CHEMOSPHERE
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2022
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IF 8.943
Hongwei Wang,Fang Wu,Zhiheng Wang,Yang Wang,Shufang Zhang,Haijun Luo,Zhiqin Zheng,Liang Fang
Chromium (VI) removal is crucial to the safety of water resources, but there is still a lack of effective and fast dislodge methods, especially the on-site rapid remediation and emergency removal technology . Herein, the monolayer (ML) Ti 3 C 2 T x nanosheets (NSs) were prepared to remove Cr (VI) from water. The solution sample of the two-dimensional (2D) Ti 3 C 2 T x NSs demonstrate ultrafast adsorption kinetics (the concentration decreasing from 300 to 3 mg L −1 in 10 min) and impressively high capacity (1483 mg g −1 ), which is several times higher than that of the most reported Cr (VI) adsorption by Ti 3 C 2 T x . The analysis of the adsorption kinetics and isotherm models indicates that the adsorption reaction is endothermic, with physical and chemical adsorption coexisting (mainly monolayer chemical adsorption). The joint study of the experimental analysis and theoretical calculation based on the density functional theory (DFT) demonstrates that the extraordinary removal performance of Cr (VI) is due to the synergetic effect of reduction reaction removal and electrostatic adsorption. It is found that the Cr (VI) is mainly reduced by the OH- terminals on Ti 3 C 2 , and the detoxified Cr (III) is anchored on the surface of Ti 3 C 2 T x through complexation reaction with O terminal. The advantages of ultrafast adsorption kinetics and extra-high adsorption capacity of the single-layered Ti 3 C 2 T x for Cr (VI) removal make it a remarkable candidate for rapid and urgent removal of Cr (VI) wastewater.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2022
·
IF 4.644
Meng Tan,Qiaoyuan Gao,Yangjie Fu,Youran Xu,Derek Hao,Bing-Jie Ni,Qi Wang
In this study, a new coordination polymer of Fe-2-methylimidazole (Fe-2MI) was successfully loaded onto F-doped tin oxide (FTO) via a one-pot solvothermal method, using Fe(NO 3 ) 3 and 2MI as raw materials. For X-ray diffraction patterns (XRD) and scanning electron microscope (SEM) analysis, it can be deduced that Fe-2MI assembles were evenly dispersed on the surface of FTO, and were partially encapsulated by tiny FeOOH particles. The as-prepared Fe-2MI film electrode was used as photoanode with titanium sheet (Ti) as the cathode. Simultaneous photoelectrocatalytic (PEC) removal of phenol and Cr(VI) can be effortlessly accomplished under noticeable light illumination. Meanwhile, the impact of initial Fe state was also investigated. Fe-2MI prepared with Fe(III) behaved better PEC performance than that with Fe(II). Furthermore, the Fe-2MI photoanodes were optimized by adjusting the initial concentration of Fe(III) and 2MI precursors. Besides, the application conditions were optimized at acidic pHs and 2.5 V bias voltage . Cr(VI) can be completely reduced with 80% removal of phenol after 5 h PEC reaction. After 5 successive cyclic runs, stable photocatalytic performance can still be observed. Therefore, Fe-2MI coordination polymer can be a promising candidate for preparing visible-light-active photoanode in the application of environmental remediation.
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ENVIRONMENTAL TECHNOLOGY
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2022
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IF 3.475
Mingxing Chen,Qinming Guo,Jinping Cui,Weiyang Lv,Yuyuan Yao
Developing high-performance adsorbent for hexavalent chromium (Cr(VI)) elimination presents an enticing prospect in environmental remediation. Herein, three-dimensional flowerlike nanospheres composed of molybdenum disulphide and polypyrrole (MoS2@PPy) were successfully prepared via a one-pot hydrothermal and subsequent carbothermal reduction process for the removal of Cr(VI). The effects of pH, adsorbent dosage, co-existing ions, initial Cr(VI) concentration and temperature were investigated systematically by batch experiments. Benefiting from the incorporation of MoS2, the obtained MoS2@PPy composites showed a dramatic increase of specific surface area (149.82 m2·g−1) and adsorption capacity (230.97 mg·g−1) when compared with the pure PPy nanoparticles. Based on the thermodynamics study and X-ray photoelectron spectroscopy analyses, the removal process of Cr(VI) was proved to be exothermic and spontaneous, and accessible under-coordinated Mo(IV) and pyrrolic N groups coupled with redox reactions were conducive to the efficient removal of Cr(VI). Attractively, the MoS2@PPy acted as the electron donor could also activate peroxymonosulphate for the efficient degradation of organic contaminants. These results suggested that the MoS2@PPy was promising in Cr(VI) elimination and other kinds of organic pollutants removal in wastewater.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Yuhan Zhu,Jia Wei,Jun Li
Biochar is a well-known material for pollutant removal owing to its low cost and rich surface functionality. A kind of highly active substance, called environmentally persistent free radicals (EPFRs), can be produced in the preparation process of biochar, playing an important role in the removal of pollutants. In this study, sludge-derived biochars (SBC 120 and SBC 270 ) were prepared by the hydrothermal carbonization under two temperatures (120 °C and 270 °C) to investigate their removal abilities of Cr(VI). The maximum removal amounts of Cr(VI) by SBC 120 and SBC 270 were 16.58 and 22.93 mg·g −1 , respectively. It was further revealed that the appearance of Cr(III), as a result of EPFRs on sludge-derived biochar (SBC) transferred electrons to Cr(VI) in neutral solutions. That is to say, oxygen-centered (O-centered) EPFRs on SBC 120 and carbon-centered (C-centered) EPFRs on SBC 270 all could be used as electron donors to Cr(VI) to make it become Cr(III). This study not only provides a theoretical basis for the mechanism of pollutants removal by sludge-derived biochar but also offers a new perspective on the direct effect of EPFRs on pollutants.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Liming Zhao,Lijun Guo,Yuling Tang,Jianfei Zhou,Bi Shi
Research on the rational design of photocatalysts for efficient hexavalent chromium (Cr(VI)) reduction from Cr(VI)-containing wastewater has attracted widespread attention. In this paper, a novel g-C3N4/C/Fe2O3 photocatalyst was successfully synthesized by anchoring g-C3N4 nanosheets onto C/Fe2O3 that was prepared using collagen fiber as the biochar resource following the Fe tanning mechanism to reduce Cr(VI) under artificial solar irradiation. Under the same conditions, the as-prepared g-C3N4/C/Fe2O3 photocatalyst exhibited higher Cr(VI) reduction efficiency than g-C3N4, and the Cr(VI) reduction efficiency increased as Fe content in the g-C3N4/C/Fe2O3 photocatalyst increased. The enhanced photocatalytic performance was primarily ascribed to the formation of an indirect Z-scheme heterojunction between C/Fe2O3 and g-C3N4, which improved the separation efficiency of the photogenerated charge carrier. Furthermore, radical trapping indicated that photoinduced electrons (e–) were the main factor for Cr(VI) reduction. This work provides guidance for high value-added utilization of collagen fiber in constructing efficient light-driven photocatalysts and practical Cr(VI) removal from wastewater.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Yunfei Zhang,Qiang Zhao,Baoliang Chen
In materials science, “green” synthesis has gotten a lot of interest as a reliable, long-lasting, and ecofriendly way to make a variety of materials/nanomaterials, including metal/metal oxide nanomaterials . To accommodate various biological materials, green synthesis of metallic nanoparticles has been used (e.g., bacteria, fungi, algae, and plant extracts). In this work, Shewanella oneidensis MR-1 was used to biosynthesize palladium nanoparticles (bio Pd) under aerobic conditions for the Cr(VI) bio-reduction. The size and distribution of bio-Pd are controlled by adjusting the ratio of microbial biomass and palladium precursors. The high cell: Pd ratio has the smallest average particle size of 6.33 ± 1.69 nm. And it has the lowest electrocatalytic potential (−0.132 V) for the oxidation of formic acid , which is 0.158 V lower than commercial Pd/C (5%). Our results revealed that the small size and uniformly distributed extracellular bio-Pd could achieve completely catalytic reduction of 200 mg/L Cr(VI) solution within 10 min, while the commercial Pd/C (5%) need at least 45 min. The bio-Pd materials maintain a high reduction during five cycles. Microorganisms play an important role in the whole process, which can fully disperse palladium nanoparticles, completely reduce Cr(VI), and effectively adsorb Cr(III). This work expands our understanding and provides a reference for the design and development of efficient and green bio-Pd catalysts for environmental pollution control under simple and mild conditions.
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Polymers
·
2021
·Vol. 13
·期 20
·3498
·
IF 4.329
Shengqi Liu,Ye Meng,Hu Li,Song Yang
Considering economic and environmental impacts, catalytic biomass conversion to valuable compounds has attracted more and more attention. Of particular interest is furfural, a versatile biorefinery platform molecule used as a feedstock for the production of fuels and fine chemicals. In this study, the Cr-based metal-organic frameworks (MOFs) MIL-101 were modified by chlorosulfonic acid, and MIL-101 was changed into a hierarchical MOF structure with smaller particles and lower particle crystallinity by CTAB, which significantly improved the acidic sites of the MOFs. The original and modified MIL-101(Cr) catalysts were characterized by XRD, N2adsorption-desorption, SEM, TEM, and FT-IR. The effects of different catalysts, reaction temperature, catalyst amount, and alcohol type on the reaction were studied. Under the action of the MOFs catalyst, a new mild route for the condensation of furfural with various alkyl alcohols to the biofuel molecules (acetals) was proposed. The conversion route includes the conversion of furfural up to 91% yield of acetal could be obtained within 1 h solvent-free and in room-temperature reaction conditions. The sulfonic acid-functionalized MIL-101(Cr) is easy to recover and reuse, and can still maintain good catalytic activity after ten runs.Keywords:biomass conversion;MIL-101(Cr);furfural;green chemistry;heterogeneous catalysis
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JOURNAL OF SOLID STATE CHEMISTRY
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2021
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IF 3.498
Jun Jiang,Zhidong Chen,Peng Wang,Pei-Yang Gu,Jiadi Liu,Zhuzhu Zhang,Qingfeng Xu
At present, hexavalent chromium (Cr(VI)) has a serious impact on the water environment and human beings since it can be easily absorbed by the human body, lethal to aquatic organisms and carcinogenic to humans. Based on this, a black hollow TiO 2 nanotube supported polydopamine (PDA)@Ag 2 S composite photocatalytic material was prepared, which can be used for the efficient photocatalytic reduction of Cr(VI) in wastewater. Both black hollow TiO 2 and Ag 2 S have the shortcoming of undergoing ready recombination of photogenerated carriers. The introduction of PDA can not only improve the photogeneration of composite photocatalytic materials, but also broaden the absorption range in the visible-light region. A detailed mechanism for the TiO 2-x @PDA@Ag 2 S photocatalytic system has been proposed at the same time. This work provides a new methodology for the design and synthesis of sandwich organic-inorganic hybrid photocatalytic materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Dingliang Dai,Jianhao Qiu,Lu Zhang,Hong Ma,Jianfeng Yao
A subtle flower-like MIL-125-NH 2 @BiOI was fabricated by a facile solvothermal method for simultaneously eliminating Cr(VI)/tetracycline mixed pollutants under visible light . The strong interaction between amino in MIL-125-NH 2 and Bi 3+ of BiOI promotes the formation of this unique inlaid structure and enables the favorable contact between MIL-125-NH 2 and BiOI, thus accelerating the transfer of charge carriers. Remarkably, MIL-125-NH 2 @BiOI displays a superior activity compared with that of two monomers for the photocatalytic reduction of Cr(VI) and degradation of tetracycline . More significantly, the photocatalytic efficiency can be further boosted in the coexistence of Cr(VI) and tetracycline , which is 1.8 and 1.6 times that of single Cr(VI) and tetracycline, respectively. The synergistic effect between Cr(VI) reduction and tetracycline oxidative degradation can further facilitate the separation of photo-induced electrons and holes, resulting in the improved efficiencies in the Cr(VI)/tetracycline coexistent environment. This work sheds light on that MOF-based photocatalysts possess huge potential for practical environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Shanshan Mao,Tao Shen,Tong Han,Fan Ding,Qing Zhao,Manglai Gao
The functionalized organo-vermiculite (BDIEP-Vt) is prepared by combining the imidazole-ether-containing gemini surfactant into vermiculite, and serves as adsorbent for single and simultaneous removal of triclosan (TCS), p -chlorophenol (4-CP) as well as Cr(VI) from aqueous solution. The physicochemical properties of the resultant BDIEP-Vt are characterized via FT-IR, XRD, TG-DTG, SEM, TEM as well as BET analysises. In single system, the results of standard batch adsorption experiment represent that BDIEP-Vt could adsorb the three contaminants (220.4 mg/g for TCS, 74.6 mg/g for 4-CP, 18.4 mg/g for Cr(VI)) effectively as well as rapidly within 5–10 min. The adsorption process is in great pertinence with pseudo second-order model, and the equilibrium data are befitted Freundlich model greatly for TCS and Cr(VI), while Langmuir model suites for 4-CP. In TCS-Cr(VI)/4-CP-Cr(VI) binary system, the maximum adsorption capacity of BDIEP-Vt for TCS, 4-CP as well as Cr(VI) is 182.1, 44.1 and 12.7 mg/g, respectively. The trend variation of φ value indicates an antagonism effect is exerted by Cr(VI) ions on TCS/4-CP removal whereas Cr(VI) uptake is slightly affected. Interestingly, the impact sequence of Cr(VI) on the removal of TCS/4-CP follows as: TCS < 4-CP. The adsorption mechanism is clarified by means of the characterization of spent adsorbent together with theoretical calculations: (i) Expect for hydrophobic interaction, the adsorption of TCS/4-CP is mainly driven by π-π along with π-π stacking interactions; (ii) Both π-π (betwixt imidazole ring and orthogonally benzene) and π-π stacking interactions (among the orthogonally benzenes) are more stronger than imidazole-isolated benzene/isolated benzene-isolated benzene systems; (iii) The removal of Cr(VI) is controlled by electrostatic interaction. The study proves that BDIEP-Vt as an effective multifunctional adsorbent has a momentous application prospect in potential environmental remediation.
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RSC Advances
·
2021
·Vol. 11
·期 54
·33969-33979
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IF 3.361
Luxin Zhang,Yuting Liu,Ruijun Sun,Simin Yi
5-Ethoxymethylfurfural (EMF) has been identified as a potential biofuel and fuel additive, for which the production from glucose (the most abundant and inexpensive monosaccharide) in a one-step process would be highly desirable. Here, the synthesis of sulfonic acid-functionalized porous coordination polymers (PCPs) and their application as catalysts for EMF synthesis are reported. PCP(Cr)-BA (PCP material with Cr3+ ions and H2BDC-SO3H linkers) and PCP(Cr)-NA (PCP material with Cr3+ ions and H2NDC(SO3H)2 linkers) materials containing both Cr3+ sites and Brønsted-acidic –SO3H sites were prepared. The morphology, pore structure, acidity, chemical composition, and thermal stability of the two functionalized PCP(Cr) catalysts were analyzed by systematic characterization. The catalysts featured a porous morphology and dual Cr3+ and –SO3H sites, which enabled the cascade conversion of glucose to EMF. PCP(Cr)-BA exhibited higher performance than PCP(Cr)-NA with an EMF yield of 23.1% in the conversion of glucose at 140 °C after 22 h in an ethanol/water system. In addition, the as-prepared catalyst exhibited a high stability in the current catalytic system for EMF production from glucose with a constant catalytic activity in a four-run recycling test without an intermediate regeneration step.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Longwen Li,Lin Chi,Hongxu Zhang,Shuming Wu,Han Wang,Zhimin Luo,Yanwei Li,Yanhui Li
This article prepared a nanoparticle (NP) Ti-PDA made from bis (2-hydroxy propionic acid) diammonium titanium hydroxide (Ti-BALDH) chelating dopamine (DA), as a photocatalyst to absorb and reduce hexavalent chromium (Cr(VI)) under visible light with recycling ability from waste water. Ti-PDA NPs with part of TiO 2 -like structure can perform some function of TiO 2 , while participation of PDA will not only broaden absorption spectrum from UV to visible light, but offer the ability to absorb Cr(VI). Compared with TiO 2 Ti-PDA NPs would make full use of sunlight, increasing the photocatalytic efficiency. The adsorption results of Ti-PDA NPs for Cr(VI) showed that the adsorption capacity of Ti-PDA NPs can reach 500.24 mg/g when the concentration of Cr(VI) was 300 mg/L, and the adsorption data matched well with the Langmuir isotherm model, and confirmed to a quasi-second-order dynamics. Under visible light irradiation, Ti-PDA NPs could reduce Cr(VI) to Cr(III) within 30 min, and can almost completely reduce Cr(VI) within 15 min even at pH = 4. After three cycles, photocatalytic reduction efficiency was still 95.02%. Thereby the toxic Cr(VI) can be effectively eliminated by Ti-PDA NPs from sewage. As a result, Ti-PDA will be a promising green photocatalyst to remove Cr(VI) in disposal of water pollution.
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