RSC Advances
·
2016
·Vol. 6
·期 43
·37110-37117
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IF 3.289
Mingjuan Han,Zheng Gu,Chong Chen,Zuowang Wu,Yigen Que,Qiang Wang,Hui Wan,Guofeng Guan
A new, simple and effective strategy to confine dicationic acid ionic liquids (DAILs, 1,4-bis[3-(propyl-3-sulfonate) imidazolium] butane hydrogen sulfate) in the cages of MIL-100(Fe) frameworks was constructed. The target catalyst, defined as MIL-100(Fe)@DAILs, was characterized by XRD, FTIR, SEM, TEM, EA, TGA and N2 adsorption–desorption. Meanwhile, the catalytic activity of the MIL-100(Fe)@DAILs catalyst was evaluated by the esterification reaction with oleic acid and methanol. The results indicated that the DAILs had been effectively encapsulated within the cages of the MIL-100(Fe) frameworks. Moreover, the influence of reaction time, reaction temperature, molar ratio of methanol to oleic acid and catalyst dosage on the conversion of oleic acid was studied by univariate analysis. The conversion of oleic acid decreased from 93.5% to 86.0% when the catalyst was reused five times, which indicated that the target catalyst possessed higher catalytic activity and superior catalytic activity. Finally, an esterification mechanism catalyzed by this novel catalyst was illustrated.
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MOLECULES
·
2017
·Vol. 22
·期 6
·920
·
IF 2.861
Youxun Liu,Yuanyuan Geng,Mingyang Yan,Juan Huang
The successful encapsulation of 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS), a well-known laccase mediator, within a mesoporous metal-organic framework sample (i.e., MIL-100(Fe)) was achieved using a one-pot hydrothermal synthetic method. The as-prepared ABTS@MIL-100(Fe) was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, nitrogen sorption, and cyclic voltammetry (CV). Our ABTS@MIL-100(Fe)-based electrode exhibited an excellent electrochemical response, indicating that MIL-100(Fe) provides an appropriate microenvironment for the immobilization and electroactivity of ABTS molecules. ABTS@MIL-100(Fe) was then evaluated as an immobilized laccase mediator for dye removal using indigo carmine (IC) as a model dye. Through the application of laccase in combination with a free (ABTS) or immobilized (ABTS@MIL-100(Fe)) mediator, decolorization yields of 95% and 94%, respectively, were obtained for IC after 50 min. In addition, following seven reuse cycles of ABTS@MIL-100(Fe) for dye treatment, a decolorization yield of 74% was obtained. Dye decolorization occurred through the breakdown of the chromophoric group by the Laccase/ABTS@MIL-100(Fe) system, and a catalytic mechanism was proposed. We therefore expect that the stability, reusability, and validity of ABTS@MIL-100(Fe) as a laccase mediator potentially render it a promising tool for dye removal, in addition to reducing the high running costs and potential toxicity associated with synthetic mediators.Keywords:laccase;ABTS;metal-organic framework;mediator;decolorization
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2016
·
IF 1.207
Zhiliang Zhang,Guangquan Wang,Yong Nie,Jianbing Ji
Hydrodynamic cavitation, a newly developed process intensification technique, has demonstrated immense potential for intensifying diverse physical and chemical processes. In this study, hydrodynamic cavitation was explored as an efficient method for the formation of sub-100 nm oil-in-water (O/W) emulsions with high stability. O/W emulsion with an average droplet size of 27 nm was successfully prepared. The average droplet size of O/W emulsions decreased with the increase of the inlet pressure, number of cavitation passes and surfactant concentration. The formed emulsion exhibited admirable physical stability during 8 months. Moreover, the hydrodynamic cavitation method can be generalized to fabricate large varieties of O/W emulsions, which showed great potential for large-scale formation of O/W emulsions with lower energy consumption.
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Nanoscale
·
2024
·Vol. 16
·期 6
·3034-3042
·
IF 5.8
Haoyang Wu,Zhili Wang,Benqiang Tian,Yaping Li,Zheng Chang,Yun Kuang,Xiaoming Sun
Electrocatalytic CO2 reduction (ECR) to high value-added chemicals is an excellent method to attenuate the impact of greenhouse effect caused by CO2. At the same time, multicarbon products (C2+) get extensive attention in view of their relatively high energy density and market price. At present, Cu is an important metal electrocatalyst to convert CO2 into multicarbon products (e.g. ethylene, ethanol, and n-propanol); however, its poor selectivity impedes its practical application. It is well-known that the Cu(100) crystal facet can enhance the selectivity toward multicarbon products among different Cu crystal facets. Herein, the Cu nanoparticles were firstly prepared using the inductive effect of different gases (CO2, CO, Ar, N2, and air) during the Cu electrodeposition processes, in which the CO2-induced Cu catalyst (Cu-CO2) showed the largest normalized content of the Cu(100) crystal facet and the highest C2+ faradaic efficiency of 69% at a current density of 80 mA cm−2 in ECR. Subsequently, the different CO2 pressures during the Cu electrodepositions were studied to reveal the optimal CO2 pressure in the CO2-induced Cu synthesis for improved Cu(100) content as well as C2+ faradaic efficiency. Finally, density functional theory (DFT) calculations confirmed that CO2 molecules preferred to get adsorbed on the Cu(100) crystal facet, which resulted in not only the presence of dominant Cu(100) during the CO2-induced Cu synthesis but also the good electrocatalytic performance in ECR.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 26
·16043-16051
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IF 10.7
Keying Su,Shan Yang,Yulu Zhu,Yujia Liang,Yawen Tang,Xiaoyu Qiu
High-entropy alloy (HEA) nanoparticles have been recognized as one kind of efficient electro-catalyst for water splitting. However, their higher catalytic activity is restrained by the difficulty in precisely shaping the HEAs into ordered facets and fully exposed surface structures. Herein, we report a seed-mediated conformal growth and partial etching method for the controlled synthesis of PtIrRuRhPd HEA cubic nanocages (CNCs), which feature the ordered {100} facets and ultrathin shells of five atomic layers. The slow injection of a PtIrRuRh layer on Pd nanocubes and the subsequent capture of dissociative Pd atoms in the etching step are responsible for the formation of nearly equimolar PtIrRuRhPd HEAs. Due to the synergistic effects derived from the multicomponent high-entropy effects, the ordered (100) facets, and the ultrathin feature, the PtIrRuRhPd HEA CNCs exhibit significantly high electro-catalytic activities for hydrogen and oxygen evolution reactions in an acidic medium, with overpotentials of 20 mV and 272 mV at 10 mA cm−2 (η10), respectively. As electrodes for a water electrolyzer, the PtIrRuRhPd HEA CNCs afford an η10 as low as 196 mV, together with superior long-term durability for 200 000 s.
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Advanced Science
·
2025
·
IF 14.1
Guannan Zhang,Zhao Sun,Zhuofei Gan,Chuwei Liang,Liyang Chen,Hongbo Mo,Yuanzhi Jiang,Mingjian Yuan,Aleksandra B. Djurišić,Ji Tae Kim,Wen-Di Li
Halide perovskite single crystals have demonstrated enormous potential for next-generation integrated optoelectronic devices. However, there is a lack of a facile method to realize the controllable growth of large-scale, high-quality, and high-resolution perovskite single crystal arrays on diverse types of substrates, which hinders their application in practical scenarios. Here, a one-step wettability-guided blade coating approach is reported for the rapid in situ crystallization of large-scale, multicolor, and sub-100 nm perovskite single-crystal arrays in the ambient environment. By this strategy, the physical dimensions of perovskite single crystals can be precisely regulated from 90 to 260 nm, with a size variation coefficient < 10% and an area of over 900 mm 2 . All three typicalhalogen perovskites for multi-color luminescence, CsPbX 3 (X = Cl, Br, I) and their mixtures (Cl/Br or Br/I systems), are appliable to this fabrication process through the demonstration of complex RGB patterns with remarkable photoluminescence properties. Moreover, various rigid substrates such as silicon oxide (SiO 2 ), silicon (Si), and glass can also be used to construct the wettability-constrast templates where perovskite crystal nucleate and grow. After that, the perovskite single-crystal arrays or complex patterns can be transferred onto flexible substrates, for instance, COC. This method combines convenient solution processing with conventional photolithography to prepare the high-resolution, large-area, and superior-quality perovskite single crystal arrays in a high-throughput manner, showing great potential in the integration of perovskite nano-optoelectronic devices and chips.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 10
·3417-3424
·
IF 4.099
Huairu Tian,Jun Peng,Qiuzheng Du,Xuanhong Hui,Hua He
A novel, rapid and simple method is described for the synthesis of magnetic MIL-100(Fe) with novel Fe3O4 morphology, which significantly improved the sustainability of conventional fabrication processes in several aspects. The magnetic MOFs were prepared (i) in one pot (instead of multiple steps), (ii) at room temperature (instead of temperatures over 150 °C), (iii) within a few hours with excellent yield (instead of in few days with low productivity) and (iv) in the absence of any corrosive inorganic acid and organic reagent. The materials were tested in the industrially demanded photocatalytic and photo-Fenton degradation of sodium sulfadiazine. The degradation results indicated that the Fe3O4 nanorods could accelerate the catalytic efficiency. The catalyst would be of potential application due to its stable catalytic activity in repeated reaction cycles and no need for regeneration. Therefore, the MIL-100(Fe) and magnetic MIL-100(Fe) proposed in this study are ideal catalysts for the heterogeneous degradation of sodium sulfadiazine.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·
IF 3.582
Zuohua Liu,Yujie Zheng,Tingting Gao,Jing Zhang,Xuefeng Sun,Guowei Zhou
In this study, anatase TiO 2 nanorods with exposed high-energy {100} and {001} facets and low-energy {101} facets were fabricated in the presence of surfactants cetyltrimethylammonium bromide , didecyldimethylammonium bromide, and ammonia via a facile hydrothermal method without the erosive reagent hydrofluoric acid . The particle size and morphology were mainly tuned by regulating the hydrothermal temperature. When the temperature was increased from 150 °C to 180 °C and 200 °C, the length of the nanorods decreased from 700-1000 nm to 400–500 nm and 100–200 nm, respectively. Concurrently, the edges and tops of the truncated tetragonal pyramid of the TiO 2 nanorods became blurry and flattened. The synthesized typical TiO 2 nanorods were then used as photocatalysts , and their performance during the direct generation of H 2 from water was evaluated. The TiO 2 nanorods obtained at 150 °C successfully produced high amounts of H 2 evolution (281.36 μmol) in the presence of methanol as a sacrificial agent under ultraviolet light irradiation for 4 h. The outstanding photocatalytic activity of the nanorods was mainly ascribed to the formation of surface heterojunctions in the edges and corners between adjacent high-energy {001} or {100} facets and low-energy {101} facets. The formed heterojunctions could facilitate charge separation through preferential carrier flow toward the specific facets.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yue Xiao,Haodong Huang,Shangpu Zhuang,Dong Yang
Metal oxide cluster MOF nodes are a good platform to understand the reactivities and catalysis. MIL-96, MIL-100 and MIL-110 are drastically different in their node structures. Following our previous reported results for MIL-100, we report the modified synthesis and characterization of the node sites of MIL-110 and MIL-96 and their catalytic sites by using methanol dehydration as probe reaction. We show that these MOFs can be synthesized from the same solution by adding various amounts of formic acid as modulator. Herein, the chemistry of hydroxyl, formate and methoxy groups were used to probe the three MOFs’ node sites. IR data show the bonding structures of these ligands are highly diverse, with reactivities and flexibilities depending on node sites. We identified terminal OH group and various µ 2 -OH groups in single, paired or hydrogen bonded modes on the MOF nodes. Formate ligands were introduced to the node sites during the synthesis or by a post treatment in formic acid/DMF solution. Surprisingly, the bonding modes of formate ligands on Al 3 (OH) 3 node structure of MIL-96 can be reversibly switched between monodentate and bidentate through a process induced by water molecules. Further, methoxy ligands—likely to be the intermediate for catalytic reaction—were also observed on the node sites under methanol dehydration conditions at 250 ℃. The activities of MIL-100 and MIL-96 for methanol dehydration determined by TOF per node were similar, both approximately 3-fold higher than that of MIL-110. The data suggests that catalytic sites incorporate adjacent vacancy and defect node sites, which constitute a minority among all observed MOF node sites. We foresee the opportunities in expanding the chemistry and understanding into other MOFs with metal oxide cluster nodes.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Tianyi Huang,Jiajia Wu,Yongqi Pan,Zhiyuan Yu,Fangyu Zhao,Shafqat Ullah,Yang Xu,Yong Chen,Zhehao Sun,Zongyou Yin,Qiangqiang Xue,Sibudjing Kawi,Shuliang Lu,Yujun Wang,Guangsheng Luo
The hydrogenation of the C=C bond in α-β unsaturated aldehydes faces substantial difficulties due to the steric hindrance and the conjugation effects of macromolecular unsaturated aldehydes. Herein, we introduce a novel approach to prepare nanosheet-structured Ni-Al 2 O 3 catalysts featuring exposed {100} crystal planes and hydroxyl groups, utilizing a microfluidic system to easily control crystal plane growth achieve support modification. In-situ characterizations and DFT calculations reveal that the exposed {100} crystal plane, a strong metal-support interaction (SMSI) promotes electron transfer of Ni and significantly reducing the C=C hydrogenation energy barrier from 3.12 eV to 1.79 eV. The hydroxyl environment facilitates effective adsorption of the C=O bond, accelerating the reaction and enabling rapid desorption of the product. Under modified reaction conditions for the preparation of 2-ethylhexanol, the catalyst still achieved a yield of 99.9%. This simple method of support modification enables rapid large-scale preparation, possessing significant potential for industrial applications.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zixia Tang,Hong Tao,Xiao Wang,Lu Chen,Chi Song,Guanhong Lu,Xiaofeng Xie,Jing Sun
The implantation of metal nanoparticles (MNPs) into metal–organic framework (MOF) hosts is a promising means to prepare high-performance photocatalysts for the degradation of gas pollutants. However, the uniform encapsulation of MNPs in MOFs is still challenging. Herein, a facile “quasi-in situ” encapsulation method is proposed by utilizing the spatial confinement effect of the colloidal network formed during the synthesis of the MIL-100(Fe) monolith [noted as m-MIL-100(Fe)]. Highly dispersed Ag NPs with an average diameter of ∼2 nm are encapsulated in the MIL-100(Fe) monolith to form a unique “watermelon-seed” structure, which ensures the large contact area between the two components and protects Ag NPs from being oxidized. The fast charge transfer between m-MIL-100(Fe) and Ag NPs enables the spatial separation of electron–hole pairs and promotes the generation of oxidative radicals. Compared with pristine m-MIL-100(Fe), the 0.2 wt % Ag@m-MIL-100(Fe) composite shows obviously enhanced photodegradation efficiencies for flowing o-xylene under both xenon (∼97%) and visible light (∼80.0%) with high stability. This work not only provides a promising Ag@m-MIL-100(Fe) material for eliminating air pollutants but also gives a versatile means for the design and synthesis of nanoparticles@MOFs composites with desired performance.
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PROCESS BIOCHEMISTRY
·
2021
·
IF 3.757
Kun Xiao,Rennv Wang,Congyang Liu,Meini Wang,Wei Dong,Tao Pan
PAH biodegradation aided by surfactants and cyclodextrins has been widely studied because the former's micelles and the latter's hydrophobic cavities can increase the apparent solubility of PAHs. In this work, the effects of Triton X-100 (TX-100) and β-cyclodextrin (β-CD) on the bioavailability and biodegradation of phenanthrene (PHE) were investigated. The degrading microorganism used was Moraxella osloensis CFP312, a new strain screened from polluted soil and could form biofilms on crystalline PHE. At the same concentrations, β-CD solubilized less PHE than TX-100 but promoted PHE biodegradation. The two solubilizers had almost no different effects on CFP312 hydrophobicity; however, β-CD significantly eluted fewer cells from biofilms on crystalline PHE than TX-100. Microscopy observation revealed that the residual structure of the biofilm treated with β-CD was more complete than that of the biofilm treated with TX-100. This effect is beneficial to the function of biofilms and conducive to mass transfer from the exposed area in the crystalline PHE to the aqueous phase. Although TX-100 and β-CD could enhance the mass transfer of PHE to the aqueous phase, the latter significantly improved the bioavailability and biodegradation of PHE mainly because its solubilization was accompanied by easy desorption and retention of the biofilm functional integrity.
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