FUEL
·
2022
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IF 8.035
Ruolan Li,Zongqian Wu,Ya Chen,Xingyan Liu,Weiwei Guo,Yumin Huang,Min Fu,Youzhou He
An efficient bifunctional porphyrin-based MOF is fabricated for photocatalytic hydrogen evolution and NO removal, in which the mixed Zr/Ti-oxo clusters are the metal nodes and uniformly distributed Pt nanoparticles (Pt NPs) are the co-catalysts. It is worth noting that the optimal Zr-MOF-s(Pt)(Zr/Ti)-R is obtained through replacing partial Zr(IV) with Ti(IV) in the original Zr-based porphyrin MOFs and in-situ generating confined Pt NPs with a relatively small size within the internal cavities. Compared with the majority of reported Zr-based porphyrin MOFs, the Zr-MOF-s(Pt)(Zr/Ti)-R exhibits an extremely high hydrogen evolution activity (2545.11 μmol·g −1 ·h −1 ) and NO removal rate (46.6 %) under visible light irradiation. The excellent photocatalytic performance should be ascribed to the reason that the mixed Zr/Ti-oxo cluster and the in-situ generated Pt NPs significantly promote the rate of charge transfer and separation. Moreover, the photocatalytic NO oxidation process was also monitored by in - situ DRIFTS, which indicates the Zr-MOF-s(Pt)(Zr/Ti)-R could realize the effective oxidation of NO and intermediates to the final product (NO 3 – ). This work provides us with a practical route to further improve the photocatalytic performance by synergistically modifying the original metal clusters to adjust the ligand-to-metal charge transfer efficiency and in-situ introducing metal nanoparticles to form Schottky junctions.
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高影响因子
POLYMER COMPOSITES
·
2023
·
IF 5.2
Yi Li,Ning Zhang,Jicai Liang,Kaifeng Yu,Zengxia Zhao,Ce Liang
Composites with good thermomechanical and UV-shielding properties are essential in fiber-reinforced composites. This paper focuses on composites' ultraviolet (UV) shielding efficiency with added Ce-Zr-Si oxide nanoparticles/epoxy resin. The Ce-Zr oxide nanoparticles were first functionalized with a silicon coupling agent and ethyl silicate to improve their dispersion and surface activity. In this work, we prepared epoxy nanocomposites with the addition of Ce-Zr -Si oxides(1,3,5,7 wt%) and found that the materials had good enhancement of the UV shielding properties of the epoxy resin matrix. Meanwhile, it was used in basalt fiber (BF)/epoxy composites prepared by the hot-pressing method, and surface treatment of basalt fibers was carried out. The results showed that the modified fiber composites could effectively enhance the thermomechanical properties of epoxy resin composites. It is noteworthy that the tensile strength and flexural strength of the hybrid composites reached their peak when 5 wt% Ce-Zr-Si was added, increasing by 13.8% and 33.67% respectively. The modified (BF)/epoxy composites exhibited improved thermal stability compared to pure epoxy resin, with the maximum weight loss temperature of BF-1/EP reaching 349°C. The T(UVA) decreased to 2.41%, while the T(UVB) decreased to 0.053%, and almost all the ultraviolet irradiation was blocked. These results show that our prepared composites have good thermomechanical and UV shielding properties. Highlights Ce-Zr oxide nanoparticles were functionalized with a silicon coupling agent. Ce-Zr-Si oxide was added to enhance the ultraviolet shielding efficiency. Modified BFs were composited to improve thermomechanical properties.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2022
·
IF 12.545
Xiaohai Yan,Gengan Du,Hong Chen,Qiannan Zhao,Qi Guo,Jianlong Wang,Zhouli Wang,Wei Song,Qinglin Sheng,Yane Luo,Yahong Yuan,Tianli Yue
Patulin (PAT) is an unsaturated lactone mycotoxin primarily produced by Penicillium expansum and Aspergillus clavatus . Given the potential health risks and economic losses associated with PAT, the rapid detection of PAT using fluorescent aptasensors is of significant importance in evaluating food safety. However, it easily increases the cost and complexity caused by signal labeling. We combined TCPP/BDC-NH 2 mixed ligands functionalized Zr metal–organic frameworks (Zr-MOF mix ) and terminated three-stranded DNA gates (ttsDNA gates) to fabricate a label-free fluorescent aptasensor for PAT detection. The Zr-MOF mix system was synthesized via a one-pot strategy and could be used to address the problem of pore size limitation and increase the loading amounts of dyes. TtsDNA gate was integrated into the Zr-MOF mix system to control the release of dyes, exhibiting a high signal-to-background ratio. The single-stranded aptamer region in ttsDNA gate situated away from the surface of the Zr-MOF mix , resulting in a natural release of dyes in the absence of PAT. While binding to PAT resulted in target-induced conformational changes that helped form the hairpin structure of the aptamer. This structure hindered the release of dyes from the pores of Zr-MOF mix , thus reducing the fluorescence signals intensity. The stimuli-responsive DNA-gated material provides a platform for PAT analysis under conditions of a low limit of detection (0.871 pg/mL). Furthermore, the excellent specificity and anti-interference of the fluorescent aptasensor make the system suitable for the analysis of apple juice samples. This label-free strategy is cheaper and simper compared with labeled detection, especially for the development of multi-target-detection.
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DOI
PubMed
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2022
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IF 6.47
Kai Shi,Xia An,Yali Du,Zhaoyang Fan,Xu Wu,Xianmei Xie
A series of nickel catalysts supported on Al 2 O 3 that modified with Ce-, Zr-, and Mg-promoter were prepared via a sol-gel method and a subsequent impregnation method for the ethanol steam reforming reaction (ESR). The effect of promoters on the carbon deposition was focused. Compared with Ni/Al 2 O 3 catalyst, the introduction of different promoters decreased the selectivity for CH 2 CH 2 to different extent, especially, Ce-, Mg- containing catalysts completely suppressed the production of CH 2 CH 2 for 30 h tested at 500 °C. And the medium and strong acid sites were confirmed as the major sites for CH 2 CH 2 production. Encapsulation carbon derived from ethylene takes the primary responsibility for carbon deposition, and the formation of metal carbide is the other reason for causing carbon deposition. Among the tested catalysts, Ni/Mg–Al 2 O 3 exhibited a better performance for anti-carbon, which was attributed to the blockage of medium and strong acid sites as well as the high Ni crystallinity .
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Liang Xu,Lei Su,Hongjie Wang,Hongfei Gao,Pengfei Guo,Min Niu,Kang Peng,Lei Zhuang,Zhiwei Dai
Materials with ultralow thermal conductivity and good thermal stability are of great interest in numerous applications such as energy storage and conversion devices, and thermal insulation components. In this work, a family of high-entropy Sm 2 B 2 O 7 (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) oxides with highly disordered cations on the B-site has been synthesized by introducing large atomic-size mismatch, mass and charge disorder. Through tuning the composition, the high-entropy Sm 2 B 2 O 7 oxides can be engineered from pyrochlore to fluorite structure, accompanied with an order-disorder transition. The pyrochlore Sm 2 (Nb 0.2 Sn 0.2 Ti 0.2 Y 0.2 Zr 0.2 ) 2 O 7 and fluorite Sm 2 (Nb 0.2 Ta 0.2 Y 0.2 Yb 0.2 Zr 0.2 ) 2 O 7 exhibit low thermal conductivities of 1.35 W·m −1 ·K −1 and 1.23 W·m −1 ·K −1 , respectively, indicating their good thermal insulation. In addition, the high-entropy fluorite Sm 2 (Nb 0.2 Ta 0.2 Y 0.2 Yb 0.2 Zr 0.2 ) 2 O 7 also shows average thermal expansion coefficient of 10.2 × 10 −6 °C −1 and high-temperature stability even after thermal exposure at 1600 °C in air for 30 h. These results indicate that the high-entropy Sm 2 B 2 O 7 (B=Ti, Zr, Sn, Hf, Y, Yb, Nb, and Ta) can be promising candidates for thermal barrier coatings and thermally insulators.
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高影响因子
Nuclear Engineering and Technology
·
2022
·
IF 2.817
Yan Wang,Jin Wang,Xue Zhang,Nan Li,Junxia Wang,Xiaofeng Liang
Series of unequal quantity Nd/Ce co-doped ceramic nuclear waste forms, (Gd, Nd) 2 (Zr, Ce) 2 O 7 , were prepared to tailor its ordered pyrochlore or disordered fluorite structure. The phase transition, microtopography, and elemental composition of the ceramic samples were systematically investigated, especially the effect of order-disorder structure on the chemical stability. It was confirmed that unequal quantity of Nd/Ce could synchronously replace the Gd/Zr-sites of Gd 2 Zr 2 O 7 . And the phase transition of order-disorder structure could be successfully tailored by regulating the average cationic radius ratio of (Gd, Nd) 2 (Zr, Ce) 2 O 7 series. The elements of Gd, Nd, Zr, and Ce are uniformly distributed in the ordered or disordered structures. The MCC-1 leaching results showed that (Gd, Nd) 2 (Zr, Ce) 2 O 7 pyrochlore ceramic nuclear waste forms had excellent chemical stability, whose elements' normalized leaching rates were as low as 10 −4 -10 −7 g‧m −2 ‧d −1 after 7 days. In particular, the chemical stability of disordered structure was superior to that of ordered structure. It was proposed that the force constant and the closest packing were changed with the structure transformation resulting the chemical stability difference.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
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IF 3.573
Jincheng Mu,Jianfang Liu,Zhenzhen Ran,Muhammad Arif,Min Gao,Chen Wang,Shengfu Ji
MOF-808(Zr) with the coordinated unsaturated (CUS) Zr4+ centers was synthesized by the thermal reflux method, and a series of Au/MOF-808(Zr) catalysts with different Au loading percentages have been prepared by the impregnation–reduction method. The related X-ray diffraction, Fourier transform infrared spectroscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption, Inductively coupled plasma-mass spectrometry, and NH3 temperature-programmed desorption characterizations have been undertaken to understand the structure of catalysts. The catalytic activity in CO2 with aniline/H2 to N-methylation and N-formylation has been studied in a batch reactor. Results show that the MOF-808(Zr) structures in catalysts are of high quality and damage-free. The Au nanoparticles (NPs) are highly dispersed on the surface of the MOF-808(Zr) cage with a mean size of 2–20 nm. Also, the catalysts could catalyze the conversion of CO2 with aniline/H2 to N-methylation and N-formylation products with a high efficiency. With a 3.0 wt % Au/MOF-808(Zr) catalyst, the conversion of aniline is 18.4%, and the selectivity of N-methylaniline is 80.9% and that of N,N-dimethylaniline is 19.1%. The preliminary reaction mechanism and the critical role of CUS were also studied. It is determined that H2 is adsorbed and activated on Au NPs. CO2 is adsorbed on the CUS Zr4+ acidic sites and O2– basic sites. The primary and secondary amines are adsorbed on the CUS Zr4+ acidic sites, where they react with CO2 and H2 to form N-formamide. Subsequently, N-formamide reacts with activated H2 to yield N-methylamine.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
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IF 6.735
Chuanzhi Sun,Hao Liu,Wei Chen,Dezhan Chen,Shuohan Yu,Annai Liu,Lin Dong,Shuai Feng
A series of Sm- and/or Zr-doped MnO x -TiO 2 catalysts were prepared, and the catalysts exhibited better N 2 selectivity and SO 2 resistance than the undoped MnO x -TiO 2 catalyst for the selective catalytic reduction of NO by NH 3 (NH 3 -SCR). The reasons for the good N 2 selectivity and SO 2 resistance of the catalysts were proposed. X-ray photoelectron spectroscopy (XPS) combined with density functional theory (DFT) calculations suggested that electron transfer between the manganese and samarium species by Mn 4+ + Sm 2+ ↔ Mn 3+ + Sm 3+ redox cycles occurred in the Sm-containing catalysts. Furthermore, electron transfer from Sm 2+ to Mn 4+ suppressed electron transfer from NH 3 to Mn 4+ , inhibiting the formation of NH 2 or NH. Thus, the pathway for NH generation was removed, and the reaction of 2NH + 4NO → 3N 2 O + H 2 O was prevented. Consequently, the N 2 selectivity of the NH 3 -SCR reaction was enhanced. In situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) combined with thermogravimetry, differential scanning calorimetry and mass spectrometry (TG-DSC-MS) results revealed that the deposition rate of sulfate species decreases after Sm doping, which was also attributed to the suppressed electron transfer from SO 2 to Mn 4+ , i.e., the oxidation of SO 2 to SO 3 . Thus, the catalysts exhibited better SO 2 resistance.
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高影响因子
ACS Applied Materials & Interfaces
·
2016
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IF 7.145
Lianfang Chen,Junjie Ou,Hongwei Wang,Zhongshan Liu,Mingliang Ye,Hanfa Zou
Although thousands of metal–organic frameworks (MOFs) have been fabricated and widely applied in gas storage/separations, adsorption, catalysis, and so on, few kinds of MOFs have been used as adsorption materials while simultaneously serving as matrixes to analyze small molecules for laser desorption/ionization mass spectrometry (LDI-MS). Herein, a new concept is introduced to design and synthesize MOFs as both adsorption materials and matrixes according to the structure of ligands and common matrixes. The proof of concept design was demonstrated by selection of 2,5-pyridinedicarboxylic acid (PDC) and 2,5-dihydroxyterephthalic acid (DHT) as ligands for synthesis of MOFs. Two Zr(IV)-based MOFs of UiO-66-PDC and UiO-66-(OH)2 were synthesized and applied for the first time as new matrixes for analysis of small molecules by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS). Both of them showed low matrix interferences, high ionization efficiency, and good reproducibility when used as matrixes. A variety of small molecules, including saccharides, amino acids, nucleosides, peptides, alkaline drugs, and natural products, were analyzed. In addition, UiO-66-(OH)2 exhibited potential for application in the quantitative determination of glucose and pyridoxal 5′-phosphate. Furthermore, thanks to its intrinsically large surface area and highly ordered pores, UiO-66-(OH)2 also showed sensitive and specific enrichment of phosphopeptides prior to MS analysis. These results demonstrated that this strategy can be used to efficiently screen tailor-made MOFs as matrixes to analyze small molecules by MALDI-TOF-MS.
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Huadong Fu,Yan Qin,Zhengwei Peng,Jipeng Dou,Zhixiong Huang
Lightweight phenolic matrix composites are highly potential in ablative thermal protective materials for future aerospace vehicles, and hybrid modification is considered as one of effective ways to improve the oxidation and ablation resistance of phenolic matrix. Herein, the co-continuous silica zirconium hybrid phenolic resin (SZRx) was synthesized, which can be used to prepare lightweight ablation resistant aerogel composites by the sol-gel method. The SZRx aerogel showed stable porous structure and excellent hydrophobicity, and the silicon zirconium hybrid greatly improved the high temperature carbon residue and oxidation resistance of phenolic resin. The SZRx aerogel composites also possessed excellent integrated characteristics of heat protection and insulation, with a linear ablation rate as low as 0.032 mm/s and a back temperature below 200 °C. The synergistic effect of silicon and zirconium formed the multiphase ceramic layer (C, SiO 2 , SiC and ZrO 2 ) with the sea-island-like structure on the surface of the composite material, which can effectively resist high-temperature ablation and aerodynamic exfoliation. This can indicate that silicon zirconium dual element hybrid phenolic resin is the highly competitive matrix for lightweight and ablation resistant composite materials.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiaxin Qu,Xueqian Wang,Langlang Wang,Bowen Xu,Ping Ning,Yixing Ma,Yibing Xie,Rui Cao,Qiang Ma
A nonmetallic N-doped Zr/Ti-based catalyst was prepared to investigate the effect of N addition on catalytic performance for carbon disulfide (CS 2 ) hydrolysis. The characterization of the catalyst indicated that doped N atoms were present as interstitial N in the TiO 2 lattice, resulting in an increase in the number of basic sites of the catalyst from 1.64 to 2.37 and from 0.68 to 2.53 for weakly basic and strongly basic sites, respectively. In addition, the doping of N promoted the formation of OH groups, which were favorable for the hydrolysis of CS 2 , from water (H 2 O) adsorbed on the catalyst, thus greatly improving the performance of catalytic CS 2 hydrolysis. However, N doping reduced the amount of chemisorbed oxygen on the catalyst surface from 44.7% to 33.4%, thus decreasing the oxidation reaction of the hydrolysis product H 2 S and improving the stability of the catalyst. CS 2 hydrolysis reaction activity and catalyst lifetime were tested. The experimental results demonstrated that the catalytic CS 2 hydrolysis performance was greatly improved after N doping, and the temperature to obtain 100% conversion was reduced from 180 °C to 130 °C. Selectivity to H 2 S was greatly improved with N-doped catalysts. Furthermore, the resistance of the catalyst to sulfate was improved. Nonmetallic N-doped Zr/Ti-based catalysts offer a new strategy for blast furnace gas desulfurization.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8534-8544
·
IF 3.925
Ruowei Lu,Cuijuan Wang,Yanxia Chen,Lichuan Tan,Peng Wang,Siwen Feng
Adsorption and Fenton catalysis technologies have been widely used to treat wastewater. Herein, Zr-MOF composites are synthesized with Mn-doped magnetic hierarchical porosity and ionic liquid (IL) post-functionalization (MFC@Mn-NH2-UiO-66@IL). The characterization of the composite shows that the MOF we synthesized is laminar and porous, which promotes the adsorption process and subsequent H2O2 decomposition catalysis. Electrostatic interactions, hydrogen bonds, and π–π stacking interactions between [BMIM][PF6] and methylene blue (MB) greatly improve the adsorption performance. Subsequently, H2O2 is rapidly decomposed in a Zr-MOF and Fe3O4 system to produce ˙OH for the oxidative decomposition of MB. Zr plays an electron transfer role in the catalytic reaction. The MFC@Mn-NH2-UiO-66@IL material has a high adsorption capacity for aqueous MB solutions. In combination with the subsequent Fenton-like oxidation reaction, a removal efficiency of 98% is achieved in 90 min. We believe that our work has essential impact in the field of wastewater treatment based on the advantages of the MOF's dual function in degrading pollutants in water.
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高影响因子
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