overlap between Mn and Tl in the geopolymerized matrix.
研究领域:
环境科学
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材料科学
·
化学工程
·
土壤学
✓ 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）