CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tong-liang Wu,Qian Sun,Guo-dong Fang,Pei-xin Cui,Cun Liu,Marcelo Eduardo Alves,Wen-xiu Qin,Dong-mei Zhou,Zhen-qing Shi,Yu-jun Wang
Natural organic matter (NOM) profoundly influences the metal(loid)s immobilization by iron (Fe) minerals, which, in turn, are the host phase for Sb that control its mobilization and bioavailability. However, the potential effect of the redox-active phenolic acids derived from NOM on this process has rarely been explored. Therefore, the adsorption of Sb(III) on goethite and Sb(III) oxidation in the presence of a common phenolic acid—gallic acid (GA)—was systematically investigated. The reaction mechanisms were unraveled by the combination of wet chemistry, electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine structure (XAFS) spectroscopy. Our results showed the addition of GA significantly inhibited Sb adsorption on goethite as the pH increased. Except for the competitive adsorption by GA, the inhibition also resulted from the extensive Sb(III) oxidation in the suspension and the lower Sb(V) sorption capacity of goethite at higher pH. The alkaline condition facilitated the generation of reactive oxygen species (hydrogen peroxide) and quinone species (semiquinone radical (SQ − ) and oxidized GA), accounting for the significant Sb(III) oxidation in the solution and on the goethite surface. Besides, the edge-sharing inner-sphere complexes were formed between Sb and goethite regardless of the presence of GA. Our findings demonstrated the remarkable role of the phenolic groups in NOM on the adsorption of Sb(III) on goethite.
研究领域:
环境科学
·
土壤化学
✓ 已验证
产品关联
DOI
高影响因子
GEODERMA
·
2023
·
IF 6.1
Tongliang Wu,Cun Liu,Peixin Cui,Hongjing Zhang,Sainan Hu,Peng Zhang,Qin Xue,Yaodong Wang,Chenglong Feng,Marcelo Eduardo Alves,Matthew K. Tighe,Yujun Wang
A quantitative evaluation of the dynamics of antimony (Sb) species transformation when Sb(III) enters the soil matrix would facilitate the understanding of the speciation and environmental fate of Sb in natural environments. Towards this end, the coupled sorption and abiotic oxidation kinetics of Sb(III) were examined across 12 soils with a 24 h timeframe. The soil-solution distribution coefficients (K d ) of Sb ranged between 214 and 5965 L kg −1 . Both apparent and mechanistic kinetic models were used to described the process. The apparent kinetic model indicated a two-rate oxidation and associated stabilization behavior of Sb in soils. The fast oxidation rate constants ranged from 0.147 to 0.763 h −1 , which were one to two orders of magnitudes higher than the slow rate constants (0.002–0.039 h −1 ). Iron and Mn oxides were identified as the key soil components associated with adsorptive-oxidative sites (SOH) and oxidative sites (Mn-OH) of soils for Sb species, and these were subsequently integrated into the mechanistic kinetic model. This model included the adsorption–desorption of Sb(III) as well as the oxidation product, Sb(V) on the SOH, the oxidation of Sb(III) by SOH and Mn-OH, and the stabilization of both Sb(III) and Sb(V). The model produced a global fit for dissolved and adsorbed Sb species across the 12 soils. This study provides new information for predicting the dynamics of Sb in soils when multiple adsorption–desorption, oxidation and stabilization reactions are coupled in natural environments.
研究领域:
环境科学
·
土壤学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Hong-Tao Fan,Qi Tang,Yang Sun,Zhi-Gang Zhang,Wen-Xiu Li
A Sb(III)-imprinted iodole-functionalized organic–inorganic hybrid sorbent was synthesized by combination of surface imprinting technique with sol–gel process for the selective removal of Sb(III) from aqueous media. The material was characterized by Fourier-transform infrared spectroscopy, transmission electron microscopy, thermogravimetric analysis and nitrogen adsorption–desorption isotherms. Compared to the non-imprinted sorbent, the imprinted hybrid sorbent had higher selectivity and adsorption capacity for Sb(III) ion. The static adsorption capacity of the imprinted and non-imprinted sorbents for Sb(III) was 32.4 and 11.1 mg g −1 , respectively. The relative selectivity coefficients of the imprinted hybrid sorbent for Sb(III)/Cr(III) Sb(III)/Fe(III) and Sb(III)/As(III) were 13.2, 10.4 and 11.8, respectively. The imprinted hybrid sorbent possessed fast kinetics for the removal of Sb(III) from aqueous solution with a saturation time of 30 min, had a stable binding capacity in the range of pH 4–6, and could be used repeatedly. Both the pseudo-second-order kinetic model and the Langmuir model fit the experimental data well. It could be concluded from the thermodynamic parameters that the adsorption of Sb(III) on the imprinted hybrid sorbents was an exothermic and spontaneous process.
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
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Qi Cheng,Qingrui Li,Xiaojie Huang,Xiaoqin Li,Yunyan Wang,Weizhen Liu,Zhang Lin
In this study, cauliflower like amorphous nanoscale zero-valent iron (A-nZVI) was prepared and its performance on the removal of Sb(III) was investigated and compared with that of nZVI. The results indicated that the removal of Sb(III) by nZVI and A-nZVI followed the pseudo-second-order kinetic model and Langmuir isotherm model, but the removal of Sb(III) by A-nZVI was more stable and its removal capacity (558.2 mg/g) is much higher than that of nZVI (91.3 mg/g). Moreover, the effects of initial Sb(III) concentration, initial pH and anions such as Cl - , NO 3 - , SO 4 2- , PO 4 3- , and AsO 4 3- were also investigated. A-nZVI showed extremely high selectivity towards Sb(III) in that 500 mg/L of AsO 4 3- and PO 4 3- shows little impact on its removal, while the removal of Sb(III) by nZVI was almost inhibited under the same condition. The combination of SEM-EDS, XPS, XRD and FTIR revealed the removal of Sb(III) by nZVI and A-nZVI were synergistic effects of oxidation and adsorption, but less Sb(III) (39.5%) was oxidized by A-nZVI. More γ-FeOOH and γ-Fe 2 O 3 were formed at the surface of A-nZVI during the reaction. Both oxides have high affinity toward Sb(III), which might cause the higher removal capacity and selectivity for the removal of Sb(III) by A-nZVI. In conclusion, A-nZVI showed great potential for the remediation of Sb(III) in groundwater.
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
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Pengyang Bian,Bei Gao,Junhao Zhu,Huimin Yang,Yue Li,Ermao Ding,Yixuan Liu,Yaxing Liu,Shichen Wang,Weibo Shen
The pollution and harm of Sb 3+ to aquatic systems is a global problem, so Sb 3+ removal from the water environment to make sure environment safety and human beings wellbeing is of urgency. This study explored the effect of chitosan combined with nicotinamide-modified eupatorium adenophorum biochar (CEBC) on adsorbing Sb 3+ through batch adsorption experiments. The experiments indicated CEBC's maximum adsorption capacity to Sb 3+ is 170.15 mg·g −1 . Meanwhile, the capacity of the original biochar (EBC) is only 9.97 mg·g −1 . Compared with EBC, CEBC contains more functional groups, such as C O, -OH and -NH 2 . In addition, the pseudo-second-order kinetic model and the Langmuir model are fit to describe the kinetics and isotherms of adsorption of CEBC to Sb 3+ , which suggests that the adsorption of CEBC to Sb 3+ is dominated by monolayer chemisorption. Density functional theory (DFT) calculations confirmed that the chelation between –NH 2 and Sb 3+ is of significance in the adsorption process of CEBC. DFT calculations also found that the newly added –OH and C O in EBC have a synergistic enhancement effect on the absorption of Sb 3+ . The mechanism of CEBC absorbing Sb 3+ includes electrostatic interactions, pore filling, Л–Л interactions, hydrogen bonding, functional group complexation, chelation, and oxidation . CEBC has an excellent anti-interference ability for inorganic anions (NO 3 − , SO 4 2− and Cl − ) and can also use the coexisting HA to improve its adsorption performance. In addition, CEBC has better mitigation of Sb 3+ on the performance of Sb 3+ about its secondary release and good reproducibility, which indicates that CEBC is a viable Sb 3+ adsorbent.
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
ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Si Xu,Zuqi Zhong,Weizhen Liu,Hong Deng,Zhang Lin
Pollution and remediation of antimony in aquatic ecosystems have been paid increasing attention. In the present work, environmentally friendly nano-MgO was used for the first time to remove Sb(III) from the water system. The batch experiments indicated that the nano-MgO calcined at 400 °C (named 400-MgO) exhibited superior adsorption capacity for Sb(III). The adsorption isotherm was fitted well with the Freundlich model, and especially when the initial concentration is 15 mg‧L −1 , the adsorption capacity is as high as 140.1 mg‧g −1 . Researches through X-ray diffraction (XRD), Transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS) showed that the main removal mechanisms lie in the generation of Mg active sites, which is capable of coordinating Sb(III), during the hydration process of MgO, providing a nucleation center for the progressive production of MgSb 2 O 4 . As a whole, precipitation is the predominant mechanism for MgO to remove Sb(III). Over time, a part of MgO is hydrated to Mg(OH) 2 , and consequent chemisorption also helps to remove Sb(III). Our work has demonstrated that nano-MgO is a promising adsorbent for Sb(III) removal from contaminated water and provided new insights into the interaction mechanism between MgO and Sb(III).
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Pengfei Qi,Rong Luo,Thomas Pichler,Jianqiang Zeng,Yan Wang,Yuhua Fan,Kunyan Sui
Removal of trivalent species of As and Sb from wastewater is crucial due to their more toxic and mobile properties. In this study, a novel magnetic core-shell microsphere Fe 3 O 4 @TA@UiO-66 was developed via in-situ crystal growth of UiO-66 around the magnetic Fe 3 O 4 modified by Tannic Acid (TA). Characterization of the microsphere by transmission electron microscopy (TEM) and X-ray diffraction spectroscopy (XRD) confirmed that UiO-66 was adhered on the surface of Fe 3 O 4 functionalized by TA. Adsorption experiments showed that the magnetic Fe 3 O 4 @TA@UiO-66 had high adsorption capacity for As(III) and Sb(III) and could be rapidly separated from aqueous media within two minutes after treatment. The adsorption kinetics and adsorption isotherms were described well by the pesudo-second order model and Langmuir model, respectively. In addition, the composite exhibited excellent removal performance for As(III) and Sb(III) in a broad solution chemistry environment, including pH and co-existing anions. Based on X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) measurement, we proposed that the removal mechanism was mainly controlled through a synergistic interaction of surface complexation and hydrogen bonding. This study indicates the potential of the magnetic microsphere to be used as an effective material for the removal of As(III) and Sb(III) from water.
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
Surfaces and Interfaces
·
2024
·
IF 5.7
Jianle Wang,Na Li,Le Yuan,Qing Zhu,Nan Lan,Zejia Zhao,Zhixu Chen,Xueming Liu,Hong Deng
In recent years, the search for effective antimony adsorption materials has been unyielding. However, the exploration of zeolite imidazolate frameworks (ZIFs) as potential adsorbents, along with the influence of material surface structure and water chemistry on their performance remain under explored. In this study, various molar ratios of Zn 2+ and 2-methylimidazole are employed to synthesize three distinct shapes of ZIFs: cube , leaf, and dodecahedron . The experimental outcomes reveal that Leaf-ZIFs, exhibit exceptional adsorption capabilities for Sb(III), the maximum adsorption capacity of Leaf-ZIFs was 57.3 mg g −1 . The adsorption kinetics adhere to the pseudo-second-order model, and equilibrium is achieved in approximately 10 h. Additionally, the adsorption isotherm curve is consistent with the Freundlich model. Through comprehensive batch experiments, we thoroughly examined the impact of varying solution pH levels, coexisting ions, and the coexistence of humic acids on the adsorption of Sb(III). The Leaf-ZIFs exhibited remarkable adaptability in neutral, alkaline, and low-concentration heteroionic environments, while demonstrating minimal interference from humic acid present in the solution. Analysis using SEM, XPS, and FTIR techniques revealed that the adsorption mechanism of Leaf-ZIFs primarily involved the partial breakage of the Zn-N bond within the material's structure . This breakage led to the formation of Zn-OH groups, which subsequently reacted with Sb(III) molecules through the -OH groups. The culmination of this process was the formation of Zn-O-Sb bonds, resulting in the effective adsorption of Sb(III) from aqueous solutions.
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
·
2024
·
IF 12.2
Yuhan Zhang,Huan Wang,Zhichao Song,Caijian Wang,Jingwei Hou,Kunyan Sui,Pengfei Qi
Selective autonomous enrichment of micropollutants in the aquatic media has attracted increasing attention because of their low concentration characteristics and diverse coexisting species. Herein, the gradient hydrogels were prepared via free redical polymerization of AA and NH 2 -β-CD under the induction of unilateral UV illumination (P(AA-NH 2 -β-CD)). The gradient hydrogels present autonomous enrichment towards Sb(III) with a higher selectivity both in single and binary solutions. The simulation calculations proved that the electrostatic potential of the gradient hydrogel is almost identical before and after enrichment of Sb(III), suggesting that the formed hydrogen bonds between carboxyl and hydroxyl groups with gradient distribution play vital voles on its higher selectivity by gradient hydrogels. Moreover, the gradient P(AA-NH 2 -β-CD) hydrogels showed selective self-driven enrichment performance for identically charged organic dyes based on host-guest and electrostatic interactions. For the positively charged model pollutants, the gradient hydrogels exhibited a superior selective enrichment performance for MG than X-GRL with a lower K value. The as-prepared gradient hdyrogel may have potential applications for the self-driven and selective removal of micropollutants.
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
Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·3047-3061
·
IF 7.683
Yang Bai,Fan Wu,Yanyan Gong
Antimony(III) or Sb(III) contamination in surface waters poses a serious threat to the ecological system and human health, and green and cost-effective technologies are urgently needed to mitigate its toxic effects. We green synthesized a novel oxidative sorbent, referred to as Al2O3-supported Fe–Mn binary oxide nanoparticles (Fe–Mn@Al2O3), and investigated its removal effectiveness and dynamic quantitative removal mechanisms of Sb(III) at environmentally relevant levels from simulated surface water. Fe–Mn binary oxides (Fe–Mn) were successfully attached on the surface of Al2O3via intermolecular hydrogen bonding, resulting in the formation of Fe–Mn@Al2O3 with a larger specific surface area, greater oxidizing reactivity, and more sorption sites compared to Fe–Mn. The resulting composite is mainly composed of FeOOH, Fe2O3, MnO2, and Al2O3. Life cycle assessment (LCA) indicated that the Fe–Mn@Al2O3 synthesis met green chemistry principles. Fe–Mn@Al2O3 at a Fe : Al2O3 molar ratio of 1 : 2 displayed an enhanced Sb(III) sorption capacity of 272.2 mg g−1 at pH 6.4 within 48 h. Sorption kinetic data were adequately simulated with the pseudo second-order kinetic model and the intraparticle diffusion model, suggesting that the sorption kinetics were a combination of chemisorption and intraparticle diffusion. The Freundlich isotherm model outperformed the Langmuir model in simulating the sorption isotherm data, which aligns with the heterogeneous surface sorption sites of Fe–Mn@Al2O3. MnO2 in Fe–Mn@Al2O3 oxidized Sb(III) to Sb(V), whereas FeOOH and Al2O3 acted as adsorption sites towards Sb(III) and Sb(V). Most importantly, Fe–Mn@Al2O3 still maintained high sorption efficiencies towards Sb(III) after five consecutive regeneration cycles. The dynamic quantitative removal mechanisms were proposed thereafter. Upon equilibrium, 92.8% of Sb(III) was sorbed by Fe–Mn@Al2O3, and 94.9% of sorbed Sb(III) was oxidized to produce Sb(V) and Mn(II). 59.1% of the formed Sb(V) was adsorbed onto Fe-Mn@Al2O3 and 40.9% of Sb(V) was released into the solution. The new quantitative and mechanistic insights contribute to an improved understanding of the uptake of Sb(III) by Fe–Mn@Al2O3 in natural and engineered systems, and the results may guide further preparation and application of reactive adsorbents for removal of redox-active contaminants from water.
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
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2020
·
IF 4.872
Cong Liu,Ye Li,Xiaoli Wang,Bolin Li,Yuzhi Zhou,Dongbin Liu,Dongxue Liu,Shuang Liu
Antimony has been listed as a critical pollutant in many countries because of its toxic effects on earth organisms. In this study, titanate nanosheets (TNS) were prepared with a high specific surface area by alkaline hydrothermal method. The adsorption mechanism and adsorption capacity of removing Sb(III) from aqueous solutions with TNS as an adsorbent were investigated for the first time. The FTIR and XPS analysis indicated that the interlayer sodium ions of TNS were responsible for Sb(III) adsorption. The batch experiments were conducted on solution pH, adsorbent dosage, initial concentration and reaction time. The results exhibited that when pH was 2, the removal rate was about 90% with the dosage of TNS was 0.1 g/L. The adsorption reaction was exceedingly rapid in the initial 5 min, and then the reaction was in equilibrium after about 30 min. The experimental data were better fitted with Langmuir isotherm model, and the maximum adsorption amount could attain 232.56 mg/g. The experiments showed that TNS had outstanding anti-interference performance to common cations. Therefore, TNS were considered to be an excellent material for removing Sb(III) from aqueous solutions.
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
Journal of the Taiwan Institute of Chemical Engineers
·
2014
·
IF 2.637
Hong-Tao Fan,Yang Sun,Qi Tang,Wen-Liu Li,Ting Sun
In this work, a novel Sb(III)-imprinted organic–inorganic hybrid sorbent was synthesized by surface imprinting technique combined with a sol–gel process, and characterized by scanning electron microscopy, Fourier-transform infrared spectroscopy, and N 2 adsorption–desorption isotherms. The imprinted sorbent showed the higher capacity and higher selectivity than that of non-imprinted sorbent. The optimal pH range for adsorption of Sb(III) was 3.5–6.5. The imprinted sorbent possessed a rapid kinetics for adsorption of Sb(III) with saturation time of 20 min. After nine adsorption/desorption cycles, no obvious decrease of adsorption capacity was observed. The experimental data showed that the adsorption process obeyed the pseudo-second-order rate mechanism and Langmuir isotherm. The thermodynamic parameters indicated that the adsorption of Sb(III) on the imprinted sorbent was an exothermic and spontaneous process.
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）