LANGMUIR
·
2023
·
IF 3.9
Wenjing Zhu,Zhinan Xia,Bingfeng Shi,Changli Lü
A series of 2D M(Cu, Zn, Co, and Mn)-TCPP MOFs/TiO2 binary nanocomposites (TCPP = tetrakis(4-carboxyphenyl)porphyrin) were constructed by solvothermal in situ loading of flaky TiO2 on the surface of 2D metal–organic frameworks (MOFs). The influence of different coordination metals on the catalytic activity was studied, and it was found that the 2D Cu-TCPP MOFs/TiO2 nanocomposite exhibited the best photo-Fenton performance. The superior property can be attributed to the high absorption coefficient and ultrathin two-dimensional structure of the 2D Cu-TCPP MOFs nanosheets. Meanwhile, the 2D Cu-TCPP MOFs/TiO2 II heterostructure can effectively promote the separation and transfer of photoformed carriers. Moreover, under visible irradiation, the optimized 2D Cu-TCPP MOFs/TiO2 composite can convert 99.9% of Cr(VI) to Cr(III) within 60 min with methanol as the hole scavenger at pH 3.14. Also, the photocatalytic performance of 2D Cu-TCPP MOFs/TiO2 was maintained after five reaction cycles. Furthermore, the proposed visible-light-driven photocatalysis mechanism of the 2D Cu-MOFs/TiO2 composite was reasonably derived according to experimental results. This study demonstrates the potential of building efficient TiO2-based visible light photocatalysts with 2D metal-porphyrin MOFs.
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PubMed
高影响因子
ACS ES&T Engineering
·
2023
·
IF 7.1
Huan Tang,Shimao Deng,Zheting Chu,Yangzi Shangguan,Jiaxin Liang,Qian Zheng,Ranhao Wang,Hong Chen
Simultaneously reducing and immobilizing Cr(VI) anions in groundwater are crucial to minimize their hazardous effects. Herein, benefiting from the feasible chemical-/photo-reduction capability of greigite, together with the ion-exchange functionality of zeolites, the integrated three-in-one function in greigite/Re-ANA composites (GRAs) material has been employed for removing and immobilizing Cr(VI) in groundwater remediation. GRA-3 achieved a 99.4% Cr(VI) removal efficiency in a Cr(VI) solution with 1 mg/L. Cr(VI) residue concentration is 0.006 mg/L, complying with the control guideline in drinking water according to WHO regulations. A comprehensive mechanism study reveals that the chemical reduction and photoreduction processes are involved within greigite, which drives the process of reducing Cr(VI) to Cr(III). Subsequently, the as-reduced Cr(III) is either adsorbed on a greigite surface or ion-exchanged with zeolite microporous channels, thus getting immobilized. Furthermore, environmentally relevant Cr(VI) contaminated groundwater sampling from the chromate plant has been employed for the fixed-bed column study, which achieved the discharge standard for practical Cr(VI) polluted groundwater. This work reported a composite material matrix with great potential and significance for Cr(VI) remediation, which could be employed in permeable reactive barriers for Cr(VI)-polluted groundwater remediation in the future.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Guangping Lei,Yang Lu,Zihan Liu,Yayun Zhang,Guojun Xi,Huiyuan Cheng,Wenji Rao,Xuhuan Guo
The greenhouse effect associated with excessive CO 2 emission has led to a series of environmental issues, thus developing excellent adsorbents for CO 2 capture from flue gas offers a sustainable approach. To combine the merit of multiple functional components, novel FeTPP@MIL-101(Cr) was prepared by incorporation of 5,10,15,20-tetrakis(4-methylphenyl)porphyrinato iron (III) chloride (FeTPP) into MIL-101(Cr) cages via in-situ packaging strategy. The cage-confined FeTPP can both regulate the pore structures of MIL-101(Cr) and provide additional binding sites for CO 2 adsorption. Profiting from extra interactions for CO 2 component and the “sieving effect” for N 2 component induced by incorporation of FeTPP, the discrepancy of isosteric heat for CO 2 and N 2 was largely amplified. Notably, the CO 2 /N 2 selectivity (15/85, v / v ) calculated by ideal adsorbed solution theory (IAST) increased from 17.1 (MIL-101 (Cr)) to 41.8 (FeTPP@MIL-101 (Cr) with FeTPP loading of 4.98 wt%) at 273 K, 100 kPa, which is 2.44 times larger than that of pristine MIL-101 (Cr) and also exceeds most reported adsorbents.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 29
·15760-15768
·
IF 11.9
Chunyan Xiong,Shan Xu,Xiantao Li,Tong Liu,Yuan Tan,Pei Zhao,Peng Qiu
The sluggish oxygen reduction reaction (ORR) kinetics and the fast performance degradation caused by Cr-poisoning greatly hinder the commercialisation of an LaxSr1–xCoyFe1–yO3–θ (LSCF) cathode in solid oxide fuel cells (SOFCs). Herein, a surface regulating and hetero-interface engineering method by chemical vapour deposition (CVD) was applied to construct a CeO2-coated LSCF cathode with enhanced ORR activity and durability. By controlling the CVD operating time, and the thickness of the CeO2 coating, the CeO2/LSCF heterointerface could be precisely engineered. With the optimal CVD time of 7 min, the x-LSCF cathode exhibited a minimal polarisation resistance (Rp) value of 0.11 Ω cm2 at 750 °C, which is almost one-fifth of that of an LSCF cathode (0.46 Ω cm2). Moreover, the CeO2-coated LSCF cathode exhibited a much lower degradation rate than the LSCF cathode in the long-term Cr-poisoning test. The improved ORR catalytic activity and durability of the CeO2-coated LSCF cathode were also verified in the single-cell mode. This study provides a comprehensive and novel strategy for tailoring the surface of the SOFC cathode for achieving enhanced performance and Cr-tolerance.
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Biochar
·
2023
·Vol. 5
·期 1
·1-20
·
IF 12.7
Yang Bowen,Dai Jiawei,Zhao Yuan,Wang Zhanchao,Wu Jingwei,Ji Caiya,Zhang Yuhu,Pu Xiao
Biochar-coupled Fe 3 O 4 @SiO 2 /TiO 2 /g-C 3 N 4 composites were successfully constructed through simple sol–gel and calcination methods. The composites efficiently removed high-concentration toxic tetracycline (TC) by means of ·OH and · \({\rm O}_2^{-}\) , whose removal rate exhibited 91.88% during 3 h, and the degradation rate constant reached up to 0.0068 min −1 . The excellent performance can be attributed to the high specific surface area, enhanced visible light response, the introduction of magnetic nanoparticles and biochars expediting charge transfer, Z-scheme heterojunction enhancing the spatial separation of photo-generate carriers and, importantly extraordinary adsorption capacity of 147.96 mg g −1 . Moreover, the composites showed the most excellent efficiency under the calcination temperature of 450 ℃, and exhibited good stability with tolerance to a wide range of pH and anions. Interestingly, a synergistic photocatalytic effect was discovered in the TC/Cr(VI) combined pollution systems, resulting in significantly improved removal of Cr(VI). Besides, the photocatalytic mechanism and degradation path of tetracycline were also elucidated. All these findings suggested the as-synthesized catalyst was an excellent photocatalyst for removal of TC/Cr(VI)-contaminated water. Graphical Abstract
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Sandip Mondal,Jianqiao Xu,Guosheng Chen,Siming Huang,Chuyu Huang,Li Yin,Gangfeng Ouyang
Antibiotics are a group of antibacterial drugs used in the treatment and prevention of bacterial diseases in humans, veterinary animals, and farmed fish. Inappropriate and excessive use of antibiotic therapy leads to antibiotic fragment in the water bodies thus affect the aquatic organisms . In this study, an amino group modified high surface area metal-organic framework (MOF) MIL-101(Cr)-NH 2 was used to prepare solid-phase microextraction (SPME) fiber to detect four different classes (total 6 ABs) of antibiotics for the first time from living tilapia fish ( Oreochromis mossambicus) by coupling SPME with high performance liquid chromatography-tandem mass spectrometry (LC-MS/MS). The extraction efficiencies of the custom-made fiber were superior as compared with the commercial C18, polydimethylsiloxane (PDMS), PDMS/divinylbenzene (DVB) and polyacrylate fibers. The custom-made fiber also exhibited excellent reproducibility with the low intra-fiber relative standard deviations (RSDs 1.5%–8.3%) and inter-fiber RSDs (7.3%–14.5%), which made it ideal for in vivo extraction in fish muscle. The as-prepared MIL-101(Cr)-NH 2 fiber was then used to determine antibiotics in the dorsal-epaxial muscle of living fish. Comparing to the traditional solid-liquid extraction (SLE) method, the SPME method showed reduced invasiveness and higher sensitivity than the SLE method. In general, this study explored a convenient, cost-effective and highly sensitive SPME method based on amino modified MOF for in vivo antibiotic detection in fish muscle.
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PubMed
高影响因子
Environmental Science-Nano
·
2018
·Vol. 5
·期 11
·2570-2578
·
IF 6.087
Xinwen Ou,Xueming Liu,Weizhen Liu,Wencong Rong,Jingyuan Li,Zhang Lin
The surface defects of adsorbents are generally considered to be the active sites for adsorbates, and the adsorption behaviors of a variety of pollutants in wastewater are strongly influenced by the surface defects of the adsorbents. With simple chemical and structural properties, nano-Mg(OH)2 exhibits a high adsorption affinity and selectivity to heavy metals from wastewater. The insight into the surface complex structures of heavy metals on the Mg(OH)2 surface is fundamental for both the mechanism and application of defective adsorbents in wastewater treatment. In this study, the impact of surface defects of Mg(OH)2 nanoplates on the structure, energy, and adsorption amounts of toxic heavy metal oxyanions (HAsO42− and CrO42−) was investigated by combining the first-principles calculations and batch experiments. The first-principles calculations illustrated that the heavy metal oxyanions can be steadily incorporated into the surface defects to form inner-sphere complexes. The incorporated heavy metal oxyanions have strong charge–charge and chemical bonding interactions with the surface defect sites, which are much stronger than the hydrogen bonding interactions with the surface OH sites. Moreover, the adsorption affinity of surface defects towards heavy metal oxyanions is stronger than that towards other oxyanions (e.g. SO42− and NO3−), indicating the high adsorption selectivity of heavy metal oxyanions over other oxyanions. Batch adsorption experiments verified that the adsorption of defect-rich Mg(OH)2 adsorbents towards heavy metal ions, e.g., As(V) and Cr(VI), was favorable even under the condition of low concentration (mg L−1 level). These findings reveal the significance of surface defects of Mg(OH)2 for extracting As(V) and Cr(VI) from low-concentration solutions. The proposed strategy of surface defect-fabrication should provide a useful insight into designing effective adsorbents for the selective extraction of heavy metal oxyanions at low concentration.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Haoran Tian,Qingyu Wu,Qiuju Wu,Chengyou Sun,Ruimei Zhang,Jie Wei,Haiyin Xu,Zhiming Liu,Chao Huang,Ping Wang
Nano zero-valent iron (nZVI) has been widely employed for the elimination of heavy metals from wastewater. However, the practical application of nZVI is greatly limited due to its fast aggregation and surface passivation. In this study, a carbon nanotube-supported nZVI composite (nZVI@CNTs) was synthesized and coupled with Shewanella oneidensis MR-1 to enhance the removal of Cr(VI) from aqueous media. The results demonstrated that the coupling of nZVI@CNTs and MR-1 (nZVI@CNTs/MR-1) exhibited superior performance in eliminating Cr(VI) compared to using nZVI@CNTs or MR-1 alone. Electrochemical characterization demonstrated that CNTs acting as electron shuttles improve the electron transfer from MR-1 to nZVI, thus facilitating the passivation layer dissolution. XRD analysis proved that MR-1 can effectively promote the dissolution of the Fe(III) passivation layer with the existence of CNTs. FTIR and XPS analyses confirmed that CNTs contain many functional groups (such as C − C and C = O) related to extracellular electron transfer, thus promoting the electron transfer of MR-1 to nZVI. Three-dimensional excitation-emission matrix (3D-EEM) analysis showed that the extracellular polymeric substances (EPS) generated from MR-1 participated in the Cr(VI) elimination. The mechanism analysis demonstrated the Fe(II) dissolved from the nZVI passivation layer reduces Cr(VI) to Cr(III) and then removes it by co-precipitation, and the EPS secreted by MR-1 also participates in the Cr(VI) adsorption and reduction. Generally, the coupling of nZVI@CNTs and MR-1 successfully addresses the drawbacks of nZVI and demonstrates a remarkable ability to remove Cr(VI).
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Runming Wang,Gang Cheng,Zan Dai,Jie Ding,Yunling Liu,Rong Chen
A general ionic-assisted microwave-ultrasonic combined synthetic strategy was developed to fabricate Bi 2 E 3 (E = S, Se, and Te) hierarchitectures. To understand the crystal phase transformation and morphological evolution of Bi 2 S 3 hierarchical nanostructures, the fabrication of Bi 2 S 3 hierarchitectures was investigated by varying sulfidation time and chlorination time. A topotactic transformation from BiOCl microsphere to Bi 2 S 3 hierarchitectures was proposed. It was found that the structure, size, and morphology of Bi 2 S 3 hierarchitectures could be delicately engineered by varying chlorination time, alkyl chain length, and concentration of ionic liquid. Moreover, the as-prepared Bi 2 S 3 hierarchitectures displayed superior capacity of Cr(VI) photoreduction to P25 and irregular Bi 2 S 3 nanostructures under visible light irradiation. Effects of morphology, pH value of reaction system, Cr(VI) concentration, and catalyst dosage on the Cr(VI) photoreduction capacity of Bi 2 S 3 hierarchitectures were also discussed. The enhancement of photoreduction capacity is not only attributed to the intrinsic good electron transfer ability of Bi 2 S 3 , but also to synergetic effects of special architectures, wide photoresponse range, high light photoadsorption, high BET surface area and good electron-hole separation performance. The systematic condition experiments and Cr(VI) photoreduction in electroplating and tannery wastewater experiments further demonstrated that the hierarchical Bi 2 S 3 nanospheres can be used in the actual Cr(VI)-containing wastewater treatment.
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Journal of Materials Chemistry A
·
2013
·Vol. 2
·期 8
·2599-2608
·
IF 0
Xingqi Wang,Wenxia Liu,Jian Tian,Zhenhuan Zhao,Pin Hao,Xueliang Kang,Yuanhua Sang,Hong Liu
Uniform well-defined nanostructured BiOBr microspheres have been fabricated via a simple hydrothermal method in the presence of cetyltrimethylammonium bromide (CTAB) and ethylene glycol (EG). The heavy metal ion adsorption on the as-synthesized nanostructured BiOBr microspheres was systematically assessed by measuring the residual concentration during the adsorption process using a colorimetric method for Cr(VI) concentration, and an extraction-colorimetric method for Cd(II) and Pb(II) concentrations. The nanostructured BiOBr microspheres showed good removal capacity for heavy metal ions (Cr, Cd, Pb), and excellent adsorption properties for low concentration heavy metal ions, indicating potential applications in water purification. Based on the quick and efficient heavy metal ion removal ability of nanostructured BiOBr microspheres, a continuous filtering-type water purification device was designed and constructed. In using this continuous filtering type water purification device, 1 g of adsorbent can purify about 4900 g of Pb(II) contaminated water, 5900 g of Cd(II) contaminated water, or 21 500 g of Cr(VI) contaminated water having initial concentrations of 200 μg L−1 to successfully attain the World Health Organization standard for drinking water. The good removal capacity can be attributed to the hierarchical nanostructure, which displays a large specific surface area and strong adsorption of heavy metal ions.
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Nano Research
·
2017
·Vol. 10
·期 10
·3543-3556
·
IF 7.354
Pi Yunhong,Li Xiyi,Xia Qibin,Wu Junliang,Li Zhong,Li Yingwei,Xiao Jing
Efficient separation and transfer of photogenerated electron/hole as well as enhanced visible light absorption play essential roles in photocatalytic reactions. To promote the photocatalytic reduction of Cr(VI), a toxic heavy metal ion, multiwalled carbon nanotube (MWCNT) was introduced as an electron acceptor into NH 2 -MIL-68(In). This led to the growth of a willow leaf-like metal-organic framework (MOF) on an MWCNT backbone forming MWCNT/NH 2 -MIL-68(In) (PL-1), which showed a highly efficient transfer of photogenerated carriers. Moreover, MWCNT incorporation introduced more mesopores for Cr(VI) diffusion and enhanced the visible light adsorption without lowering the conduction band position. As a result, the photocatalytic kinetic constant of PL-1 was found to be almost three times higher than that of the parent NH 2 -MIL-68(In). Thus, growing MOFs on MWCNTs provides a facile and promising solution for effective remediation of environmental pollution by utilizing solar energy. This work provides the first example of using MWCNT/MOF composites for photocatalytic reactions.
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Tungsten
·
2024
·
IF 5.6
Lan Qing,Jin Su-Juan,Liu Ying,Jin Xiao-Li,Xie Hai-Quan,Li Yu-Zhu,Liu Ke-Cheng,Chen Li
With environmental issues gaining increasing attention, the demand for developing economical and reusable catalysts has become increasingly critical. Although precious metal catalysts are effective in photocatalytic pollutant decomposition and Cr(VI) reduction, their high price, instability, and recovery difficulty constrain their application. This study introduces an approach where Ag + ions are exchanged with cations in polyoxometalate (POM) via a mild grinding method, followed by in situ illumination under ultraviolet light to produce Ag/Ag-POM composite nanomaterials. Upon interaction with POM clusters, Ag + ions are reduced to Ag nanoparticles, which enhances visible light absorption in the composite, thereby improving its photocatalytic efficiency. Ag/Ag-POM nanomaterials obtained from this process exhibit efficient and stable catalytic performance, efficiently degrading tetracycline (TC) and reducing hexavalent chromium (Cr(VI)) under visible light (λ > 420 nm). Especially, the Ag/AgHPMo 11 V composite demonstrated superior catalytic performance, achieving degradation efficiencies of 99.9% for 40 mg·L −1 TC. Moreover, it also exhibited efficient photoreduction of Cr(VI), achieving a reduction rate of 62.81% for 80 mg·L −1 Cr(VI) in a 100 mL solution using just 10 mg of the catalyst within 40 min of visible-light exposure. This research highlights the potential of polyoxometalate-based catalysts in the photocatalytic treatment of pollutants.
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