JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Cuili Xing,Xinyi Yao,Kaiwei Zheng,Yang Liu,Yuankui Sun,Xiaohong Guan
Efficient removal of recalcitrant Cr(III)-organic complexes is always challenged by slow decomplexation process and the possible accumulation of highly toxic Cr(VI). Herein, a sulfidated zero-valent iron coupled ozonation strategy (S-ZVI/O 3 ) was proposed to achieve efficient decomplexation and simultaneous abatement of Cr(III)-EDTA without Cr(VI) accumulation. Results revealed that S-ZVI could catalyze O 3 to enhance removal of Cr(III)-EDTA and total organic carbon. Moreover, 88.3 % of total Cr was sequestrated by S-ZVI/O 3 and the corresponding kinetic constant was 3.1 times higher than that of ZVI/O 3 . Mechanistically, electron paramagnetic resonance and probing tests verified HO • was the dominant reactive oxidation species for decomplexation of Cr(III)-EDTA in both S-ZVI/O 3 and ZVI/O 3 . More attractively, it was found that structural Fe(II) was the major O 3 activator in S-ZVI/O 3 , whereas dissolved Fe 2+ accounted for O 3 catalyzation in ZVI/O 3 . The X-ray absorption spectroscopy analysis revealed that sulfidation treatment could enhance corrosion of ZVI with the formation of sufficient Fe(II) species. The in-situ formed Fe(II) could not only transform undesired Cr(VI) back to Cr(III) but also co-precipitate with Cr(III) to form solid Fe-Cr hydroxides. Besides Cr(III)-EDTA, S-ZVI/O 3 is also applicable to other EDTA complexed heavy metals. This work would provide a new method for the heavy metal complexes removal from water.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Minzi Liao,Shengxi Zhao,Kai Wei,Hongwei Sun,Lizhi Zhang
Cr(III)-organic complexes removal from wastewater is challenging to decompose the complexes without producing toxic Cr(VI). Herein we demonstrated that oxalated zero-valent iron (Ox-ZVI) could one-step decomplex 95.4% of Cr(III)-EDTA with 94.2% removal of total Cr and 60.5% removal of TOC without generating Cr(VI) at pH 6.0. Ox-ZVI with FeC 2 O 4 shell preferred to adsorb and activate O 2 to produce more reactive species than ZVI with iron oxide shell, while the generated 1 O 2 could selectively break the Cr-O and Cr-N bond to precisely decomplex Cr(III)-EDTA without producing Cr(VI). The released Cr(III) was in-situ precipitated on the surface of ZVI in Cr(OH) 3 form. Interestingly, •OH preferred the effective degradation of the released EDTA ligand to the oxidation of the chelated Cr(III) at pH 6.0. This study offers a green and facile method for the Cr(III)-organic complexes treatment, and also sheds light on the importance of reactive species adjustment for the precise pollutant control.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
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2024
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IF 2.2
Hao Zhang,Jiahong Wang,Peiling Han,Zhi Hu
Industrial wastewater often contains potentially toxic metals and it’s chelates, posing serious threats to human health and aquatic ecosystems, and adsorption is frequently used for the minimization of potentially toxic metals from water. In this study, citric acid modified MOF-808 (MOF-808-CA) was prepared by using citric acid to modify MOF-808 for the removal of Cr(III) and Cr(III)-EDTA from wastewater. MOF-808-CA with the BET surface area of 653.59 m2 g−1 and the pore volumes of 0.467 cm3 g−1 was successfully synthesized. The adsorption of Cr(III) and Cr(III)-EDTA by MOF-808-CA was 40.46 and 17.03 mg g−1 at pH 4.0 and 25°C, respectively. The adsorption isotherms and adsorption kinetics of Cr(III) and Cr(III)-EDTA were summarized using Langmuir-Freundlich isothermal adsorption model and the pseudo-second-order model. Even in high salinity wastewater (35,000 mg L−1), MOF-808-CA displayed a strong affinity for Cr(III) and Cr(III)-EDTA. The site energy (E*) values reduced with the increasing of adsorption capacities, and Cr(III) and Cr(III)-EDTA firstly dominated the high-energy adsorption sites before low-energy adsorption sites. The average site energies for the adsorption of Cr(III) and Cr(III)-EDTA by MOF-808-CA were 26.7 and 24 kJ mol−1, respectively, and the differences in the average site energies further illustrated the essential differences in their adsorption mechanisms. The adsorption by electrostatic adsorption and surface complexation were the main adsorption mechanisms for Cr(III) on MOF-808-CA, whereas hydrogen bonding and complexation were the main adsorption mechanisms for Cr(III)-EDTA on MOF-808-CA. The results showed that the MOF-808-CA adsorbent has a great potential for the removal of both Cr(III) and Cr(III)-EDTA from aqueous solutions.
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
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Zhi Hu,Jiahong Wang,Tongtong Sun
A novel tetraethylenepentamine (TEPA) functionalized magnetic mesoporous silica adsorbent (FNMs/TEPA) was prepared for adsorption of Cr(III)-EDTA from wastewater. Characterization of the prepared adsorbent certified that TEPA was modified onto the magnetic mesoporous silicon (FNMs), while FNMs/TEPA maintained the ordered mesoporous and pristine magnetic properties. The batch adsorption experiments demonstrated that TEPA significantly enhanced the removal capacity of the adsorbent for Cr(III)-EDTA. FNMs/TEPA exhibited an excellent adsorption property (13.84 mg∙g –1 ) at pH 4.0. Even in the existence of high concentrations of coexisting ions and organic acids, the adsorption performance of FNMs/TEPA was stable. Experimental characterization and density functional theory (DFT) demonstrated that the adsorption of Cr(III)-EDTA was ascribed to the electrostatic interaction, hydrogen bonding, and complexation between Cr(III)-EDTA and amino groups on the adsorbent surface. The analysis of the Independent Gradient Model (IGMH) shown that electrostatic interaction is the main mode of action in the adsorption process. Moreover, FNMs/TEPA demonstrated remarkable reusability in three regeneration cycles. These findings indicated that FNMs/TEPA possessed excellent application prospect in the disposal of wastewater containing Cr(III)-EDTA.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
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2020
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IF 3.333
Jiahong Wang,Min Mao,Saleem Atif,Yao Chen
The presence of widely used chelating agents such as ethylenediaminetetraacetic acid (EDTA) in aqueous solution increases the difficulty of heavy metal removal by the formation of heavy metal chelates. In this study, diethylenetriaminepentaacetic acid (DTPA)-chitosan functionalized magnetic silica (Fe 3 O 4 @SiO 2 /Cs-DTPA) was developed for the removal of Cr(III) and Cr(III)-EDTA. The obtained results from characterization confirmed that Fe 3 O 4 @SiO 2 /Cs-DTPA with the core-shell structure and superparamagnetic properties was synthesized. The maximum theoretical adsorption capacity of Cr(III) and Cr(III)-EDTA chelates on the adsorbents were 39.27 and 22.24 mg/g at 25 °C and pH 4.0, respectively. Adsorption equilibrium of Cr(III) and Cr(III)-EDTA on Fe 3 O 4 @SiO 2 /Cs-DTPA was achieved within 15 min, and the adsorption data fit the pseudo second-order model. The co-existing complex agents (EDTA) and cations (Na + , Ca 2+ , and Mg 2+ ) in the aqueous solution reduced Cr(III) adsorption by the competition with Cr(III) and Cr(III)-EDTA chelate for active groups of the adsorbent. The affinity of the Fe 3 O 4 @SiO 2 /Cs-DTPA for Cr(III) and Cr(III)-EDTA was excellent even at high salt and organic chelates concentration. The Cr(III) adsorption was attributed to surface complexation between Cr(III) and DTPA moieties of the adsorbent, while Cr(III)-EDTA as a whole was adsorbed on the adsorbent by the complexation and electrostatic interaction . Cr(III) saturated Fe 3 O 4 @SiO 2 /Cs-DTPA can be readily regenerated in acid solution and Cr(III) or Cr(III)-EDTA adsorption of regenerated adsorbent exhibits no obvious reduce.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Linqing Liang,Jiahong Wang,Yanxin Zhang
In this study, H 2 O 2 oxidized magnetic mesoporous carbon hollow microspheres (Fe 3 O 4 @void@C@H 2 O 2 ) with core-shell structure, high magnetic properties and abundant oxygen-containing functional groups was synthesized for removal of Cr(III)-EDTA and Cr(III) in high salinity wastewater. Fe 3 O 4 @void@C@H 2 O 2 was synthesized at optimum conditions of H 2 O 2 concentration of 20%, oxidation temperature of 40 °C and oxidation time of 4 h, and the determined adsorption amount of Cr(III)-EDTA and Cr(III) on the adsorbent was 9.72 and 10.53 mg g −1 at pH 4.0 and 25 °C, respectively. Adsorption behavior of Cr(III)-EDTA could be better described by Langmuir isotherm and Cr(III) adsorption followed Freundlich isotherm. Cr(III)-EDTA and Cr(III) adsorption on the adsorbent followed pseudo-second-order kinetics, and adsorption rate of Cr(III) adsorption on the adsorbent is higher than that of Cr(III)-EDTA. Fe 3 O 4 @void@C@H 2 O 2 showed strong affinity for Cr(III) and Cr(III)-EDTA even in high salinity water. Moreover, Fe 3 O 4 @void@C@H 2 O 2 exhibited the high stability in acid solution and Cr(III) saturated adsorbent can be easily regenerated in 0.1 mol L −1 HCl. Cr(III)-EDTA adsorption was described to the surface complexation between the oxygen-containing groups (such as hydroxyl, carbonyl and carboxyl groups) of the adsorbent and Cr(III) in Cr(III)-EDTA, and the hydrogen bonding between oxygen-containing groups of the adsorbent and EDTA of Cr(III)-EDTA, while Cr(III) adsorption on the adsorbent was surface complexation and ion exchange. The results highlighted that Fe 3 O 4 @void@C@H 2 O 2 have great potentials for adsorptive removal of Cr(III) and it's chelate from the high salinity 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
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2020
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IF 4.872
Jiahong Wang,Yao Chen,Tongtong Sun,Atif Saleem,Chuanyi Wang
A novel amino-functionalized magnetic adsorbent (Fe 3 O 4 @C@DETA) was developed for adsorption of Cr(III) and Cr(III)-EDTA from wastewater. Fe 3 O 4 @C@DETA were successfully prepared by modification of Fe 3 O 4 @C with diethylenediamine (DETA), which exhibits a core-shell structure and sufficient saturation magnetization. Fe 3 O 4 @C@DETA exhibits much better adsorption performance for Cr(III) and its chelates than the Fe 3 O 4 @C because of newly introduced amino active sites. The enhanced adsorption capacity of Fe 3 O 4 @C@DETA for Cr(III) is 44.74 mg g −1 (at 25 °C and pH 3.0), which is due to the surface coordination with the newly introduced amino functional sites. The Cr(III)-EDTA anions as a whole was adsorbed through the electrostatic interaction with protonated amino species of the Fe 3 O 4 @C@DETA and have maximum adsorption capacity of 47.27 mg g −1 (at 25 °C and pH 3.0). The adsorption data of free and EDTA coordinated Cr(III) were followed the Langmuir equation, while the adsorption dynamics was well explained by pseudo second order model indicating the chemical nature of adsorption process. The higher concentration of Ca 2+ ions in the wastewater compete for adsorption sites and inhibit the Cr(III) removal, while on other hand Ca 2+ ions promotes the adsorption of Cr(III)-EDTA, because of electrostatic interaction with adsorbent active sits. Furthermore, the adsorbent can be easily separated by external magnetic field and regenerated in acidic solution. The adsorbent is stable, recyclable and have more than 75% regeneration efficiency and can be repeatedly used in the adsorption process.
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 SCIENCE AND TECHNOLOGY
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2024
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IF 2.3
Yuanpei Zhang,Jiahong Wang,Jinming Huang,Zhi Hu
In this study, zirconia-functionalized magnetic core-shell mesoporous carbon composites (Fe3O4@C-ZrO2) were synthesized for the effective removal of Cr(III)-EDTA in high-salinity wastewater. Fe3O4@C-ZrO2 with Fe3O4 as a magnetic core and ZrO2 embedded in a mesoporous carbon skeleton were prepared by the sol-gel method in the nano-casting stage, which can be magnetically separated. The presence of ZrO2 on the adsorbents enhanced the adsorption of Cr(III)-EDTA and the maximum adsorption capacity of Fe3O4@C-ZrO2 was 16.21 mg·g−1 at pH = 3.0, which is remarkably higher than that of Fe3O4@C (3.65 mg·g−1). Fe3O4@C-ZrO2 has a strong anti-interference capability for cations in water, which can exhibit effective adsorption properties in presence of high concentration cations and anions (80 mmol·L−1) and high salt/complexant agent environments. Cr(III)-EDTA removal by adsorption of Fe3O4@C-ZrO2 was mainly through the formation of ternary complexes between ZrO2 in Fe3O4@C-ZrO2 and carboxylic acid groups in Cr(III)-EDTA. The Cr(III)-EDTA saturated Fe3O4@C-ZrO2 can be easily regenerated in 0.1 mol·L−1 NaOH than in 0.1 mol·L−1 HCl and still demonstrated an effective adsorption capacity for Cr(III)-EDTA after three repeated cycles. The results reflect the effective removal of Cr(III)-EDTA by Fe3O4@C-ZrO2 in high-salinity water, providing a new method for removing heavy metals in complex water.
研究领域:
环境科学
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材料科学
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水处理
✓ 已验证
产品关联
DOI
高影响因子
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