CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1845-1855
·
IF 2.372
Wang Tao,Hu Aiyun,Xu Guangzhi,Liu Chen,Wang Haijun,Xia Yongmei
Furfural (FAL) is one of the most important biomass-derived platform compounds. The catalytic transformation of FAL was investigated with three porous Zr–thiophenedicarboxylate hybrids for the production of furfuryl alcohol (FOL). Three Zr-based catalysts, including DUT-67(Zr), DUT-68(Zr) and DUT-69(Zr) were synthesized through a facile assembly of 2,5-thiophenedicarboxylate acid with ZrCl 4 using the acetic acid as a modulator under hydrothermal conditions. These catalysts were also characterized using FT-IR, XRD, SEM, TEM, N 2 adsorption–desorption, XPS and TG. The specific surface area of the DUT-69(Zr) is smaller than that of the DUT-68(Zr) and slightly larger than that of the DUT-67(Zr), but it has a relatively large pore volume and pore diameter. Although all three catalysts showed excellent catalytic activity towards the catalytic transfer hydrogenation of FAL into FOL, the DUT-69(Zr) material has slightly higher catalytic activity than the other two catalysts. Besides, considering the cost of catalyst preparation, the DUT-69(Zr) material was used as the optimal catalyst and studied in detail. A high FOL yield of 92.2% at 95.9% FAL conversion was achieved at 120 °C for 4 h over DUT-69(Zr). Meanwhile, the DUT-69(Zr) could be reused more than six times with a minor decrease in catalytic activity. Finally, a plausible mechanism for catalytic transfer hydrogenation of carbonyl compounds to produce corresponding alcohols was presented based on the results of the experiments and previous reports. Graphical Abstract
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Analytical Methods
·
2018
·Vol. 11
·期 1
·36-43
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IF 2.073
Shun-Hua Wu,Shu Wang,Wen-Le Fang,Xiao-Feng Guo,Hong Wang
In this study, we synthesized metal–organic frameworks (MOFs) UiO-67-bpydc using H2bpydc as ligands and Zr6 clusters as vertexes. Due to the protonation of the bipyridine group, UiO-67-bpydc shows pH-dependent fluorescence (365 nm/530 nm) in the pH range from 1 to 9, which shows its feasibility as a wide-range pH sensor. Further study indicated that UiO-67-bpydc exhibits stability, reusability, selectivity and has an excellent linear relationship in the pH range 4.0–6.5, and the mechanism of the UiO-67-bpydc fluorescence intensity with the variation of pH has been studied in detail. This MOF-based fluorescent sensor has been applied to specifically detect the pH of solutions in the presence of the body fluid matrix. Compared with reported pH-MOF sensors, UiO-67-bpydc can be practically applied in real samples and is easily prepared with excellent stability in different buffer solutions.
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CHEMISTRY OF MATERIALS
·
2017
·
IF 9.466
Jian Yang,Xiaojing Chen,Yongsheng Li,Qixin Zhuang,Peifeng Liu,Jinlou Gu
For practical biomedical applications, the stabilization of nanoscale metal–organic frameworks (NMOFs) in the presence of phosphate is of prime importance but remains a significant challenge because of the inevitable and strong driving force between metal clusters and phosphate species to form metal-phosphate in physiological environments. Through shielding Zr-NMOFs within the continuous phospholipid bilayers (PBLs), herein, we figured out a unique way to protect the vulnerable coordination bonds in their frameworks from the attack of phosphate. To exemplify the facility of constructing PBLs on Zr-NMOFs core, a porphyrinic NMOF of PCN-223 (standing for a platform with broad biological applications) was elaborated using a triethylamine (TEA)-modulated strategy. TEA could not only control the phase transformation of porphyrinic MOFs to achieve pure-phase PCN-223 crystals but also minimize their particles size down to sub-200 nm. Negative-stained TEM, FT-IR and XPS techniques revealed that PBLs could be closely coated onto the surface of nanoPCN-223, thanks to the strong Zr–O–P chemical complexation between Zr-NMOFs and phospholipid. The resultant coated nanoPCN-223 exhibited significantly enhanced phosphatic-resistance in phosphate buffer solution (PBS) and presented exceptional stability in harsh chemical environments. Furthermore, the MOFs-supported PBLs could effectively provide a stable biocompatible interface for subsequent cell culture and improve their biocompatibility, cellular uptake efficiency and real biostability of NMOFs in cellular environments. This study offers an alternative system for forming stable PBLs supported on NMOFs, and represents the first example of stabilizing Zr-NMOFs free from the attack of phosphate species in biological media.
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Catalysis Science & Technology
·
2016
·Vol. 6
·期 14
·5543-5553
·
IF 5.287
Xin Zhao,Lei Huang,Supawadee Namuangruk,Hang Hu,Xiaonan Hu,Liyi Shi,Dengsong Zhang
A novel Zr–CeVO4/TiO2 catalyst was developed for the selective catalytic reduction (SCR) of NO with NH3. Both TiO2 nanosheets (TiO2-NS) and nanoparticles (TiO2-NP) with different crystal facets were used as supports for the catalyst. It was found that the TiO2-NS-supported catalyst showed much better activity, stability and H2O/SO2 durability than the TiO2-NP-supported catalyst. In particular, the catalyst loading amount was much lower than those of previously reported vanadate-based SCR catalysts. The crystal structures and morphologies were analysed by X-ray diffraction (XRD), Raman spectroscopy and (high-resolution) transmission electron microscopy ((HR)TEM). The redox properties, surface active species and acid sites of the catalysts were investigated through hydrogen temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), ammonia and nitrogen oxide temperature-programmed desorption (NH3-TPD and NOx-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs) experiments. The improved activity at lower temperature was due to the presence of more active oxygen species and Brønsted acid sites, as well as the formation of NO2 on the surface of the TiO2 nanosheets which have exposed (001) facets. The enhanced stability and H2O/SO2 durability of Zr–CeVO4/TiO2-NS was due to the limited formation of NH4NO3 and (NH4)2SO4/NH4HSO4. The excellent low operation temperature, low vanadium content and absence of WO3(MoO3) in this catalyst indicated that it has promising potential as a SCR catalyst for practical applications.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2016
·
IF 4.179
Jian He,Hu Li,Yanxiu Liu,Wenfeng Zhao,Tingting Yang,Wei Xue,Song Yang
A series of mesoporous acid–base bifunctional Zr/B mixed oxides with different molar ratios were prepared by a sol–gel method, and developed for conversion of ethyl levulinate (EL) to γ -valerolactone (GVL) by using alcohol as hydrogen source. The morphological structures and physico-chemical characteristics of the synthesized materials were identified by various techniques. A high GVL yield of 88.5% was achieved from EL in 2-propanol when Zr 1 B 1 was used. And acid–base sites played a synergic role in synthesizing GVL from EL as evident by poisoning experiments. Furthermore, the catalyst could be reused several times without significant loss of its catalytic activity.
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Radiation Effects and Defects in Solids
·
2024
·
IF 1.1
X.L. Ren,G. Yao,L.M. Luo,Y. Xu,A. Yabuuchi,Q. Xu
In the present study, we developed Mo- and Zr-added W-Y2O3 composites, and investigated their surface damage, including commercially available W induced by He and D as well as He and D mixture plasmas. Blistering was not observed in the D-plasma-irradiated W and W composites. The thickness of the damaged surface layer due to He plasma exposure of the W-Mo-Y2O3 composite was similar to that of W. However, the thickness of the damaged surface layer of the W-Y2O3 composite was half that of W. In addition, the thickness of the damaged surface layer of the W-Zr-Y2O3 composite was further improved by 5 times. Y2O3 nanoparticles, especially refined Zr-Y-O nanoparticles, act as He trap sites to suppress the formation and growth of He bubbles. Furthermore, the W-O-Y and W-O-Zr-Y nanoparticles increased the solubility of He and delayed He diffusion, hindering the formation of He bubbles.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Chenyang Liu,Wei Ju,Yili Wang,Shuoxun Dong,Xiaolin Li,Xiaoyang Fan,Siying Wang
For metal-based phosphate adsorbents, the dispersity and utilization of surface metal active sites are crucial factors in their adsorption performance and synthesis cost. In this study, a biochar material modified with amorphous Zr–Ce (carbonate) oxides (BZCCO-13) was synthesized for the phosphate uptake, and the adsorption process was enhanced by magnetic field. The beside-magnetic field was shown to have a better influence than under-magnetic field on adsorption, with maximum adsorption capacities (123.67 mg P/g) 1.14-fold greater than that without magnetic field. The beside-magnetic field could also accelerate the adsorption rate, and the time to reach 90% maximum adsorption capacity decreased by 83%. BZCCO-13 has a wide range of application pHs from 5.0 to 10.0, with great selectivity and reusability. The results of XPS and ELNES showed that the "magnetophoresis" of Ce 3+ under the magnetic field was the main reason for the enhanced adsorption performance. In addition, increased surface roughness, pore size and oxygen vacancies , enhanced mass transfer by Lorentz force under a magnetic field, all beneficially influenced the adsorption process. The mechanism of phosphate adsorption by BZCCO-13 could be attributed to electrostatic attraction and CO 3 2– dominated ligand exchange. This study not only provided an effective strategy for designing highly effective phosphate adsorbents, but also provides a new light on the application of rare earth metal-based adsorbent in magnetic field.
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PubMed
高影响因子
Desalination and Water Treatment
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2024
·
IF 1
Honghuan Yin,Huaiwen Wang,Dongai Wang,Miaomiao Shi,Xi Xu,Jiaqi Yang
Developing low-cost and stable adsorbent is urgent and attractive to remove hazardous dye from water. In this study, zirconium based metal-organic framework (NH 2 -UiO-66) was grown on waste wool fibers and the fabricated composite adsorbent (NH 2 -UiO-66/wool) was used to remove anionic dye methyl orange (MO). After characterizing the adsorbents, we determined the effect of pH and initial concentration of MO on adsorption performance. Moreover, adsorption kinetics and isotherms were conducted to reveal the adsorption mechanism. The results showed that NH 2 -UiO-66/wool achieved the highest adsorption capacity at natural pH with the maximum adsorption of 61.0 mg/g adsorbent, which is higher than most biomass based adsorbents. Moreover, NH 2 -UiO-66/wool enabled a broad range of pH (3−11) and initial concentration of MO (10–50 mg/L). Adsorption kinetics and isotherms of NH 2 -UiO-66/wool fitted well with pseudo-second-order model and Langmuir mode, respectively. NH 2 -UiO-66/wool presented 40.3 times higher of kinetics constant than that of original wool in the presence of initial MO concentration of 10 mg/L due to the positive nature of NH 2 -UiO-66. Ultimately, NH 2 -UiO-66/wool presented excellent regeneration ability with 500 mg/L NaCl solution and regeneration efficiency remained 98% after 10 cycles. Overall, this work may provide new insights into the development of MOFs/wool adsorbents for enhanced dye removal.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Qibin Zhu,Long Chen,Yun Da
The Calcium looping thermochemical reaction directly driven by solar energy effectively addresses the problem of efficient energy storage of concentrated solar power plants (CSP) by shortening the energy conversion path. But new requirements are put forward for energy storage materials, including high solar radiation absorption, high cycling stability and fast kinetics. To meet these challenges, we have designed porous microsphere structures for the purpose of enhancing mass transfer and the capture of solar radiation. Additionally, Zr and Mn oxides with elevated Tammann temperatures were incorporated to stabilize the morphology and prevent sintering. The synthesized porous microspheres retained abundant mesoporous channels on the surface even after undergoing 20 cycles. The addition of Mn oxide significantly enhances solar spectral absorptivity, achieving an impressive 82.88 % absorbance. The incorporation of Mn and Zr oxides increased the sintering resistance, specific surface area and porosity of CaO/CaCO 3 , especially in the 10–100 nm range, which accelerated the CO 2 transport during carbonation. These enhancements significantly improve the chemical control stage of the carbonation reaction, as further supported by kinetic models. After 50 cycle experiments at 800 °C, the energy storage density of the sample remains at 1074 kJ/kg, which is 1.86 times that of the undoped CaCO 3 . This study provides a new way to design CaCO 3 materials suitable for CSP applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu
A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.
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高影响因子
International Journal of Applied Ceramic Technology
·
2024
·
IF 1.8
Shuaijun Yang,Mei Wang,Yetong Lv,Huilin Sheng,Yexia Qin
Oxidation resistance is crucial to the potential applications of high-entropy carbides (HECs) at elevated temperatures. Here, we realize the exploration of (Hf, Ta, Zr, Cr)C high-entropy carbides (HEC-TM, TM = Hf, Zr, Ta, and Cr) with good oxidation resistance by optimizing their compositions. To be specific, 21 kinds of HEC- x TM ( x = 0–25 mol%) samples are fabricated by a high-throughput ultrafast high-temperature sintering technique, followed by oxidation testing at 1673 K for 30 min. Among all the HEC samples, the as-fabricated HEC-0Zr samples are proved to possess the best oxidation resistance with an oxidation depth of only 53 µm. Further study on isothermal oxidation kinetics demonstrates that the as-fabricated HEC-0Zr samples follow a linear oxidation law. The good oxidation resistance of the as-fabricated HEC-0Zr samples is believed to result from the (Ta, Me) 2 O 5 phase with a low melting point, which can promote the densification of the oxide layer. This research opens up a new way for efficiently discovering new HECs for extreme applications.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 45
·19220-19228
·
IF 2.7
Peng Lu,Qianwen Hu,Kui Wang,Shiyong Chen,Zongxiao Li,Xinjie Chen,Chuang Xing,Yanhong Wang,Ce Du
The efficient CO2 conversion to light olefins through hydrogenation is a feasible strategy to achieve carbon neutrality goals. Herein, a series of bimetallic Zn–Zr/supports are synthesized by a conventional impregnation method. We demonstrate that different supports endow catalysts with various specific surface areas, pore sizes, chemical adsorption performances, and acid densities. The effects of different support-loaded Zn–Zr coupled with SAPO-34 on CO2 hydrogenation to light olefins are investigated systematically. The CO2 conversion of Zn–Zr/Q10-SAPO-34, Zn–Zr/Q50-SAPO-34, Zn–Zr/γAl2O3-SAPO-34, Zn–Zr/MgO-SAPO-34 and Zn–Zr/S-1-SAPO-34 is 11.4%, 9.2%, 24.0%, 8.8%, and 16.2%, respectively, with corresponding light olefin selectivity of 39.0%, 28.1%, 30.4%, 4.8%, and 14.7%, respectively. Significantly, γAl2O3 is more conducive to CO2 conversion, while Q10 tends to produce light olefins. This work provides an effective reference for support selection in CO2 hydrogenation to light olefins.
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