CARBOHYDRATE POLYMERS
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2023
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IF 11.2
Yanxiao Yang,Yunfeng Guo,Zhe Qiu,Weihua Gong,Yonggui Wang,Yanjun Xie,Zefang Xiao
Metal-organic frameworks (MOFs) are characterised by high porosity levels and controllable structures, making them ideal adsorbents for wastewater. However, obtaining substrate materials with mechanical stability, excellent pore accessibility, and good processability for compositing MOF crystal powders to adsorb multiple pollutants in complex aqueous environments is challenging. In this study, porous MOFs@ modified cellulose sponge (MCS) composites were fabricated using MCS as a scaffold to provide anchoring sites for the coordination of Zr 4+ ions and further in situ synthesis of MOFs, namely UiO-66@MCS and UiO-66-NH 2 @MCS, which effectively removed heavy metal ions and organic dyes. MOFs@MCS composites exhibit excellent water and dimensional stability, maintaining the pore structure by ambient drying during reuse. Compared with UiO-66@MCS composite, UiO-66-NH 2 @MCS composite exhibited a higher adsorption capacity of 224.5 mg·g −1 for Hg 2+ and 400.9 mg·g −1 for methylene blue (MB). The adsorption of Hg 2+ onto the MOFs@MCS composites followed the Langmuir and pseudo-second-order models, whereas the Freundlich and pseudo-second-order models were more suitable for MB adsorption. Moreover, the MOFs@MCS composites exhibited excellent reusability and were selective for the removal of Hg 2+ . Overall, this approach effectively combines Zr-based MOFs with mechanically and dimensionally stable porous cellulose sponges, rendering the approach suitable for purifying complex wastewater.
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高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 6
·3565-3574
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IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jie Chen,Jianzhong Ma,Qianqian Fan,Wenbo Zhang,Ruyue Guo
The development of chrome-free tanning agents is of great significance for the green and sustainable improvement of the leather industry. Metal organic framework (MOFs) is a kind of nanomaterial with steady framework formed by the coordination of metal clusters with organic ligands, which gives it a natural self-masking structure. Herein, two kinds of bimetallic MOFs were obtained via post-synthesis modification and used in the tanning to produce leather with good hydrothermal stability. M n+ - replacing Zr-MOFs is denoted as Zr/M−MOFs (M n+ = Ti 4+ , Al 3+ ). Zr/M−MOFs were characterized by XRD, SEM, FT-IR, TG, XPS, and N 2 adsorption/desorption. The results indicate that M n+ - replacing provides more active site that can be combined with collagen fibers. Compared to the Zr-MOFs tanned leather (75.3 °C), the shrinkage temperature of Zr/M−MOFs tanned leather (79.9 °C) has been further improved. In addition, Zr/M−MOFs can also avoid the problems caused by traditional metal tanning, such as the worse washability of aluminum tanning. A new strategy to improve the tanning performance of MOFs-based tanning agents was provided. It gives a new approach to the development of chrome-free tanning agents.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Jiesong Tan,Yiqing Zeng,Ze-Xian Low,Zhaochen Lin,Xinxiang Xu,Shasha Feng,Zhaoxiang Zhong,Weihong Xing
The filtration of high-temperature flue gases containing complex gas composition and oily particulate matter (PM) poses great challenges to the design of air filtration membranes. Ceramic nanofibers are potential membrane materials that possess the thermal resistance necessary for high-temperature filtration but the inherit poor brittleness limits their use. Herein, we report the fabrication of a flexible and porous Zr-doped TiO 2 nanofibrous membrane (Zr–TiO 2 NFM) for oily PM removal from high-temperature flue gas. The doping of Zr 4+ ions not only improved the mechanical strength , leading to an outstanding tensile strength as high as 1.78 MPa, but also endowed a high specific area (68.34 m 2 g −1 ). The prepared Zr–TiO 2 NFMs possessed a high filtration efficiency of 99.98% with low pressure drop of 96 Pa (industrial gas velocity of 1 m∙min −1 ) and excellent long-term stability after 5 cycles of filtration at 350 °C. Significantly, different capture and evolution behaviors of PM at 25–350 °C were discovered. Below 200 °C, the oily particles would adhere, coalesce, spread out and form oil film on fibers. Different from oily particles, the non-oily particles would attach and accumulate on the fibers when temperatures are higher than 200 °C. This study brings a new insight to deeply understanding the capture process of PM at different temperatures and designing next-generation membranes for high temperature flue gas filtration.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
·
IF 5.2
Yunlong Li,Miao Liu,Yixian Liu,Lilong Zhou,Jilong Han,Zhengjie Li,Jimmy Yun,Runjing Liu
Two kinds of Ce-doped UiO-66 were synthesized by using CeCl 3 ·7H 2 O and (NH 4 ) 2 Ce(NO 3 ) 6 as cerium precursors, namely Ce(III)- and Ce(IV)-UiO-66. The effect of valence states of cerium precursors on adsorption performance towards Rhodamine B (RhB) was investigated for the first time. Ce atoms are in two valence states of +3 and + 4, where Ce 3+ ions turn their surfaces negatively charged. The higher cerium content (24.8%) and ratio of Ce 3+ /Ce 4+ ions (1.4:1) of Ce(IV)-UiO-66 made its surface more negatively charged, which is contributed to form stronger electrostatic interaction with cationic dyes. The adsorption amounts of RhB were 239.5 mg/g and 431.7 mg/g for Ce(III)- and Ce(IV)-UiO-66, which are 2.38 and 5.11 times higher than pristine UiO-66, respectively. The well-fit Langmuir model and pseudo-second-order model suggest a monolayer chemisorption process. The adsorption mechanism suggests that the electrostatic interaction and the complexation interaction between Ce 3+ and RhB are dominant factors affecting RhB adsorption. Since Ce 3+ severed as adsorption sites, the higher Ce content and stronger electrostatic interaction of Ce(IV)-UiO-66 together promoted its RhB adsorption than Ce(III)-UiO-66. The obtained results help to understand how the mixed-valences of incorporated metals affect the adsorption behaviors of bimetallic MOFs deeply.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 6
·971
·
IF 3.9
Chunjie Shi,Xiaofeng Yu,Wei Wang,Haibing Wu,Ai Zhang,Shengjin Liu
The catalytic activity and cyclic catalysis of different methyl benzoates were studied by using a series of Lewis solid acid catalysts. The iron-supported zirconium/titanium solid acid catalysts were characterized using FTIR, SEM, XRD, and BET. The details of catalytic activity and cyclic catalysis verified that the catalyst catalyzed the reactions of 31 benzoic acids with different substituents and methanol. In addition, the mechanism was revealed according to the microstructure, acid strength, and specific surface area of the catalysts, and the yields of methyl benzoates by the GC-MS. Zr ions had significant effects on the catalytic activity of the catalyst. A certain proportion of Fe and Ti ions additionally enhanced the catalytic activity of the catalyst, with the catalyst-specific composition of Fe:Zr:Ti = 2:1:1 showing optimal catalytic activity. A variety of substituents in the benzene ring, such as the electron-withdrawing group, the electron-donating group, large steric hindrance, and the position of the group on the benzene ring, had regular effects on the catalytic activity of the methyl benzoates. An increase in the catalyst activity occurred owing to the increases in the catalyst surface and the number of acid sites after the Fe ion was added. The catalytic activity remained unchanged after the facile recycling method was performed.Keywords:zirconium/titanium solid acid;iron-supported;methyl benzoate compounds
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Biomaterials Advances
·
2023
·
IF 0
Renhao Xue,Xinru Deng,Xiaoning Xu,Yueyan Tian,Abshar Hasan,Alvaro Mata,Ligang Zhang,Libin Liu
The biocompatibility of biomedical materials is vital to their applicability and functionality. However, modifying surfaces for enhanced biocompatibility using traditional surface treatment techniques is challenging. We employed a mineralizing elastin-like recombinamer (ELR) self-assembling platform to mediate mineralization on Zr-16Nb-xTi (x = 4,16 wt%) alloy surfaces, resulting in the modification of surface morphology and bioactivity while improving the biocompatibility of the material. We modulated the level of nanocrystal organization by adjusting the cross-linker ratio. Nanoindentation tests revealed that the mineralized configuration had nonuniformity with respect to Young's modulus and hardness, with the center areas having higher values (5.626 ± 0.109 GPa and 0.264 ± 0.022 GPa) compared to the edges (4.282 ± 0.327 GPa and 0.143 ± 0.023 GPa). The Scratch test results indicated high bonding strength (2.668 ± 0.117 N) between the mineralized coating and the substrate. Mineralized Zr-16Nb-xTi (x = 4,16 wt%) alloys had higher viability compared to untreated alloys, which exhibited high cell viability (>100 %) after 5 days and high alkaline phosphatase activity after 7 days. Cell proliferation assays indicated that MG 63 cells grew faster on mineralized surfaces than on untreated surfaces. Scanning electron microscopy imaging confirmed that the cells adhered and spread well on mineralized surfaces. Furthermore, hemocompatibility test results revealed that all mineralized samples were non-hemolytic. Our results demonstrate the viability of employing the ELR mineralizing platform to improve alloy biocompatibility.
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ChemistrySelect
·
2023
·Vol. 8
·期 16
·e202300902
·
IF 2.1
Panli Liu,Shengbin Shi,Ruiping Wei,Lijing Gao,Jin Zhang,Guomin Xiao
Graphical P-Zr-SBA-15 catalyst with bifunctional acidity was synthesized by introducing Zr 4+ into the mesoporous material SBA-15 structure for intra skeleton modification, and then impregnated with phosphoric acid solution to modify the outer skeleton. The catalyst exhibits excellent catalytic activity, good thermal stability, and recoverability in the preparation of furfural. A series of bifunctional P-Zr-SBA-15 catalysts with Lewis acid and Brønsted acid sites were prepared by modifying mesoporous material SBA-15 with Zr 4+ and phosphate group, which were used in the conversion of xylose and xylan into furfural. The structure and acidic characteristics of the catalyst were analyzed by X-ray diffraction, Fourier transform infrared spectroscopy, N 2 adsorption desorption, scanning/transmission electron microscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, NH 3 temperature programmed desorption, and pyridine adsorption infrared spectroscopy. The effects of different process parameters on the catalytic performance of the catalyst were studied. when using the xylose and xylan as substrates, the furfural yield were 80.3 % and 68.8 % under the optimal conditions in the H 2 O (NaCl) /toluene (3/3 mL) biphasic solvent system, respectively, and 52.5 % furfural yield was obtained using xylose as substrate in aqueous system. In addition, the catalyst has good thermal stability and easy recovery in the recycling experiment.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 98
·期 7
·1620-1630
·
IF 3.4
Minhua Zhang,Yan Zhang,Yuxin Tan,Guochao Yang,Haoxi Jiang,Lingtao Wang
BACKGROUND With the improvements in bioethanol production, the process of converting ethanol to 1,3-butadiene (ETB) has received substantial scholarly attention, whose industrialization has been constrained by the stability of the catalysts. RESULTS In this work, the deactivation behavior of Zr- β zeolite in the process of ethanol/acetaldehyde conversion to 1,3-butadiene was investigated. In addition, the deactivation kinetics of ETB was studied using an isothermal differential microreactor. A kinetic model was developed and parametrized with the Langmuir–Hinshelwood mechanism, and the intrinsic kinetic equation was derived. The deactivation kinetic model of the ETB reaction was established from the active site content of the catalyst as a function of time on stream. The validity of the kinetic model was tested, and the results were found to be accurate. CONCLUSIONS Catalyst deactivation was mainly caused by coke species, which are mainly long-chain unsaturated oxygenated organic compounds and aromatic compounds, covering Lewis acid sites in the microporous channels of the catalyst; nevertheless the zeotype topology and morphology were not destroyed. The kinetic data suggested that the reaction was of first order and the activation energy of the deactivation process was 75.59 kJ mol −1 . © 2023 Society of Chemical Industry (SCI).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Guang-Rong Ding,Yao-Feng Wang,Guo-Yi Duan,You-Qian Fan,Bao-Hua Xu
In this study, a tungstated zirconia (WOx/ZrO2) catalyst was developed for the continuous synthesis of adiponitrile (ADN) by gas-phase nitrilation of dimethyl adipate (DMA) with NH3. The highest TOFADN could be reached on WOx/ZrO2 bearing ∼1D WOx species (highly dispersed and discontinuous status) at the surface, which, however, delivered the poorest selectivity toward nitrilation (SADN+MCP). In comparison, both efficient and selective transformation of DMA to ADN was achieved by fabricating WOx/ZrO2 with continuously distributed oligomeric WOx species (∼2D) at the surface, either by varying the dosage of the W-reagent in the preparation of WOx(m)/ZrO2 or by doping a proper amount of the Mn element into WOx(5.0)/ZrO2, bearing WO3 NPs. Furthermore, the in situ diffuse reflectance infrared Fourier transform spectroscopy investigations of both independent and competitive adsorptions of ester functionality and NH3 over W–O–Zr, W–O–W, and Zr–O–Zr boundaries at the surface clarified the synergistic effect of these species in the activation of DMA/NH3 and thereby nitrilation.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Fufeng Cai,Peijing Lu,Jessica Juweriah Ibrahim,Yu Fu,Jun Zhang,Yuhan Sun
Methanol steam reforming is regarded as a very promising process to generate H 2 suitable for fuel cells. Typically, the Pd-based catalysts can catalyze efficiently methanol steam reforming for hydrogen production . But their high selectivity to CO, a byproduct of methanol reforming reaction , severely limits their potential application. In this work, a series of Nb-modified Pd−Zr−Zn catalysts with different Nb loadings were prepared to study their catalytic activities with more focus on the role of Nb on Pd−Zr−Zn catalyst for methanol steam reforming. The prepared catalysts were fully analyzed by using various characterization techniques, for example, ICP , BET, SEM, XRD , H 2 -TPR, NH 3 -TPD, HRTEM , CO chemisorption , XPS, and Raman. The experimental results showed that an increase in Nb loading for the Nb-modified Pd−Zr−Zn catalysts led to a decrease of the methanol conversion and H 2 production rate. This was probably due to the decrease in the amount of oxygen vacancies on the catalyst surface . However, introduction of Nb into Pd−Zr−Zn catalyst increased the acid strength on the catalytic surface. The aldehyde species derived from methanol decomposition were readily transformed to HCOOH, thus yielding high selectivity to CO 2 for the Nb-modified Pd−Zr−Zn catalysts. Significantly, the addition of Nb to Pd−Zr−Zn catalyst facilitated the incorporation of Pd into the ZnO lattices, which led to the formation of Pd−Zn alloy. Consequently, the Nb-modified Pd−Zr−Zn catalysts exhibited significantly lower CO selectivity and production rate than the Pd−Zr−Zn catalyst. From the results, this work offers a new way to the rational design of selective methanol steam reforming catalysts to decrease the formation of byproduct CO.
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高影响因子
ACS Applied Nano Materials
·
2019
·
IF 0
Xian Fang,Xiaoyan Chen,Ying Liu,Qiuju Li,Zhongrun Zeng,T. Maiyalagan,Shun Mao
Rapid determination of trace antibiotics is critical for environmental monitoring and the ecosystem. In this study, a sensitive and selective electrochemical sensor for ciprofloxacin (Cip) detection by anodic stripping voltammetry of Cu2+ is designed. Zr(IV)-based metal–organic framework (MOF) NH2–UiO-66 and reduced graphene oxide (RGO) composites are used as working electrodes, which have a large surface area with porous structure and high electrical conductivity. Because Cip can form a stable composite with Cu2+ due to the complexation reaction, the anodic stripping voltammetry method is used for Cip determination with Cu deposition on the NH2–UiO-66/RGO-modified electrode. When Cip is present, the oxidization current of Cu2+ decreases significantly due to the formation of Cu2+–Cip complex. The prepared NH2–UiO-66/RGO sensor can detect trace levels of Cip down to 6.67 nM with a sensitivity of 10.86 μA μM–1, and a linear working range from 0.02 to 1 μM, which is superior to other electrochemical Cip sensors reported previously. The sensor also shows high selectivity, reproducibility, and stability in Cip sensing. Meanwhile, the electrochemical sensor is capable to detect Cip in real water samples with satisfactory recoveries. The ultrasensitivity, rapid detection, and easy operation of the reported sensors present significant potentials for real-time analysis and monitoring of trace antibiotic contaminants in water.
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