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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

One-step synthesis of magnetically recoverable AgCl/Fe3O4@MIL-100(Fe) for high-performance photocatalysis

Jun Liu,Hui Wang,Wen-Yao Zhu,Heng-Xue Xie,Xin Li,Wen-Juan Li,Ge Bai,Meng-Jie Chang,Xiao-Jiao Chai,Hui-Ling Du,Shi-Jie Song

We present a novel method to facilely prepare magnetically recoverable AgCl/Fe 3 O 4 @MIL-100(Fe) (ACFM) nanostructures for photocatalytic degradation of rhodamine B (RhB). The ACFM was directly prepared via a simple successive ionic layer adsorption and reaction (SILAR) deposition of MIL-100(Fe) on solvothermal synthesized Ag/Fe 3 O 4 nanoparticles , in which process Ag was completely oxidized into AgCl concurrent with the formation of MIL-100(Fe). The ACFM prepared with 15 SILAR cycles exhibits 92.9% efficiency towards photodegrading RhB within 30 min under visible light illumination, which is higher than that of the individual structure of AgCl/Fe 3 O 4 , Ag/Fe 3 O 4 @MIL-100(Fe) or Fe 3 O 4 @MIL-100(Fe). The remarkably enhanced photocatalytic performance is attributed to the abundant active sites and sufficient visible light response of MIL-100(Fe), as well as effective charge separation at the heterojunction interface between AgCl and MIL-100(Fe). Furthermore, the obtained ACFM can be quickly separated from the pollutant solution with a magnet and possesses good stability for recycling photocatalysis . In light of the study, the ACFM nanostructures are believed to be applied as promising photocatalysts for practical applications.

CAS / MDL: 554-95-0
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DESALINATION · 2022 · IF 11.211

Boron adsorption and isotopic separation from water by isostructural metal-organic frameworks MIL-100(M)

Xiangyunxiu Meng,Ruiwen Luo,Guijie Guo,Yulin Li,Hui Fang,Peng Bai,Jiafei Lyu,Xianghai Guo

Adsorption has been expected to be promising for boron-containing water treatment , boron resources recovery and boron isotopic separation. Although metal-organic frameworks have been demonstrated to be potential adsorbent candidates, in-depth investigation of the structure-performance relationship remains insufficient. Herein, the performance and mechanism of boron adsorption and isotopic separation were systematically investigated with isostructural MOFs. Six isomorphic MIL-100(M) materials with metal species from the third main group (Al, Ga and In) and the fourth period (Sc, Cr and Fe) were solvothermally synthesized as boron adsorbents. Superior boron isotopic separation factors ( S ) with 10 B preference and comparable boron adsorption capacity ( Q ) were observed through batch boron adsorption experiments, where MIL-100(Al) exhibited the highest S of 1.618 and MIL-100(Sc) achieved the largest Q of 8.74 g-B/mol-MOF. A high correlation between metal atomic radius and performance was revealed and a plausible mechanism was proposed for boron adsorption and isotopic separation involving the important role of the metal center through post-adsorption characterization. This study will pave the way for designing boron adsorbents with improved properties and promote the efficient utilization of boron resources in water.

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Journal of Advanced Dielectrics · 2022 · IF 0

Piezoelectric, ferroelectric and pyroelectric properties of (100 − x)Pb(Mg1/3Nb2/3)O3 − xPbTiO3 ceramics

Chuan Chen,Yan Wang,Jiajiu Li,Chaofeng Wu,Guanrong Yang

A series of (100 − x ) Pb(Mg 1 / 3 Nb 2 / 3 ) O 3 − x PbTiO 3 (PMN − x PT, x = 24, 25, 26) ceramics were prepared by solid-state reaction technique using MgNb 2 O 6 precursor. The results of the detailed characterizations reveal that the content of PT has negligible influence on the grain size, and all samples possess the perovskite structure. As the PT content increases, the samples changed from the normal ferroelectric phase to the ergodic relaxor state at room temperature. As a result, PMN– x PT ceramics are endowed with electro-strain of 0.08% at a relatively low electric field of 2 kV/mm, and effective piezoelectric coefficient of 320 pm/V was obtained. Simultaneously, the PMN– x PT ceramics have exceptional pyroelectric performance, exhibiting a high pyroelectric coefficient p ∼ 5.5 – 6.3 × 10 − 8 C⋅cm − 2 ⋅K − 1 . This study demonstrates the great potential of PMN– x PT for piezoelectric and pyroelectric device applications.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Bi-Eu bimetallic catalysts enabling ultrastable electroreduction of CO2 with a ∼ 100% formate Faradaic efficiency

Jiaying Yan,Yayu Guan,Barbara Marchetti,Yuyu Liu,Fanghua Ning,Jin Yi,Xiao-Dong Zhou

Electrochemical reduction of CO 2 (ERCO 2 ) is an effective way to convert CO 2 into useful chemical products. However, most catalysts used for ERCO 2 show poor selectivity and stability. Here, we design a Bi 8 Eu 1 bimetallic catalyst, which exhibits both excellent stability (>400 h) and Faradaic efficiency for formate production (∼100% at − 0.89 V RHE ). Moreover, high Faradaic efficiency (>97%) is observed over a wide potential window (from − 0.89 V RHE to − 1.19 V RHE ). In a flow-cell, the Bi 8 Eu 1 catalyst shows an ultra-high current density of 250 mA cm −2 at − 0.77 V RHE . Density functional theory calculations indicate that the Bi-Eu interactions activate the Bi sites for strongly stabilizing *OCHO intermediates, thus promoting the conversion of CO 2 to formate. This work provides insights into the design of excellent electrocatalysts for ERCO 2 with improved activity and durability.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Highly dispersed nickel site catalysts for diluted CO2 photoreduction to CO with nearly 100% selectivity

Shujie Liang,Xiaohui Zhong,Zuqi Zhong,Hong Deng,Wai-Yeung Wong

Photoconversion of CO 2 into value-added fuels has aroused widespread interest; however, this process is significantly limited by the inefficient thermodynamics and sluggish reaction dynamics in the diluted CO 2 . To circumvent these obstacles, we design a bipyridine-based polyimide polymer for anchoring single Ni site for diluted CO 2 photoreduction. The desired Ni single atomic catalysts achieve high generation activity of ∼ 2262 μmol/h with apparent quantum efficiency (A.Q.E.) of 0.20% for CO 2 -to-CO in 0.1 atm CO 2 pressure. No measurable H 2 is produced in the catalytic process, affording nearly 100% CO selectivity over water splitting. This superior activity and selectivity outperform most previous atomical catalysts. Mechanistic analyses elucidate that the highly dispersed Ni atoms act as active sites for effective CO 2 binding and activation, and stabilize the rate-determining step of intermediates for CO generation. This work discloses the relationship between catalytic properties and single atoms for efficient solar-driven diluted CO 2 reduction.

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Journal of the American Chemical Society · 2020 · IF 14.612

Monodisperse CdSe Quantum Dots Encased in Six (100) Facets via Ligand-Controlled Nucleation and Growth

Liulin Lv,Jiongzhao Li,Yonghong Wang,Yufei Shu,Xiaogang Peng

Zinc-blende CdSe quantum dots (QDs) encased in six equal (100) facets are synthesized in a noncoordinating solvent. Their monodispersed size, unique facet structure, and single crystallinity render the narrowest ensemble photoluminescence for CdSe QDs (full width at half-maximum being 52 meV). The nucleation stage can selectively form small-size CdSe QDs (≤3 nm) as seeds suited for the growth of cube-shaped QDs by reducing the concentration of cadmium carboxylates (Cd(RCOO)2) as the sole source of ligands. While resulting in poorly controlled nucleation, chloride-ion ligands introduced in the form of soluble CdClx(RCOO)1–x (x = 0.1∼0.2) would thermodynamically stabilize the cadmium-terminated (100) facets yet kinetically accelerate the deposition of selenium ions onto the (100) facets. Results suggest that it is fully feasible to synthesize QDs simultaneously with monodisperse size and surface structure through ligand-controlled nucleation and growth.

CAS / MDL: 7647-14-5
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ACS Applied Nano Materials · 2021 · IF 5.097

MIL-100(Fe) Metal–Organic Framework Nanospheres Embedded in Graphene Matrixes for Xanthine Fluorescence Sensing

Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha

Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.

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RENEWABLE ENERGY · 2021 · IF 8.001

Carbonized MIL−100(Fe) used as support for recyclable solid acid synthesis for biodiesel production

Hui Li,Junchi Wang,Xiaoling Ma,Yangyang Wang,Guoning Li,Min Guo,Ping Cui,Wanpeng Lu,Shoujun Zhou,Mingzhi Yu

Solid catalyst loss is inevitable by using the traditional separation methods of centrifugation or filtration. To this end, the carbonized MIL−100(Fe) is used to support ammonium sulfate ((NH 4 ) 2 SO 4 ) for synthesizing magnetic solid acid on the purpose of biodiesel production . Influence of preparation factors of loading amount, activation temperature, and activation time on catalytic activity are initially evaluated. With that, the prepared catalyst (CIS) is comprehensively investigated to obtain the optimal esterification parameters for biodiesel production . Moreover, characterizations of TG, XRD, BET, SEM, EDS, FTIR, py−FTIR, VSM, XPS, and Hammett indicator are conducted to elucidate the structure−function relationship between physicochemical property and catalytic activity . Results indicated the CIS is a superparamagnetism material with the saturated magnetism of 22 emu/g, which could be easily recovered from mixture with external magnet. Furthermore, the maximum conversion of 95.68% is obtained with mild conditions: molar ratio of methanol/oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C for 2 h. Negligible impact is detected for CIS with presence of 5 wt% water content, even with 20 wt% water content, the conversion of 85.88% is still achieved.

CAS / MDL: 554-95-0
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CATALYSIS COMMUNICATIONS · 2017 · IF 3.33

Glycol assisted synthesis of MIL-100(Fe) nanospheres for photocatalytic oxidation of benzene to phenol

Bo Xu,Zhiming Chen,Bing Han,Cuncheng Li

This work presents MIL-100(Fe) nanoparticles synthesized using glycol with uniform size and morphology. This is the first report of nanoscale MOFs material synthesized using glycol. The MIL-100(Fe) particles have been characterized by SEM, TEM, XRD and the results indicate that the MOFs particles show monodispersed nanospherical morphology. Photocatalytic study reveals that the MIL-100(Fe) nanospheres exhibit good oxidation ability of benzene to phenol under visible light irradiation with high selectivity.

CAS / MDL: 10060-10-3 554-95-0
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Feasible defect and hydrophobic modification of MIL-100(Cr) for efficient toluene removal from air

Yong Fu,Pengyi Zhang,Xianjie Wang

We developed a feasible strategy to obtain the defective MIL-100(Cr) (De-M) via doping 3,5-pyridinedicarboxylate and subsequently loaded polydivinylbenzene (PDVB) by thermal deposition to obtain a hydrophobic MOFs composite (De-M@PDVB). De-M 10 (10 % defective ligand/total ligands) exhibited excellent performance for the capture of toluene due to uniform particle size, high specific surface area and pore volume. Subsequent thermal deposition with PDVB further increased the hydrophobicity, as-obtained De-M 10 @PDVB in the dynamic adsorption experiment showed about 2 and 1.5 time adsorption capacity as that of primary MIL-100(Cr) and De-M 10 under 50 % RH at 298 K. In addition, the toluene uptake of De-M 10 @PDVB (0.95, 298 K) in static adsorption experiments was 1320 mg/g, much higher than many reported MOFs. Furthermore, De-M 10 @PDVB could be regenerated at 378 K, demonstrating its excellent regenerability at low temperature. The adsorption mechanism of toluene on De-M 10 @PDVB could be attribute to the π-π stacking interaction between the benzene ring of toluene with H 3 BTC and adsorption sites offered by the incorporation of H 2 DL in the framework of MIL-100(Cr) according to XPS analysis. Our finding provided a novel strategy by constructing defective MIL-100(Cr) and introducing PDVB to enhance efficient adsorption for toluene capture even in humid air.

CAS / MDL: 78-67-1
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ChemCatChem · 2024 · IF 3.8

Generation of Reactive Oxygen Species on MIL-100(Fe)/TiO2 Driven by Mild Natural Light

Chengzhuo Yu,Jin Xu,Yarui Wang,Silong Wang,Li Xiong,Fanglan Geng,Zesen Shang,Huasheng Wu,Jitao Lv,Lixia Zhao,Yawei Wang

Graphical Untill now, reactive oxygen species (ROS) are difficult to generate in the natural light conditions, since most photocatalysts require external strong stimuli. We surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. The ROS generation patterns and mechanism of MIL-100(Fe)/TiO 2 was revealed by chemiluminescence (CL) and density functional theory (DFT). Reactive oxygen species (ROS), as one kind of the most highly oxidizing oxidants, are difficult to generate and utilize in the natural light conditions, since many materials require external strong stimuli for ROS release to be effective as pollutant degradation or biocide. In this work, we surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. Then ROS generation patterns and mechanism was revealed by chemiluminescence (CL) and density functional theory (DFT). Meanwhile, rhodamine B (RhB) can also be removed by MIL-100(Fe)/TiO 2 under natural light, which further evidence the ROS generation under the natural light. This work provides a new direction for spontaneously generating ROS releasing without external strong stimuli and has the broad potential applications in the field of pollutant degradation or antimicrobials under natural conditions.

CAS / MDL: 67-43-6 98-00-0
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ANALYST · 2017 ·Vol. 143 ·期 2 ·409-414 · IF 3.885

Ultra-facile and rapid colorimetric detection of Cu2+ with branched polyethylenimine in 100% aqueous solution

Hong Shao,Yadan Ding,Xia Hong,Yichun Liu

The detection of copper ion (Cu2+) has become a long-term and arduous task in the field of environmental monitoring and human health. Current methods based on branched polyethylenimine (BPEI) for the detection of Cu2+ more or less suffer from being time-consuming and having a high cost or complex surface modifications. Herein, an ultra-facile and rapid colorimetric method was explored to detect Cu2+ in 100% aqueous solution by a direct format using only BPEI. Cu2+ could be captured by BPEI and form BPEI–Cu2+ complexes, which resulted in a color change from colorless to blue within 5 s, associated with the strong absorption peak at 278 nm. The lower the molecular weight and the concentration of BPEI are, the lower the detection limit is. When the molecular weight and the concentration of BPEI were 600 and 21.5 mg L−1, respectively, the detection limit was calculated to be 1.21 μM, and the linear range was 2 μM to 50 μM. Besides, BPEI also had an excellent selectivity toward Cu2+. This ultra-facile, rapid and inexpensive method offers great potential for various applications in biomedicine, environmental protection, food safety and so on.

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