BIORESOURCE TECHNOLOGY
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2022
·
IF 11.889
Yu-Nan Zhang,Jian-Zhong Guo,Chunzheng Wu,Wei-Wei Huan,Lin Chen,Bing Li
Chemical modification on hydrochars can significantly improve their ability of removing heavy metal ions from wastewater, but so far no research has focused on the chemical modification through free radical reaction. In this work, a cation functionalized hydrochar (CFHC) bearing − N + H 2 R was synthesized by grafting-polymerization of glycidyl methacrylate (GMA) onto bamboo hydrochar under initiation by benzoyl peroxide, followed by the amination with the introduced epoxy group and diethylenetriamine and a subsequent hydrochloric acid treatment. The resulted CFHC exhibited a superior removal capacity of 424.09 mg·g −1 for Cr(VI), and the highest sorption occurred at pH of 2. Combining a series of characterizations and tests, it was concluded that the sorption conformed to the pseudo-second-order and Freundlich equations, indicating a multilayer chemisorption process that mainly driven by electrostatic reaction, reduction, and surface complexation. This research proved that a free radical polymerization treatment could effectively transform hydrochars into super adsorbents for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xuheng Li,Chunli Wang,Feng Liu,Zhihao Zhang,Jafar Ali,Qingwen Long,Jing Zhang
Electrochemical reduction and treatment of Cr(VI)-contaminated wastewater normally suffer from a high overpotential, due to the extravagant consumption of electrons by the adverse reactions of hydrogen evolution and oxygen reduction. In this work, the MoS 2 film electrode prepared by electrochemical deposition-annealing method was applied into the electrochemical reduction of Cr(VI), with the aim to suppress the over-potential of the reduction and improve the utilization of electrons. Results demonstrated that the 2H/1T′ heterostructure of MoS 2 enhanced the reduction efficiency of Cr(VI) up to 99% at a lower potential of −1.0 V vs. Ag/AgCl. The in-situ electrochemically generated hydrogen peroxide was found to play a critical role in accelerating the reduction of Cr(VI). Selective oxygen reduction reaction (ORR) via a two-electron pathway on the MoS 2 cathode was responsible for the formation of hydrogen peroxide, where the MoS 2 film electrode annealed at 700 °C can obtain a high productivity of 360 μM hydrogen peroxide within 60 min. The plenty of preserved interfaces between 2H and 1 T′ in the heterophase MoS 2 were crucial to the selective electrocatalytic activity. In addition, this electrode also presented an excellent electrocatalytic activity in hydrogen evolution reaction (HER), which could form atomic hydrogen on the surface of cathode to facilitate the reduction of Cr(VI) under the anoxic condition. This study paves a novel pathway to in-situ deposit the MoS 2 film electrode for the sustainable electrochemical reduction and treatment of Cr(VI)-containing wastewater.
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Advanced Materials Interfaces
·
2020
·Vol. 7
·期 9
·1901879
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IF 4.948
Shuaishuai Peng,Jingxia Yang,Lei Guo,Jinjie Wang,Jiachang Zhao,Jingli Xu,Zhiquan Li
CeO 2 with different morphologies (nanoparticles/NP, nanorods/NR, nanocubes/NC, nano-octahedra/NO) are synthesized and decorated on BiOI nanoplates substrates to form CeO 2 @BiOI composites, which are used for aqueous Cr(VI) degradation. The intersurface states between BiOI and diverse CeO 2 nanoparticles exhibit distinct behaviors when checked by XPS and photoluminescence intensity. The Cr(VI) degradation results show that the synthesized CeO 2 @BiOI nanocomposites possess higher photocatalytic activity than pure CeO 2 or BiOI, and the CeO 2 -NP@BiOI nanocomposite (molar ratio of CeO 2 : BiOI = 1:2) is the best one among them, with which the Cr(VI) is degraded up to 95.0% after 30 min irradiation using it as the photocatalyst. The superior catalytic performance of CeO 2 -NP@BiOI can be attributed to a higher Ce 3+ ratio of CeO 2 -NP, a larger specific surface area, relatively low OH/CO 3 2− content on the composite surface, and especially the good interaction between the CeO 2 (111) facet and the BiOI surface.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
·
IF 6.1
Nian Liu,Yuqi Zhang,Jiaoyan Huang,Sicong Liu,Taiping Qing,Peng Zhang,Bo Feng
In the realm of sensing, carbon dots (CDs) have exhibited remarkable fluorescence characteristics. In the field of catalysis, CDs can function concurrently as electron donors and acceptors and have substantial electron or hole transport capacities. In this study, both merits were integrated into one, and a one-step hydrothermal approach was used to create multifunctional CDs. On the one hand, CDs are employed as a fluorescence probe with good sensitivity and selectivity to detect Cr(VI). On the other hand, CDs exhibit strong photoreduction capabilities for Cr(VI) in the absence of any external cocatalysts or photosensitizers when acting as photoinitiators. The results show that Cr(VI) quenches the CDs fluorescence as a result of the combined effects of static quenching and the inner filter effect. At the same time, under the condition of illumination, the inner filter effect encourages the CDs electrons to move from the valence band to the conduction band, resulting in electron hole pairs. With the help of electrons' reducing power, Cr(VI) can be rapidly and effectively converted to Cr(III). The findings of this study suggest that CDs are a satisfying bi-functional carbon-based material with significant potential for the treatment of industrial wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 41
·94185-94194
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IF 5.8
Chen Zi-Le,Zhang Yu-Nan,Guo Jian-Zhong,Chen Lin,Li Bing
Hydrochar is an environmentally friendly and cheap adsorbent, but its adsorption amounts for anions is very limited. The functionalized hydrochar can overcome this shortcoming. Herein, polyethyleneimine-modified hydrochar (PEI-HC) was synthesized from hydrothermal carbonization (HTC) of methyl acrylate and bamboo after addition of initiator ammonium persulfate, and then modified by polyethyleneimine (PEI), which was used to treat Cr(VI). PEI-HC was tested by XANES, EXAFS, SEM-EDS, XPS, FTIR, N 2 sorption isotherms, zeta potential, and elemental analyses. The characterizations showed that PEI was successfully grafted onto hydrochar, and the PEI-HC was rich in N and O functional groups, which presented high Cr(VI) sorption ability (528.41 mg·g −1 at pH 2). The bath experiments found the pseudo-second-order kinetic and Freundlich equations can well describe the adsorption kinetics and isotherm of the Cr(VI) adsorption onto PEI-HC, respectively. Electrostatic interaction, reduction, complexation, and H-bonding are the main removal mechanisms as supported by XANES, EXAFS, XPS, and FTIR. This study provides a strategy of combining HTC and free radical graft polymerization to convert agricultural and forestry wastes into functionalized hydrochar, showing highly efficient removal of Cr(VI).
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Yefan Qing,Wei Gao,Yantong Long,Yijin Kang,Chen Xu
The removal of toxic Cr(VI) is a hot topic in the environmental remediation field. In this work, a Ti-based metal–organic framework (MOF) (MIL-125(Ti)-NH2) was successfully functionalized by introducing amidoxime groups for the first time. The functionalized material (MIL-125(Ti)-AO) exhibited excellent Cr(VI) adsorption performance with a maximum adsorption capacity of 271 mg·g–1 according to Langmuir fitting. More importantly, during the adsorption process, Cr(VI) could be simultaneously reduced to less toxic Cr(III) species, and the residual concentration of chromium in the treated water was below the drinking water limit (0.05 mg·L–1) recommended by WHO. The effects of initial pH, contact time, and the initial concentration of Cr(VI) and the presence of competitive ions on the Cr(VI) adsorption performance of MIL-125(Ti)-AO were systematically investigated. The excellent Cr(VI) removal performance of MIL-125(Ti)-AO was attributed to the synergistic effects of simultaneous adsorption of Cr(VI) and Cr(III) by a [Ti–O] bond when Cr(VI) was reduced to Cr(III) by amidoxime groups.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 1
·163-176
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IF 3.442
Yu Sheng,Yuan Guoming,Gao Hejun,Liao Yunwen
The self-assembled polymer nanotubes were obtained by a simple solvothermal method. Its physicochemical properties were characterized by SEM, BET, TGA, FT-IR, XPS, and solid-state 13 C magnetic resonance. The effects of initial pH, dosage, and coexisting ions were evaluated for its Cr(VI) adsorption performances. The result showed that polymer nanotubes surface had a large number of organic functional groups and porous structures. In 140 mg/L Cr(VI) solution, polymer nanotubes obtained the largest Cr(VI) adsorption capacity of 147.81 mg/g. Adsorption kinetics and isotherms agreed well with the pseudo-second-order and Redlich–Peterson models, respectively. The desorption process showed that the polymer nanotubes were easy to regenerate in strong polarity solution and had a high removal efficiency. Ionic strength played an important role in the adsorption and the adsorption interaction contained electrostatic interaction, reduction, and chelation in this work. The self-assembly method will constitute a highly efficient adsorbent.
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WATER RESEARCH
·
2018
·
IF 7.051
Guojun Chen,Juncheng Han,Yang Mu,Huimin Yu,Liping Qin
Chromium isotope fractionation analysis is a promising approach for the assessment of microbial Cr(VI) reduction in groundwater. Understanding the mechanisms and other parameters that control Cr isotope fractionation factors (between the product Cr(III) and reactant Cr (VI)) in microbial Cr(VI) reduction is critical to this application. To date, such studies are very limited. Here, the influence of critical factors on observed Cr isotope fractionation during Cr(VI) reduction by Shewanella oneidensis MR-1 under various conditions was investigated. The Cr(VI) concentration and Cr isotope ratio measurements were conducted on unreacted Cr(VI) remaining in solution to determine Cr isotope fractionation factors. The changes in ambient environmental conditions (e.g., pH, temperature) have limited influence on Cr isotope fractionation factors. However, as a result of Cr(VI) consumption as the experiments proceed, the change in bioavailability of Cr(VI) has a significant impact on Cr isotope fractionation factors. For example, in temperature-controlled experiments, Cr isotope fractionation showed two-stage behavior: during Stage I, the values of ε were −2.81 ± 0.19‰ and −2.60 ± 0.14‰ at 18 °C and 34 °C, respectively; during Stage II, as Cr(VI) reduction progressed, Cr isotope fractionation was significantly masked, and the ε values decreased to −0.98 ± 0.49‰ and −1.01 ± 0.11‰ at 18 °C and 34 °C, respectively. Similar two-stage isotope fractionation behaviors were observed in pH-controlled experiments (pH = 6.0 and 7.2) and in experiments with and without the addition of a competing electron acceptor (nitrate). Masking of isotope fractionation in Stage II indicated restrictions on the bioavailability of Cr(VI) and mass-transfer limitations. This study provides an explanation for the variation in Cr isotope fractionation factors during microbial Cr(VI) reduction in the environment, furthering the viability of Cr isotope ratio analysis as an approach in understanding Cr biogeochemical cycling.
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Materials
·
2022
·Vol. 15
·期 11
·3761
·
IF 3.748
Lei Wu,Doudou Qin,Fan Fang,Weifeng Wang,Wenying Zhao
Severe environmental pollution is caused by the massive discharge of complex industrial wastewater. The photocatalytic technology has been proved as an effective way to solve the problem, while an efficient photocatalyst is the most critical factor. Herein, a new photocatalyst MIL-68(Ga)_NH2was obtained by hydrothermal synthesis and were characterized by PXRD, FTIR,1H NMR, and TGA systematically. The result demonstrates that MIL-68(Ga)_NH2crystallized in orthorhombic system andCmcmspace group with the unit cell parameters:a= 36.699 Å,b= 21.223 Å,c= 6.75 Å,V= 5257.6 Å3, which sheds light on the maintenance of the crystal structure of the prototype material after amino modification. The conversion of Cr(VI) and binary pollutant Cr(VI)/RhB in wastewater under visible light stimulation was characterized by the UV-vis DRS. Complementary experimental results indicate that MIL-68(Ga)_NH2exhibits remarkable photocatalytic activity for Cr(VI) and the degradation rate reaches as high as 98.5% when pH = 2 and ethanol as hole-trapping agent under visible light irradiation with good reusability and stability. Owing to the synergistic effect between Cr(VI) and RhB in the binary pollutant system, MIL-68(Ga)_NH2exhibits excellent catalytic activity for both the pollutants, the degradation efficiency of Cr(VI) and RhB was up to 95.7% and 94.6% under visible light irradiation for 120 min, respectively. The possible removal mechanism of Cr(VI)/RhB based on MIL-68(Ga)_NH2was explored. In addition, Ga-based MOF was applied in the field of photocatalytic treatment of wastewater for the first time, which broadened the application of MOF materials in the field of photocatalysis.
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CELLULOSE
·
2018
·Vol. 25
·期 8
·4757-4769
·
IF 3.809
Li Yunhua,Zhu Hongxiang,Zhang Cunzhi,Cheng Meixiao,He Hui
A novel PEI-grafted magnetic cellulose (Fe 3 O 4 /MCC-PEI) with high amino density was prepared by grafting PEI onto the surface of magnetic cellulose in NaOH/urea aqueous solvent. The embedding of Fe 3 O 4 into cellulose provided excellent magnetic responsiveness for recycling the adsorbent in the magnetic field. The adsorbent for Cr(VI) removal from aqueous solution overcame the disadvantages of adsorbent like difficult recycling, poor regeneration performance and low removal rate at low Cr(VI) concentration. Therefore, the as-prepared Fe 3 O 4 /MCC-PEI showed high Cr(VI) adsorption capacity (198.8 mg/g) which could achieve adsorption equilibrium within 10 min, and the removal rate could reach 100% at low Cr(VI) concentration (less than 1.0 mg/L), demonstrating that the high amino density (7.85 mmol/g) and magnetic responsiveness of the adsorbent can greatly promote adsorption capacity and removal efficiency. The adsorbent also showed promising regeneration performance, and the adsorption capacity remained above 96% after six cycles. Graphical
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Qing Cen,Qiaoyuan Gao,Chenlu Zhang,Yingqi Liu,Qi Wang,Qi Wang
In this study, visible-light-active iron tungstosilicate (FeSiW) was fabricated via solvothermal method . Fe 3+ was applied as counter ion to precipitate with silicotungstic acid (H 4 SiW 12 O 40 ) in methanol solution. It can be observed from FT-IR spectra that the Keggin structure of SiW 12 O 40 4− was well maintained in FeSiW. Besides, the effect of different initial molar ratios of Fe 3+ to H 4 SiW 12 O 40 was investigated (from 4:1 to 4:4). By photoelectrochemical characterizations, such as photocurrent response and Mott-Schottky (M-S) plots, easiest generation of electron-hole pairs and lowest charge transfer resistance can be observed on FeSiW with initial molar ratio of 4:3. Moreover, FeSiW with 4:3 ratio also displayed highest activity for photocatalytic reduction of Cr(VI), despite of the largest band gap (ca. 2.71 eV). The lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) of the optimized FeSiW were estimated to be +0.03 V and 2.74 V vs NHE, respectively, which were thermodynamically feasible for Cr(VI) reduction and H 2 O oxidation . Even under acidic condition (pH 3), the optimized photocatalyst displayed good stability in cyclic runs. Therefore, the present study opens a new way for heterogeneous polyoxometalates as efficient photocatalyst for environmental application.
研究领域:
环境化学
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材料科学
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光催化
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无机化学
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污染治理
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Polymers
·
2025
·Vol. 17
·期 12
·1658
·
IF 4.9
Chenkun Yu,Ze Liang,Ruoyao Zhou,Tingting Gao,Zhaojiang Wang,Xiaoxia Cai,Qian Lu,Cong Li,Jinshui Yao,Qinze Liu
Chromium (III) ions are essential for biological functions, whereas chromium (VI) ions (Cr (VI)) pose toxicity risks to both humans and animals. Therefore, it is crucial to remove these ions from industrial sources. In this work, to remove hazardous Cr (VI) from wastewater or convert it to Cr (III), catechol-modified alkali lignin (CAL) was prepared using catechol, acetone, and alkali lignin, which is a byproduct in the paper-pulping process. The sample was characterized using a combination of techniques, including scanning electron microscopy, thermogravimetric analysis, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. Various factors influencing the adsorption behavior of CAL were investigated. The adsorption behavior aligns with the pseudo-second-order kinetic model and adheres to the Langmuir isotherm model. CAL simultaneously achieves Cr (VI) adsorption (498.4 mg/g) and reduction (54.6% to Cr (III)), surpassing single-function lignin adsorbents by integrating catechol’s redox capacity with lignin’s structural stability, which is another way to efficiently utilize Cr (VI) solutions. The mechanism of adsorption and reduction is discussed, which is influenced by its functional groups. In brief, this method paves a new path for the utilization of alkali lignin and provides novel opportunities for the removal of Cr (VI) contamination.
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