CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Siqi Hou,Wei Ding,Shuang Liu,Huaili Zheng,Jun Zhai,Liuwei Yang,Zheng Zhong
Elimination of As(III) from water has gotten more attention in comparison with As(V) due to its higher mobility and toxicity. In this work, we provide an effective method by integrating a cobalt-based metal–organic framework ZIF-67 and sulfite (S(IV)) to purify As(III)-laden water. The coupled oxidation with adsorption process (i.e., As(III) removal by ZIF-67/S(IV)) surpasses a divided preoxidation-adsorption process (i.e., As(V) removal by ZIF-67) for arsenic removal from the multi-component water containing various coexisting anions. Herein, the mechanism investigation corroborated that the S(IV) plays dual roles as a complexing ligand and a precursor of oxysulfur radicals. The enhanced As(III) removal is attributed to the S(IV) activation on the ZIF-67 surface via various reactions (e.g., surface complexation and intramolecular electron transfer), which not only generates SO 4 − radicals for rapid oxidation of As(III) to As(V), but also provides more adsorption sites for the immobilization of the oxidized product (As(V)). Furthermore, the combined process can rapidly treat arsenic in the realistic contaminated water from 242 to 7 μg L −1 within 15 min, directly meeting the provisional maximum contaminant level (<10 μg L −1 ). Overall, the proposed work may aid the rational design of S(IV) mediated oxidation-adsorption process to remove arsenic from a variety of contaminated waters.
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CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Shams Ali Baig,Jin Zhu,Lisha Tan,Xiaoqin Xue,Chen Sun,Xinhua Xu
Elevated concentration of arsenic in water supplies is detected worldwide and therefore becomes a global issue. Calcination process is known to increase the adsorbent hardness for its effective application in column-based treatment. In this study, magnetic honeycomb briquette cinders (MHBC) and its calcined products: MHBC(A) and MHBC(N) were employed for the adsorptive removal of As(III) in fixed-bed column. Characterizations revealed that the calcination at 1000 °C under nitrogen has significantly increased the adsorbent particles size; favored phase transformation and improved saturation magnetization (>20 emu g − 1 ). Additionally, the new iron silicate phase (Fe 2 SiO 4 ) in aqueous medium generated highly reactive iron oxide species (=FeOOH), which effectively bind As(III) from the influent water by ligand exchanges. In contrast, calcination under dynamic air drastically reduced the saturation magnetization (<1 emu g − 1 ) and assisted to form segregated magnetite, quartz and hematite, as revealed in XRD patterns. The breakthrough curve of each column was compared with Thomas model and found that the model could be applied to estimate As(III) adsorption in fixed-bed column. Thomas model suggested parameters follow the order: MHBC(N) > MHBC > MHBC(A) and the maximum solid phase concentration ( q T ) was found to be about 56.07 mg g − 1 for MHBC(N). The column beds could be successfully regenerated using 200 bed volume of 10% NaOH solution. This study suggests that the selective calcination process need to be integrated with the adsorbent development process for the efficient removal of As(III) from contaminated water using column-based treatment.
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WATER RESEARCH
·
2022
·
IF 13.4
Liping Fang,Baolin Gao,Fangbai Li,Kai Liu,Jialin Chi
The incorporation of secondary metal atoms into iron oxyhydroxides may regulate the surface chemistry of mediating electron transfer (ET) and, therefore, the biogeochemical pollutant processes such as arsenic (As) in the subsurface and soils. The influence of incorporating two typical metals (Cu and Zn) into a specific {001} hematite facet on O 2 activation by surface-bound Fe(II) was addressed. The results showed that Cu-incorporated hematite enhances As(III) oxidation in the presence of Fe(II) under oxic conditions and increases with increasing Cu content. Conversely, Zn incorporation leads to the opposite trend. The As(III) oxidation induced by surface-bound Fe(II) is positively related to the Fe(II) content and is favorable under acidic conditions. Reactive oxygen species (ROS), such as superoxide (·O 2− ) and H 2 O 2 , predominantly contribute to As(III) oxidation as a result of 1-electron transfer from bound Fe(II) to surface O 2 on hematite and radical propagation. Electrochemical analysis demonstrates that Cu incorporation significantly lower the oxidation potential of Fe(II) on hematite, whereas Zn led to a higher reaction potential for Fe(II) oxidation. Subsequently, distinct surface reactivities of hematite for the activation of O 2 to form ROS by surface-bound Fe(II) are evidenced by metal incorporation. Our study provides a new understanding of the changes in the surface chemistry of iron oxyhydroxides because of incorporating metals (Zn and Cu), and therefore impact the biogeochemical processes of pollutants in soils and subsurface environments.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Chengcheng Shen,Li Gu,Sihao Chen,Yajuan Jiang,Peng Huang,Heng Li,Huayang Yu,Dong Xia
Effective utilization and resourcelization of sewage sludge into value-added by-products and insights into its environmental impacts during the fabrication process are urgent tasks to be tackled. Here, we adopt FeCl 3 to activate and functionalize sewage sludge to form FeCl 3 -activated biochars, which exhibited high adsorption capabilities for the treatment of toxic As(III) and Cr(VI) containing wastewaters. Kinetic studies suggested that the adsorption of As(III) and Cr(VI) species onto the biochar surface was attributed to physisorption and chemosorption, respectively. Equilibrium was reached after 3 h for the adsorption of Cr(VI), and slightly slower for that of As(III). Additionally, the structural stability of the adsorbent was maintained even in wastewater with high acidity (pH = 1), as corroborated by microscopic observations. Structural characterization of the adsorbents after adsorption showed that the excellent adsorption performance originated from adsorptive functionalities of the surface functional groups and the active Fe 3 O 4 particles forming Fe-O-As(III)/Fe-O-Cr(VI) complexes with the As(III)/Cr(VI) adsorbates. Evaluation via the green degree method demonstrated that transforming sewage sludge into biochar exerts very low impacts on the environment. Hence, this work offers a green alternative to convert the hazardous sewage sludge into value-added biochar materials, which can be further exploited as supporting frameworks for multifunctional catalysts or expanded to be investigated in reducing carbon footprints and energy conversion areas.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Wenjuan Luo,Xiunan Cai,Zhongqiu Luo,Chaochao Lai,Qian Long,Xue Yang,Limin Ning,Pingyan Wang,Xiang Zhang,Xin Fu,Xintao Zhou
Developing efficient and cost-effective processes for removing highly toxic As(III) from water is critical for environmental restoration. Herein, an amorphous Fe–Mn composite (A-CSM) rich in oxygen vacancies was synthesized via a one-pot process. Acid etching of a pretreated copper slag product created the chemical conditions that simultaneously enabled the in situ anchoring of MnO x clusters and induced a crystalline-to-amorphous transformation. The resulting strong Fe–O–Mn interfacial coupling drives interfacial electron redistribution, which upshifts the d-band center and thereby endows the material with unique capabilities for O 2 activation and arsenic adsorption. Leveraging abundant oxygen vacancies within the amorphous structure, A-CSM efficiently activates O 2 into •O 2 − radicals to drive spontaneous As(III) oxidation to As(V), while exposed unsaturated sites in amorphous FeO x domains provide rapid adsorption sites for As(V). Consequently, A‑CSM exhibits a broad pH range (3–9), rapid adsorption kinetics (achieving complete removal of 5 mg L −1 As(III) within 30 min, which is 24.7 times faster than its crystalline counterpart, CSM), the q max calculated by Langmuir model is 84 mg g −1 , and good reusability over five consecutive cycles. Mechanistic studies confirmed that the synergy between the acid etching‑induced amorphous structure and oxygen vacancies significantly reduces the O 2 adsorption energy while it upshifts the d‑band center. This effect lowers the energy barrier for As(III) oxidation/adsorption by approximately 48.9%, and substantially enhances •O 2 − generation. Adsorption primarily involves complexation, electrostatic interactions, and hydrogen bonding, which is consistent with a heterogeneous multilayer process as described by the Freundlich isotherm.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chen Wang,Zewei Hu,Wei Lou,Mingjie Huang,Wei Xiang,Tao Zhou,Juan Mao,Xiaohui Wu
This study has demonstrated that the Fenton fluidized bed (FFB) technology could successfully immobilize As ions on the iron-crystallized (IC) carriers, with simultaneous crystallization of ferric and mineralization of organic pollutants. It was found that rapid fluidized immobilization of aqueous As(V) on the IC carriers was through surface favorable bidentate complexion, while the adsorptive removal of As(III) was rather slow. Adding Fe 3+ caused competitive complexion and inhibited the As(V) immobilization. However, effective oxidative crystallization of Fe(II) and As(III) in FFB would take place. With the simultaneous generation of As(V) and Fe(III) by rapid •OH oxidation, two different crystalline precursors would be formed on the IC carriers, leading to efficient co-crystallization of As(V)/Fe(III). Recursive Fe(III) crystallization in the FFB continuously provided essential surface hydroxyl groups for capturing As(V), inducing layer-by-layer co-crystallized immobilization As(V)/Fe(III). The long-term continuous-flow treatment of a practical As(III)-containing industrial organic wastewater exhibited effective/stable co-crystallizations of As(V)/Fe(III), as well as COD removal. The FFB technology is expected to be a good option in treating complex industrial wastewater containing heavy metal and recalcitrant organic pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ming Xiao,Ruixue Li,Xinyu Hu,Wenke Zhu,Zhuo Yu,Hongbo Xiao,Wenlei Wang,Ting Yang
This paper is focused on the functional photocatalyst of in-situ carbon-doped TiO 2 decorated Fe 3 O 4 heterojunctions (C/TiO 2 @Fe 3 O 4 ) for the efficient photocatalytic oxidation of As(III). Series of characterizations show that the photocatalytic activity of TiO 2 changes from a single UV wavelength to visible light excitation when carbon atoms are successfully doped in the TiO 2 lattice, expanding the utilization rate of light energy. DFT calculation further confirmed that the C–O–Ti bonds can diminish the theoretical band-gap of TiO 2 . Furthermore, the successful construction of C–O–Ti and Ti–O–Fe interface bonds provide pathways for fast electron transfermation, which can effectively prompt the separation of photo-generated carriers and enhance the photocatalytic oxidation efficiency of As(III). The application results showed that the synthesized C/TiO 2 @Fe 3 O 4 photocatalyst by introducing Fe 3 O 4 with a mass fraction of 1% can complete the transformation of As(III) (10,000 μg/L, 40 mL) to As(Ⅴ) within 12 min under visible light irradiation. In addition, C/TiO 2 @Fe 3 O 4 exhibits excellent reusability, which remains 100% photooxidation efficiency of As(III) without changing crystal structure after 6 cycles and can also be recovered completely with magnet. The remarkable photocatalytic oxidation performances of C/TiO 2 @Fe 3 O 4 can be ascribed to the synergistic effects of OH, O 2 − and h + in the photocatalytic oxidation process and the constructed C–O–Ti and Ti–O–Fe interface bonds.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Chun-Yang Li,Yuan-Yuan Wei,Wei Shen,Xuan Dong,Meng Yang,Juan Wei
The construction of ultrahighly sensitive electrochemical sensing interfaces is essential for the accurate determination of trace-level arsenic(III) (As(III)) due to its severe toxicity. In this report, an ultrahighly sensitive electrochemical sensor was constructed for the electroanalysis of As(III) by the uniform assembly of gold nanoparticles on porous cobaltosic oxide (Co 3 O 4 ) microsheets (AuNPs/Co 3 O 4 nanocomposites). The developed sensor-modified screen-printed carbon electrode (SPCE) detected As(III) by using square wave anodic stripping voltammetry (SWASV) with an ultrahigh sensitivity of 12.1 ± 0.2 µA ppb −1 and a low limit of detection (LOD) of 0.09 ppb (S/ N = 3). The strong electrochemical performance is attributed to the high adsorption capacity of porous Co 3 O 4 microsheets and the favorable electrocatalysis of in situ AuNPs toward As(III) reduction. In addition, the proposed method demonstrates satisfactory anti-interference performance in the presence of other metal ions (Cu(II), Pb(II), Cd(II), Zn(II), Hg(II), Ca(II), Fe(III), Mg(II), Mn(II), and Ni(II)). Robust stability and reproducibility were also realized. Most importantly, the electrochemical sensor was successfully applied to the electroanalysis of As(III) in water and human serum samples. The results of this study provide new insights into the design of sensitive and stable electrochemical sensing interfaces for the accurate analysis of trace levels of As(III) in practical applications.
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WATER AIR AND SOIL POLLUTION
·
2025
·Vol. 236
·期 2
·1-14
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IF 3
Ji Leipeng,Xu Haomiao,Zhang Fubing,Sun Xiaoming,Huang Wenjun,Qu Zan,Yan Naiqiang
H 2 S treatment is a potential method to remove As from smelting wastewater. However, it was difficult to achieve the high concentration As containing wastewater to standard through H 2 S one-step treatment. Meanwhile, the sulfide-abundant conditions after H 2 S treatment changed the As species and the pH condition, which put forward challenges for removing As deeply. In this study, we developed an H 2 S-modification method to prepare sulfide nanoscale zero-valent iron (S-nZVI) to improve the acid resistance and the adsorption performance of adsorbents for As in sulfide-abundant conditions. The results showed that the H 2 S-modification method expanded the pH windows with excellent As(III) removal efficiency from 3 to 7, and at pH value of 3, the As(III) removal efficiency reached 99%. Under pH = 3, the concentration of iron released from nanomaterials decreased from 200 to 20 mg/L, which is attributed to the protection of the surface by the FeS x layer. Moreover, through H 2 S-sulfidation, H 3 AsO 3 (As-O species) transformed to As-S species, which were more challenging to remove than As-O species. In As(III)-S(-II) solution, S-nZVI adsorbed 95% of As(III) in the range of pH 1–5, and the excessive S(-II) could react with Fe(III) to accelerate the cycle of Fe(III)/Fe(II). This improved the efficiency of the Fenton reaction to enhance the oxidation of As(III). Furthermore, consumption of the S(-II) could promote the transformation from As-S species to As-O species. Thus, excellent acid resistance and the synergy with S(-II) made S-nZVI holds great potential to be applied in As(III) removal.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qianfeng Wu,Binbin Tan,Jiang Wang,Zhihao Zhang,Jing Wang,Junlong Liu,Yao Deng,Huidi Zhang,Ting Yang,Wenlei Wang
The utilization of a low-cost common waste biomass, mugwort, with a porous structure is important for the treatment of Arsenic (III) pollution in the aquatic environment. In this study, mugwort straw was first delignified to expose more hydroxyl groups, then loaded with MnOOH and α − FeOOH and constructed with p − n heterojunctions on cellulosic biochar microinterfaces. The successful formation of p − n heterojunction effectively enhances the electric field enhancement inside the photocatalyst, promotes charge transfer and suppresses the recombination of photogenerated carriers. Application of high-energy electron beam irradiation of FMBC−LR2 to modulate the generation and dominant mechanism of Fe and Mn in the reaction system. The results showed that Mn 3+ underwent disproportionation reaction to form Mn 2+ and Mn 4+ . Among them, Mn 2+ led to the formation of MnFe 2 O 4 , while Mn 4+ exhibited stronger oxidizing properties that could promote the transformation of Fe 2+ to Fe 3+ , thus allowing more Fe 3+ to participate in the photocatalytic oxidation of As(III) in a synergistic manner. As(III) oxidation efficiency increased 9.18 times after delignification treatment (FMBC−LR2) and 12.31 times after high-energy electron beam irradiation (FMBC−LR2 − 650) as compared to mugwort straw biochar (BC). In addition, the EPR assay results indicated that ·O 2 − , ·OH, and 1 O 2 acted together in the As(III) reaction. This provides new insights into the remediation of composite modified biochar in water bodies and a new environmentally friendly strategy for the comprehensive utilization of straw materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Like Ouyang,Yan Zhang,Yuan Wang,Xinlong Wang,Shaojun Yuan
The coupled adsorption–photocatalytic oxidation process provides a great potential scenario to enhance the removal efficiency of arsenite contaminants by converting As(III) to As(V) and simultaneous adsorption. In this study, the boron-doped black TiO2/g-C3N4 nanocomposite is synthesized by combination of sol–gel and in situ decomposition-thermal polymerization methods as a photocatalyst for the photocatalytic oxidation and adsorption of As(III). Under dark conditions, the boron-doped samples (B-TiO2 and B-TiO2/g-C3N4) display an increase in the As(III) adsorption capacity by one order of magnitude up to circa 3.2 mg g–1 with an initial As(III) concentration of 2 mg L–1 at 298.15 K and pH 5. The adsorption kinetics of As(III) on B-TiO2/g-C3N4 conform to the pseudo-second-order kinetic model, revealing the chemical adsorption mechanism. Under visible light irradiation, the total arsenic removal capacity is substantially improved by 20% with a removal capacity of 3.9 mg g–1. The enhancement of arsenic adsorption is attributed to the chemical complexation and hydrogen bond, in which B–OH bonds play a dominant role. The photocatalytic oxidation mechanism of the as-synthesized B-TiO2/g-C3N4 is attributed to the synergism of superoxide radicals, hydroxyl radicals, and photogenerated holes.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guiyuan Cai,Yu Tian,Lipin Li,Wenxuan Zhang,Rui Huang,Jun Zhang,Qinyu Wang,Hua Xu,Yifeng Zhang
The activation of sulfite [S(IV)] by transition metals, a new generation of advanced oxidation processes, has been widely studied for water purification. However, the application of this process to oxidize and remove arsenite [As(III)] from water through Fe-based S(IV) activation and the associated mechanisms are not fully understood. In particular, rapid removal of As(III) and secondary metal contamination have presented challenges. Herein, we develop a novel sea urchin-like magnetic Fe-Mn bimetallic oxides (FeMnO)-activated S(IV) process to address these issues. Under neutral pH, the FeMnO/S(IV) system achieved a 99.2 % removal of As(III) within only 10 min with residual arsenic concentration below 10 µg/L, and the removed As(III) was fully oxidized to arsenate [As(V)]. Additionally, FeMnO was recyclable and capable of treating actual arsenic-contaminated water. Furthermore, the oxidation mechanism of non-radical active trivalent manganese [Mn(III)] was discovered during the reaction between the FeMnO/S(IV) system and As(III). The FeMnO catalyst activated S(IV) to generate oxysulfur radicals (i.e., SO 5 •– , SO 4 •– and SO 3 •– ), but they were not the primary oxidizing species for As(III). Instead, As(III) oxidation was mainly attributed to the active Mn(III) generated by the electron transfer between the FeMnO catalyst and SO 5 •– radicals. The discovery of active Mn(III) species in this work may provide a new avenue for developing novel Fe-Mn-type adsorbents to purify arsenic-contaminated water.
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