Journal of Environmental Chemical Engineering
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2021
·
IF 5.909
Kaihua Su,Dongmin Zhao,Ai Lu,Chaoran Zhong,Xing-Can Shen,Changping Ruan
Hexavalent chromium Cr(VI) is one of the most toxic heavy metal pollutants in water due to its high water solubility, high toxicity, strong mutagenicity and carcinogenicity . To enable efficient Cr(VI) removal from wastewater, it remains difficult to fabricate advanced adsorbents with good selectivity and high adsorption capacity in large scale. Herein, a poly(hexamethylenediamine-tannic acid)-bacterial cellulose (denoted as HTA-BC) composite was prepared by using natural raw materials with abundance, low cost and nontoxicity in a facile one-step method and applied for the decontamination of highly toxic Cr(VI). The as-synthesized HTA-BC functionalized with abundant amino and phenolic hydroxyl groups had demonstrated high capacity (534.8 mg g −1 ) and good selectivity for Cr(VI) scavenging. Notably, the treatment of real water samples with the HTA-BC composite could efficiently reduce the concentration of the spiked Cr(VI) below the acceptable levels for drinking water . Moreover, high-purity Cr 2 O 3 was obtained by calcination of the Cr species-laden HTA-BC to ensure that the toxic Cr(VI) residing in the spent adsorbents can’t leak out into the surroundings, thus avoiding the secondary pollution. The natural abundance, low cost, easy availability, and sustainability of the raw materials, combined with the facile and green synthesis endowed the HTA-BC composite with great potential for not only decontaminating Cr(VI) wastewater, but also recycling Cr by calcination of the Cr-laden HTA-BC. Moreover, no secondary pollution would be brought during the synthesis and the post-treatment after the Cr(VI) removal, thus it is expected to be a green and sustainable approach for the purification of Cr(VI) containing wastewater.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 11
·3670-3684
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IF 6.177
Chunwang Lv,Mingjiang Hu,Tianhao Yuan,Liqiang Yan,Hongwei Chen
The objective of this work was to investigate and contrast the mechanism of different B-site dopants for catalytic activity and sulfur resistance under equivalent conditions. LaCo1−xMxO3 (M = Fe, Cr, Cu) perovskite-type catalysts were synthesized by a sol–gel method, and the optimized samples were tested for toluene oxidation before and after sulfur aging. The properties of the catalysts were investigated in detail by XRD, FT-IR, N2 adsorption–desorption, H2-TPR, XPS and in situ DRIFTS to elucidate the inner mechanisms of the catalytic reaction and poisoning processes. The results indicated that introducing specific metal cations with a suitable ratio into the B-site of perovskite could improve the catalytic activity and weaken the negative effect of SO2 poisoning. The reasons for the improvement of catalytic activity on different doped catalysts are similar and mainly lie in the change of reduction property, oxidation state of the B-site, and content of oxygen vacancies. However, the mechanism of sulfur resistance caused by different dopants is not identical. The introduction of different metal cations will cause certain differences in some factors such as reducibility, lattice stability, sulfur adsorption and sulfate content, thus leading to the differentiation of sulfur tolerance for doped perovskite catalysts. In this study, the optimization effect of Fe dopant is better than that of Cr and Cu dopants, illustrating that the high stability of the perovskite lattice and the insensitivity to sulfur species are the key factors for its outstanding sulfur resistance. The results provide insights into guiding the practical composition and life cycle optimization of perovskite-type catalysts in the industrial application of removing sulfur-containing VOCs.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 18
·6394-6403
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IF 4.099
Yanqin Li,Qi Gao,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Ying Ying,Mingcai Zhang,Chunqian Huang,Yong'an Wang
Currently extensive effort is compulsively expended to decontaminate efficiently banned chemical war agents. In this work, H5PV2Mo10O40 molecules have been encapsulated in mesoporous MIL-101(Cr), which features two types of mesoporous cages (internal diameters of 29 Å and 34 Å) and microporous windows (diameters of 12 Å and 16 Å), leading to the formation of a new composite H5PV2Mo10O40@MIL-101(Cr) through a simple impregnation method. The composite was characterized thoroughly by elemental analysis, FT-IR spectroscopy, powder X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy, TG/DTA, and textural analysis thereby confirming the encapsulation of the H5PV2Mo10O40 into MIL-101(Cr). The decontamination efficiency of sulfur mustard (4 μL HD in 40 μL of petroleum ether) by 20 mg of the composite is found to be 97.39% in 120 min under ambient conditions. GC-MS analysis on the decontaminated products using 2-chloroethyl ethyl sulfide (CEES), which has been widely used as a simulant of sulfur mustard, showed that MIL-101(Cr) just decontaminates CEES by adsorption, while CEES can be decontaminated under ambient conditions by a synergetic combination of adsorption of MIL-101(Cr) and subsequent chemical oxidation degradation to nontoxic 2-chloroethyl ethyl sulfoxide (CEESO) due to the presence of highly dispersed H5PV2Mo10O40 within the composites.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhiliang Chen,Yaoyu Luo,Chuixiu Huang,Xiantao Shen
Designing a novel type of imprinted photocatalysts for selective photoreduction of highly toxic pollutants is extremely needed in semiconductor photocatalysis. In this work, imprinted photocatalysts (named ZnO/GO-MIPs) were synthesized via Pickering emulsion polymerization by in situ assembling ZnO/GO composites on the synthetic molecular receptors (MIPs). The experimental data showed that the ZnO/GO-MIPs owned specific affinity towards the target Cr(VI) in aqueous solution with an imprinting factor ( IF ) of 1.6. Under the illumination of visible light, the ZnO/GO composites could selectively photoreduce the Cr(VI) adsorbed by the MIPs. In comparison with the ZnO/GO catalysts under light illumination, the ZnO/GO-MIPs showed a 15 fold increase in photoreduction of Cr(VI). Mechanism study indicates the photoreduction of Cr(VI) by the ZnO/GO composites was occurred at the interface between the solid MIP core and the aqueous solution. Compared to the ZnO-MIPs and the GO-MIPs, the ZnO/GO-MIPs clearly showed interfacial synergistic catalysis effect. To the best of our knowledge, this is first time that selective photoreduction of highly toxic pollutants at the solid-water interface by the ZnO/GO-MIPs was achieved. We believe the ZnO/GO-MIP catalysts have great potential in interfacial synergistic catalysis in environment and catalysis fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Hiba Shaghaleh,Yousef Alhaj Hamoud,Qin Sun,Mohamed S. Sheteiwy,Hamada AbdElgawad
Soil flushing and adsorption-based soil remediation are promising options for removing heavy metals in agricultural soil. However, they encounter limitations in low removal efficiency, secondary pollution potential, or the need for a purification/recovery process. Optimizing flushing solutions or the functional properties of adsorbents could fundamentally eliminate the drawbacks of these methods. Yet, their practical application remains a formidable challenge. Herein, a new combined remediation strategy of multiple-pulse water soil flushing (MF) with novel aminated cellulose nanofibers (A-NFCs)/AEM/AM@MIL-100(Fe) nanocomposite hydrogel adsorbent (ANCMH) was adopted to remove Cr(VI) from agricultural soil. The characteristic analyses approved Cr(VI) adsorption-coupled reduction/swelling-based mechanisms on ANCMH with the maximum theoretical adsorption capacity of 338.24 mg g −1 at pH 6.8 governed by pseudo-second-order and Freundlich models. Instead of conventional MF application using environmentally problematic extractant fluids, a 5-day soil column simulation trial of MF coupled with ANCMH adsorbent layers (MF@ANCMH) was applied in medium-to-highly Cr(VI)-contaminated soil followed by easy ANCMHs separation, preventing secondary pollution. Innovatively, the water flushing-stop flux events favorably decreased the pH of neutral soil by 0.83 folds and allowed Cr(VI) release from the soil matrix to be adsorbed by ANCMHs, achieving a high Cr(VI) removal efficiency of 98.9 %. Compared to the soil treated with ANCMH individually and soil flushed with water or Na 2 EDTA, the MF@ANCMH-treated soil reached the corresponding regulation of permissible levels for Cr(VI) residential scenarios in agricultural soil of 5.6 ppm with 3-cycles of ANCMH reuse. The residual Cr in MF@ANCMH-remediated soil displayed minimal bioavailability at root-zoon soil of ≤4.2 ppm and a 97.66 % reduction in its exchangeable-carbonate fraction compared to untreated soil, corresponding to a risk assessment code score below 1 %. Also, the application of MF@ANCMH resulted in Cr bioaccumulation below 0.1 ppm in cultivated wheat plants, prevented the physiological phytotoxicity symptoms, and elevated their antioxidant enzyme activity, photosynthesis, growth, and yielding indicators compared to that grown in untreated soil. Furthermore, it improved soil organic matter, microbial community, diversity, and microecological functions. This study provides a promising alternative remediation strategy for neutral soil that can maintain soil/crop quality and soil health with high chemical/environmental stability of pollutants after remediation, demonstrating its sustainability and feasibility in agricultural soil.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
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IF 6.3
Xin Tang,Ruipeng Mao,Fan Zhang,Yongzhong Jin,Wei Su,Wu Jiang,Junhao Wang
Cemented carbides play a pivotal role in diverse industrial sectors, and controlling abnormal grain growth and regulating the homogeneity of the Co binder phase are the key challenges to improve their properties. In this study, WC-10Co alloy was prepared for the first time by low-pressure sintering technique using (Ti, Cr, V, Nb, Mo)(C, N) high entropy powder as an inhibitor, focusing on the effect of trace additions of (Ti, Cr, V, Nb, Mo)(C, N) on the microstructure and mechanical properties of the alloy as well as friction and wear properties. The results show that under the conditions of sintering at 1420 ℃, a pressure of 3 MPa, and a holding time of 1 hour, the alloy with 0.2 wt.% high-entropy inhibitor exhibited the best comprehensive properties, with a flexural strength of 3752 MPa, a Vickers hardness of 1679 HV 30 , and a fracture toughness of 13.07 MPa·m 1/2 . During the stable stage of tribological testing, the average friction coefficient reached 0.6195, and the wear rate was as low as 1.34×10 -7 mm 3 /(N·m). The toughening and strengthening mechanism of the (Ti, Cr, V, Nb, Mo)(C, N) - modified alloy is mainly attributed to the significant refinement of WC grains, WC lattice contraction, and the formation of Co-based solid solutions by the high-entropy inhibitor. However, excessive addition deteriorates the overall performance. This study provides experimental data and technical insights for the development of a new generation of cemented carbides with high strength, high toughness, and excellent wear resistance.
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Scientific Reports
·
2025
·Vol. 15
·期 1
·1-16
·
IF 3.9
Zhang Fengrong,Liu Luxing,Zhang Cuilan,Shang Dawei,Wu Lishun
A novel adsorbent ZnAl–LDHs/SiO 2 (ZA/SiO 2 ) was prepared by blending urea mixture of ZnSO 4 and Al 2 (SO 4 ) 3 while using SiO 2 as a support form. The adsorption properties of ZA/SiO 2 for the removal of toxic metal ions (Cu(II) and Cr(VI)) from water were evaluated. By batch experiment method to investigate the ZA/SiO 2 adsorption of Cu(II) and Cr(VI) solution treatment effect. The sorption kinetics curves of Cu(II) and Cr(VI) on ZA/SiO 2 were L-shaped. What’s more, the solid concentration effect was found in the process of sorption kinetics. Langmuir and Freundlich sorption isotherm models were used to analyze the adsorption data. The results showed that the adsorption conforms to Langmuir and Freundlich adsorption isotherm models. However, the adsorption capacity of ZA/SiO 2 compounds for Cu(II) and Cr(VI) is greatly improved. The adsorption capacity of Cu(II) is 158 mg·g −1 and of Cr(VI) is 176 mg·g −1 , which were 3.6 and 1.8 times of ZnAl-LDHs (ZA), respectively. Density functional theory (DFT) was utilized for the analysis of intrinsic mechanism and specific pathways. The primary mechanism for removing Cr(VI) from water mainly included the intercalation of Cr 2 O 7 2− and exchange between Cr 2 O 7 2− and OH − , excluding Cr(OH) 3 precipitation. Regarding the primary mechanism for eliminating Cu(II) from water, it involves isomorphic substitution as the predominant process, except for the formation of Cu(OH) 2 precipitates.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Shihui Wang,Yuzhou Xia,Guiyang Yan,Meixia Chen,Xuxu Wang,Ling Wu,Ruowen Liang
Inspired by the concept of frustrated Lewis pairs (FLPs) from homogeneous catalysis, an organic supramolecular bridged metal-organic frameworks (MOFs) heterojunction, i.e., a perylene-3,4,9,10-tetracarboxylic diimide@MIL-125(Ti)-NH 2 (denoted PDI@MTi) composite is successfully fabricated via a two-step synthesis method. Experimental characterisations and theoretical calculations reveal that in the obtained “TiO 5−x -ligand-PDI” FLPs, the unsaturated Ti-O clusters function as a Lewis acid to accept photogenerated electrons, and the PDI sites act as a Lewis base to capture photogenerated holes. With the unique structure characteristics, the PDI@MTi shows excellent photocatalytic activity toward the disinfection of Staphylococcus aureus and Cr(VI) reduction, with 1.0- and 10.3-fold enhancements, respectively, compared with unadorned MTi. The synergic effects of the micro polarisation field, multiple active sites, and a C-N bonded interface contributed to photoactivity enhancement. This work demonstrates the potential of using MTi as a platform for constructing FLPs-containing heterogeneous photocatalysts and provides new strategies to control carrier separation.
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JOURNAL OF SOLID STATE CHEMISTRY
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2021
·
IF 3.498
Meimei Zhou,Wei Zou,Xuemei Zhu,Huachen Ma,Pengbo Wang,Jiaxin Shang,Pingping Luo
UIO-66-NH 2 was successfully deposited on electrospun polyacrylonitrile (PAN) nanofibers treated by thermal oxidative stabilization (TOS) via a simple and effective in situ growth method. Owing to the formation of acridone rings, naphthyridinering rings and hydronaphthyridine rings during the TOS process, the thermally stabilized electrospun PAN (TSPAN) nanofibers were greatly improved in stability and heat resistance and could provide adequate nucleation points for MOFs growth, indicating an ideal MOFs deposition support without additional surface modifications. The results demonstrated that UIO-66-NH 2 crystals distributed relatively uniform and dense on the TSPAN nanofibers with mass loading up to 28.1 wt%. Compared with powdered UIO-66-NH 2 , the formed UIO-66-NH 2 @TSPAN nanofibers showed enhanced visible light driven photocatalytic activity towards reduction of Cr(VI) due to the improvement of visible light response, more excellent photothermal conversion ability and the increase of exposed active sites. The photocatalytic reduction rate of Cr(VI) over UIO-66-NH 2 @TSPAN was up to 93% within 180 min and the rate constant (k = 0.1362) was 2.3 times that of powdered UIO-66-NH 2 (k = 0.00576). Significantly, the mechanical flexibility and structural stability endowed the nanofibrous photocatalyst easy operation and outstanding reusable capability. The photocatalytic activity for Cr(VI) reduction still preserved 90% after five cycles. This work proposes a facile strategy for preparation of free-standing MOFs nanofibers and provides MOFs-based photocatalysts a new opportunitie for broad applications in water treatment.
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高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 6
Fucheng Liu,Yuhui Chen,Lei Zhuang,Hui Wang,Hulei Yu,Yanhui Chu
High-temperature materials with superior long-term oxidation resistance above 2000 °C are urgently sought for next-generation hypersonic vehicles. Here, (W 0.28 Ta 0.28 Mo 0.28 Cr 0.15 )(Al 0.2 Si 0.8 ) 2 -Al 2 O 3 dual-phase high-entropy alumino-silicides (HEAS-Al 2 O 3 ) are developed, which exhibit superior long-term oxidation resistance up to 2100 °C. To be specific, the as-fabricated HEAS-Al 2 O 3 samples are found to consistently follow an oxygen-diffusion parabolic law across 1700–2100 °C, possessing a high activation energy of 234.4 kJ mol −1 . Moreover, an ultralow oxidation depth of 0.4 mm after 120 min of laser oxidation and a linear plasma ablation rate of 0.026 μm s −1 at 2100 °C are achieved. Such remarkable oxidation resistance is mainly attributed to the increase in Al cations due to Al 2 O 3 incorporation, coupled with the inclusion of multiple cationic elements, to significantly enhance the rigidity of the glass network. Thereby, the viscosity and high-temperature stability of the resulting aluminosilicate glass are markedly improved, effectively protecting the underlying unoxidized HEAS-Al 2 O 3 . The as-developed HEAS-Al 2 O 3 shows great promise as a thermal structural candidate for next-generation hypersonic vehicles.
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高影响因子
International Journal of Minerals Metallurgy and Materials
·
2026
·Vol. 33
·期 6
·1870-1885
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IF 8.8
He Baili,Kou Jue,Sun Chunbao,Li Yue,Li Xiaolin,Temirov Uktam,Chang Ziyong
The development of effective adsorbents is crucial for the sustainable recovery of noble metals from secondary resources. In this study, MIL-101(Cr)-Tu, a Cr-based metal–organic framework (MOF) modified with thiourea, was successfully prepared by double-phase encapsulation followed by post-synthetic modification. At 298 K, the largest adsorption capacities of Au(III), Pd(II), and Pt(IV) by MIL-101(Cr)-Tu were (1230.83 ± 8.72), (330.41 ± 7.29), and (315.58 ± 13.67) mg·g −1 , respectively. The uptakes of Au(III), Pd(II), and Pt(IV) increased with temperature. The adsorption data fit well to both the Langmuir and pseudo-second-order kinetic models, indicating that the adsorption process conformed to monolayer adsorption and chemisorption. Mechanistic analysis revealed that the amino and thiourea groups facilitated the adsorption of noble metals through coordination and electrostatic attraction. Notably, Au(III), Pd(II), and Pt(IV) interacted strongly with the thiourea groups owing to their “soft–soft” interactions. Moreover, Au(III) was reduced to Au(I) and Au(0), Pt(IV) was reduced to Pt(II), and the amino groups were oxidized to NO 2 . The adsorption of Pd(II) did not involve redox reactions. Additionally, MIL-101(Cr)-Tu exhibited strong selectivity for noble metals and excellent reusability, demonstrating its great potential for the extraction of noble metals from secondary resources.
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高影响因子
Journal of Environmental Sciences
·
2026
·
IF 6.5
Mengqi Zhong,Hongrui Ma,Chao Zhu,Tingting Qu,Wenjie Quan
● The differences in the adsorption mechanisms of MIL-101(Fe) for small molecular ligands, larger molecular ligands, and mixed-ligand complexes were investigated. ● The adsorption capacity of MIL-101(Fe) for TA-Cr(Ⅲ) was superior to that of other ligands, with a maximum adsorption amount reaching 183.15 mg/g. ● The adsorption competitive of TA-Cr(Ⅲ) is stronger than that of EDTA-Cr(Ⅲ) and TA-EDTA-Cr(Ⅲ) in the mixed solution. ● The order of binding affinities for different interactions was clarified by combining DFT calculations. The ubiquity of diverse organic-Cr(Ⅲ) complexes in industrial effluents poses a significant challenge to water remediation due to their high stability and complex competitive behaviors. In this study, MIL-101(Fe) was employed to decipher the differential adsorption behaviors and mechanisms of single and co-existing Cr(Ⅲ) complexes, specifically targeting natural (Tannic acid (TA)) and anthropogenic (EDTA) ligands. The experimental results revealed a distinct selective hierarchy as TA-Cr(Ⅲ) > free Cr(Ⅲ) > EDTA-Cr(Ⅲ) > TA-EDTA-Cr(Ⅲ), with values of 183.15, 134.05, 93.02, and 73.80 mg/g, respectively. Among them, TA-Cr(Ⅲ) demonstrated an extremely strong adsorption capacity. Kinetic and isotherm analyses confirmed a chemisorption-dominated process. Crucially, the competitive mechanism was elucidated by integrating spectroscopic characterization with Density Functional Theory (DFT) calculations. The results revealed that while electrostatic interactions drive the initial approach, the specific affinity of phenolic hydroxyl groups in TA towards the Fe-clusters of metal organic frameworks (MOFs), combined with strong π-π stacking interactions, provides an advantage for TA-complexes. The differences of organic-metal complexes were revealed through analysis of electrostatic potential, frontier molecular orbitals and binding energy. This work provides a fundamental understanding of ligand-dependent competitive adsorption, offering a theoretical basis for the selective removal of complexed heavy metals in realistic aquatic environments. Download: Download high-res image (308KB) Download: Download full-size image
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