Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 14
·2629-2636
·
IF 5.958
Guoan Lin,Ran Wang,Tongcheng Cao,Liangxi Yuan,Xiaoxiang Xu
With an absorption edge as far as 690 nm, SrNbO2N holds great promise for solar energy conversion. However, very poor photocatalytic activity is generally seen for SrNbO2N, limiting its practical applications as a photocatalyst. In this work, SrNbO2N is modified by introducing Zr at B sites, i.e. SrNb1−xZrxO2+yN1−y (0 ≤ x ≤ 1), which are then investigated as photocatalysts for water oxidation reactions. Zr modification not only induces porous microstructures and inhibits the formation of Nb4+ defects, but it also ameliorates the surface hydrophilicity of SrNbO2N. Clear improvements in photocatalytic water oxidation have been realized after Zr modification and an apparent quantum efficiency of as high as 1.44% has been achieved. Further analysis of the band edge alignments suggests that Zr modification positively shifts the valence band edge of SrNbO2N, which favors water oxidation reactions.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 34
·19060-19074
·
IF 4.22
Gao Nan,Tan Runan,Cai Zhiwei,Zhao Hui,Chang Gang,He Yunbin
Methyl parathion (MP), as a typical organophosphorus pesticide, has been widely used in pest control and plant growth regulation. Simultaneously, the problem of pesticide residues also poses a serious threat to the environment and human health. Currently, pesticide residue detection technology still faces great challenges in practical applications due to the problems of expensive facilities and complicated operations in conventional analysis methods. To address these problems, a novel nonenzymatic electrochemical pesticide sensor was reported. A zirconium-based metal organic framework material with terephthalic acid as a ligand (Zr-BDC) was designed to combine with electro-reduced graphene oxides (rGO). The Zr-BDC-rGO nanocomposite contains Zr-OH groups with high affinity for phosphate groups, endowing it with selective recognition and a higher adsorption capacity for MP. Moreover, rGO has a high specific surface area and excellent electron transport capability, making it an excellent functionalized adsorption and substrate material, which could improve the conductivity of the material and achieve a lower detection limit. Upon optimization, this sensor provided a wide linear range from 0.001 to 3.0 μg mL −1 and low limit of detection 0.5 ng mL −1 for MP. This work provides a rapid, sensitive and cost-effective sensing platform for pesticide residue detection. Graphical abstract
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Haotian Li,Mao Fu,Shi-Qiang Wang,Xiangyong Zheng,Min Zhao,Fenglin Yang,Chuyang Y. Tang,Yingchao Dong
Treatment of hypersaline waters is a critical environmental challenge. Pervaporation (PV) desalination is a promising technique to address this challenge, but current PV membranes still suffer from challenging issues such as low flux and insufficient stability. Herein, we propose in situ nanoseeding followed by a secondary growth strategy to fabricate a high-quality stable metal–organic framework (MOF) thin membrane (UiO-66) for high-performance pervaporation desalination of hypersaline waters. To address the issue of membrane quality, a TiO2 nano-interlayer was introduced on coarse mullite substrates to favor the growth of a UiO-66 nanoseed layer, on which a well-intergrown UiO-66 selective membrane layer with thickness as low as 1 μm was finally produced via subsequent secondary growth. The PV separation performance for hypersaline waters was systematically investigated at different salt concentrations, feed temperatures, and long-term operation in different extreme chemical environments. Besides having nearly complete rejection (99.9%), the UiO-66 membrane exhibited high flux (37.4 L·m–2·h–1) for hypersaline waters, outperforming current existing zeolite and MOF membranes. The membrane also demonstrated superior long-term operational stability under various harsh environments (hypersaline, hot, and acidic/alkaline feed water) and mild fouling behavior. The rational design proposed in this study is not only applicable for the development of a high-quality UiO-66 membrane enabling harsh hypersaline water treatment but can also be potentially extended to other next-generation nanoporous MOF membranes for more environmental applications.
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高影响因子
JOURNAL OF MATERIALS RESEARCH
·
2019
·Vol. 34
·期 24
·4045-4055
·
IF 1.982
Bo-Qiong Li,Xin-Cheng Li,Xing Lu
In recent years, there has been a significant thrust toward the development of novel implant alloys based on β-Ti with low Young’s modulus to prevent stress shielding. In this study, porous Ti–Nb–Ta–Zr alloys with porosity of <55% and macro-pore size of 100–400 μm for biomedical applications were successfully fabricated by a space-holder method. The microstructure and compressive behavior were studied. The results show that the micro-pore size of porous Ti–Nb–Ta–Zr alloys decreases with an increase in the amount of the process control agent (PCA), which has no obvious effect on the porosity and the macro-pore size formed by the space holder. Porous Ti–Nb–Ta–Zr alloys fail mainly because of the cleavage and ductile fracture with some dimples in compression. The compressive modulus increases from 0.6 to 6.5 GPa with the increase in the PCA and decrease of the space holder. The influence mechanism has been analyzed by the finite element calculation and the Gibson–Ashby model.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Lu Li,Pan Li,Yanjie Wang,Lin Lin,Aamir Hassan Shah,Tao He
The defects like oxygen vacancy in a photocatalyst are critical factors to influence the photocatalytic reactivity since they can have an impact on the behavior of photogenerated charge carrier. Since oxygen vacancy can be readily formed in the ceria due to reversible conversion of the oxidation states between Ce 4+ and Ce 3+ , here ceria is used as the target material. A versatile and facile co-precipitation method was adopted to synthesize hydrangea-like Ce 1−x Zr x O 2 (x = 0.00, 0.025, 0.05 and 0.10). The amount of oxygen vacancy in the obtained catalysts can be modulated by altering the molar fraction of doped Zr. The composition, morphology, physico-chemical properties of the as-synthesized Ce 1−x Zr x O 2 were characterized by using different techniques. It is found that Zr doping into the ceria crystal lattice can lead not only to an enhanced specific surface area and surface adsorption capacity for CO 2 , but also to an increased concentration of oxygen vacancy that can exist in the bulk and on the surface. The Zr-doped ceria exhibits an enhanced activity for photoreduction of CO 2 , which can be explained based on the influence mechanism of oxygen vacancy. This work shows that the oxygen vacancy in the ceria can be modulated via a feasible Zr doping approach, which may help design the photocatalysts with high activity for CO 2 photoreduction.
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CATALYSIS SURVEYS FROM ASIA
·
2018
·Vol. 22
·期 4
·222-229
·
IF 3.081
Gao Meixiang,Jiang Haoxi,Zhang Minhua
Series of ZrO 2 supported on the different kinds of SiO 2 carriers were applied in the reaction of 1, 3-butadiene formation from ethanol and acetaldehyde. ZrO 2 /Nano-SiO 2 performed the best performance with the 1, 3-butadiene selectivity 91.43% and the total conversation 52.39%. Prepared catalysts were characterized by N 2 adsorption–desorption, TEM, XRD, temperature-programmed desorption of NH 3 and CO 2 , FTIR spectroscopy of adsorbed pyridine and CO 2 , Raman XPS. The results show that the weak Lewis acid and basic sites are appropriate for BD formation. Furthermore, more and balance acid-basic sites are rather important for the reaction of ethanol and acetaldehyde conversion to BD.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2018
·Vol. 45
·期 3
·1263-1279
·
IF 1.674
Feng Sheng,Wang Runbai,Feng Shanshan,Zhang Zhihui,Mao Lebao
A novel ternary complex photocatalyst (UiO-66/ g -C 3 N 4 /Ag) was fabricated by chemical protonation coating and photodeposition and its physicochemical parameters, crystal morphology, and electrochemical properties characterized using a series of techniques. Proper addition of g -C 3 N 4 and Ag effectively enhanced the separation and mobility of photoinduced charge and improved the visible-light absorption and thereby the catalytic performance. Degradation experiments on target contaminants such as Rhodamine B (RhB) dye and 2,4-dichlorophenoxyacetic acid (2,4- d ) showed that the photocatalytic ability of UiO-66/ g -C 3 N 4 /Ag(15) was greatly increased compared with the parent material. Moreover, the composite could be regenerated by a simple ethanol washing process and exhibited stability and high reusability over six cycles. Finally, experiments on trapping of active species revealed that superoxide radicals (·O
− 2
), holes (h + ), and hydroxyl radicals (·OH) were primarily responsible for the photodegradation of RhB and 2,4- d .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Weiyan Du,Yaru Li,Xing Xu,Yanan Shang,Baoyu Gao,Qinyan Yue
Bimetallic oxides nanocomposites always exhibited the better phosphate capacities than those monometallic oxides samples. Herein, the high carbohydrate-content biomaterials, shaddock peels (SP), were used as the bio-host for supporting the bimetallic oxides, zirconium (Zr) and lanthanum (La) hydroxides, forming the SP-Zr-La composites. Phosphate adsorption properties as well as stability of the novel composites were evaluated. The SP-Zr-La composites indicated that some rod-like or amorphous nanoparticles with sizes of 20–150 nm were anchored inside the SP, which exerted more available interface interactions toward the adsorbed ions. The Zr-La species were pH-sensitive and adsorption capacity of phosphate by SP-Zr-La was increased with the rise in temperature. As the molar ratio of accompanying ions/phosphate was increased from 0 to 10 times, the SP-Zr-La was observed with the adsorption loss of 27.2–36.7%. Whereas the adsorption loss of cationic SP (grafted with quaternary ammonium groups) was calculated up to 86.2–91.6%; this indicated the more feasibility of SP-Zr-La in real applications. In addition, the stability of impregnated Zr and La species in SP-Zr-La was greatly improved by the bio-carrier through the “shielding effect” in a low HA surrounding.
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APPLIED CLAY SCIENCE
·
2014
·
IF 2.703
Weiya Huang,Jie Chen,Fei He,Jinpeng Tang,Dan Li,Yi Zhu,Yuanming Zhang
Zirconium-pillared montmorillonite (Zr-Mt) and zirconium/aluminum-pillared montmorillonite (Zr/Al-Mt) were prepared by intercalating Zr 4 + and Zr 4 + /Al 3 + polyhydroxy-cations into the interlayer spaces of natural montmorillonite (Mt). Zr-Mt and Zr/Al-Mt exhibited greater specific surface areas and pore volumes, as compared with Mt. In particular, the enhancement in the phosphate removal performance of Zr/Al-Mt was more significant in terms of phosphate adsorption capacity and rate, in relation to Zr-Mt. Herein, several important parameters, such as contact time, temperature, initial solution pH and competing anion, were investigated in detail to evaluate the phosphate adsorption performances of Zr/Al-Mt. The pseudo-second-order kinetic model fitted our acquired phosphate adsorption data best, in comparison with the use of the pseudo-first-order or the pseudo-third-order kinetic model. The Langmuir model appeared to fit the adsorption process better than that of the Freundlich model, with a maximum phosphate adsorption capacity of 17.2 mg P/g at 25 °C. The thermodynamic parameters (ΔG°, ΔH° and ΔS°) were also determined, which revealed that the phosphate adsorption process was spontaneous and endothermic in nature. A high adsorption capacity was observed at pH = 3.0, which decreased by increasing pH. The presence of competitive ions, e.g. Cl − , NO 3 − , and SO 4 2 − , slightly impacted the phosphate adsorption; whereas the introduction of CO 3 2 − caused the greatest adverse effect. The study on the Zr/Al-Mt leaching strongly suggested that the risk of Zr 4 + leakage during adsorption process be negligible within a wide pH range of 3.0–9.0. After three adsorption-desorption cycles, there was no significant loss in the adsorption performance of Zr/Al-Mt.
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RSC Advances
·
2015
·Vol. 6
·期 5
·3671-3679
·
IF 3.84
Aoning Wang,Yingjie Zhou,Zhoulu Wang,Miao Chen,Luyi Sun,Xiang Liu
A UiO-66-type metal–organic framework (MOF) fabricated with titanium was successfully prepared via a facial modified post-grafting method. The as-prepared samples were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), ultraviolet-visible adsorption spectroscopy (UV-vis), and photoluminescence spectroscopy (PL) techniques. The introduction of titanium enhanced the optical properties of UiO-66 via the formation of oxo-bridged hetero-Zr–Ti clusters, but led to a sacrifice in crystallinity. The removal of methylene blue (MB) over these samples could be attributed to the dual function of the adsorption and photo-degradation mechanisms. The highest MB removal efficiency of 87.1% was achieved over UiO-66(1.25Ti) under simulated sun-light irradiation.
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RSC Advances
·
2016
·Vol. 6
·期 42
·35859-35867
·
IF 3.289
Pinghua Chen,Weibo Zhang,Menglin Li,Peng Ai,Lei Tian,Hualin Jiang
A novel magnetic composite of La–Zr was prepared by co-precipitation method, and its fluoride removal ability was investigated in batch studies. The sample was characterized by SEM, EDS and FTIR. Influence of various factors such as pH, presence of coexisting anions, contacting time and initial fluoride concentration were studied in detail by batch sorption experiments. The equilibrium data fitted to Langmuir, Freundlich and Lan–Fre isotherm model, and the maximum sorption capacity was calculated to be 88.5 mg g−1, which is higher than lots of previous adsorbents. The kinetic data can be described well by the pseudo-second-order kinetic model. It was indicated that the overall rate of fluoride sorption is likely to be controlled by chemisorption process. Based on the results, the mechanism of adsorption was discussed in detail. There is no calcination in the preparing process, so this material is considered to be lower cost as compared with some metal elements-based oxides adsorbents, and is beneficial for the practical application.
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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Chengxin Fu,Yinyan Gong,Yitao Wu,Jiaqi Liu,Zhen Zhang,Can Li,Lengyuan Niu
Visible-light photodegradation test revealed that B and Zr co-doping can raise the photocatalytic ability of the undoped TiO 2 by a fold. XRD crystallography and Raman phonon spectroscopy measurements suggest that the Zr 4+ ions replace the Ti 4+ ions while the B 3+ ions occupy the interstitial sites, expanding the unit-cell volume and reducing crystallite size. The incorporation of interstitial boron dopants creates oxygen vacancies (Ov ) and reduce Ti 4+ to Ti 3+ to form [Ov -Ti 3+ ] + , which traps the carriers and prolongs carrier lifetime. Moreover, Zr 4+ ions replace Ti 4+ ions and form impurity levels, which could improve visible light response. The co-doped samples are benefited from both B interstitials and Zr substitutes.
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