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CHEMOSPHERE · 2021 · IF 7.086

Hollow ZSM-5 zeolite encapsulating Pt nanoparticles: Cage-confinement effects for the enhanced catalytic oxidation of benzene

Jian Tian,Kok Bing Tan,Yichen Liao,Daohua Sun,Qingbiao Li

A zeolitic cage was introduced and rationally fabricated by encapsulating Pt nanoparticles (NPs) in hollow ZSM-5, a nanomaterial with a cavity and porous shell, for efficient catalytic oxidation of benzene. The structure and formation of the zeolitic cage were systematically investigated and characterized using transmission electron microscopy , nitrogen sorption investigations, X-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy , and X-ray diffraction. The obtained hollow 0.2 Pt@ZSM-5 exhibited a comparable low-temperature catalytic activity with 0.5Pt/ZSM-5 with T 90 value of 178 °C. Various characterization techniques combined with adsorption experiments uncover the tremendous role of the zeolitic cage in the catalytic activity toward benzene oxidation. The porous shell prevented benzene dilution and the acidity originating from the hollow interior of ZSM-5 promoted the storage of benzene, thereby forming a high local concentration of benzene around Pt NPs, resulting in excellent catalytic performance. These findings provide valuable insights into the rational design of efficient catalysts for the catalytic oxidation of volatile organic compounds.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Molecular Catalysis · 2023 · IF 4.6

Effective Synergistic Hafnium-Aluminum Bimetallic Oxides catalysts for the Synthesis of 5-Hydroxymethylfurfural from Glucose and Fructose

Congcong Zhao,Niuniu Zhu,Guo Qiu,Manyu Zhang,Hongyu Tian

5-Hydroxymethylfurfural (5-HMF) is considered as a bridge connecting biomass and petrochemical products with excellent application potential and market prospects. In this work, a series of hafnium-aluminum bimetallic oxide (Al-HfO x ) catalysts were synthesized with the coprecipitation method, possessing outstanding catalytic effect in the conversion of glucose or fructose to 5-HMF. 5-HMF yield of 49.31% was acquired from glucose in a methyl isobutyl ketone (MIBK)/saturated salt water (SSW) biphasic solvent at 170 ℃ after 2 h. When fructose was the substrate, 5-HMF yield was 74.85% in DMSO at 150 ℃ after 75 min. In addition, the reaction mechanism was speculated that the isomerization process could be promoted by the synergistic effects of aluminum and hafnium species, in which Hf-OH and Al-OH groups, and Hf active sites served as Brønsted and Lewis acidic sites, respectively. After at least four cycles, there was no remarkable wastage in the catalytic activity of Al-HfO x . This paper offers a prospective catalytic strategy for heterogeneous bimetallic oxide catalysts used in the effective conversion of carbohydrates to 5-HMF.

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Frontiers in Bioscience-Landmark · 2023 ·Vol. 28 ·期 7 ·139 · IF 3.1

HnRNP A1 Suppresses the Odontogenic Differentiation and the Inclusion of RUNX2 Exon 5 of Dental Mesenchymal Cells

Yanan Zhang,Junjun Huang,Lingyan Yan,Rong Jia,Jihua Guo

Background: RUNX2 (Runt-related transcription factor 2) acts as a key regulator in the odontogenic differentiation of human dental pulp stem cells (hDPSCs). Moreover, the inclusion of exon 5 is important for RUNX2 function. Our previous study showed that Y-Box Binding Protein 1 (YBX1) promoted RUNX2 exon 5 inclusion and mineralization of hDPSCs. However, the regulatory mechanism of RUNX2 exon 5 alternative splicing needed further exploration. Methods: The expression level of heterogeneous nuclear ribonucleoprotein A1 (hnRNP A1) during the odontogenic differentiation of hDPSCs was analyzed by RT-PCR and Western blot. The roles of hnRNP A1 in the alternative splicing of RUNX2 exon 5 and the odontogenic differentiation of dental mesenchymal cells were analyzed by gain- and loss-of-function experiments. Results: Surprisingly, we found an alternative splicing factor, hnRNP A1, which had an opposite role to YBX1 in regulating RUNX2 exon 5 inclusion and odontogenic differentiation of hDPSCs. Through gain- and loss-of-function assay, we found that hnRNP A1 suppressed the inclusion of RUNX2 exon 5, resulting in the inhibition of odontoblastic differentiation. The overexpression of hnRNP A1 can inhibit the expression of ALP (alkaline phosphatase) and OCN (osteocalcin), and the formation of mineralized nodules during the odontogenic differentiation of both hDPSCs and mouse dental papilla cells (mDPCs), whereas the opposite results were obtained with an hnRNP A1 knockdown preparation. Conclusions: The present study indicated that hnRNP A1 suppressed RUNX2 exon 5 inclusion and reduced the odontogenic differentiation ability of hDPSCs and mDPCs.

CAS / MDL: 123-03-5
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Catalysts · 2023 ·Vol. 13 ·期 4 ·776 · IF 3.9

Discrete Au1(0) Stabilized by 15-Crown-5 for High-Efficiency Catalytic Reduction of Nitrophenol and Nitroaniline

Xing Shen,Kairui Liu

Single-atom catalysts (SACs) have been synthesized using a variety of methods in recent years, and they have shown excellent catalytic activities. However, metal atoms show a high tendency to agglomerate in liquid media, making the single atom synthesis more difficult in liquid media. The synthesis of such metal single-atom catalysts that do not have strong ligand coordination is rarely reported in the literature. Herein, we report the facile synthesis of monodispersed Au atoms (Au1) through the reduction in HAuCl4in 15-crown-5. The complete reduction in HAuCl4was confirmed through UV-Vis spectroscopy. In addition, the Au was found in a zero valence state after reduction, which was confirmed through XPS and XANES results. Moreover, the dispersion of Au was confirmed as a single atom (Au1) through transmission electron microscopy and spherical aberration electron microscopy. The possible structure of this catalyst was proposed by matching the EXAFS results with the structure of Au1@15-crown-5 as -(OC2H4O)-AuCl2H2. The Au1@15-crown-5 showed high activity (TOF as high as 22,075) in the reduction in nitrophenol and nitroaniline to aminophenol and phenylenediamine by sodium borohydride. Because of the monodispersion of Au atoms, its performance is much better than noble nanoparticles and non-precious metal catalysts.Keywords:gold;single atom;nitroaromatic compounds reduction;catalysis

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Energies · 2021 ·Vol. 15 ·期 1 ·53 · IF 3.004

Mechanistic Insights into Hydrodeoxygenation of Acetone over Mo/HZSM-5 Bifunctional Catalyst for the Production of Hydrocarbons

Kai Miao,Tan Li,Jing Su,Cong Wang,Kaige Wang

Catalytic hydropyrolysis via the introduction of external hydrogen into catalytic pyrolysis process using hydrodeoxygenation catalysts is one of the major approaches of bio-oil upgrading. In this study, hydrodeoxygenation of acetone over Mo/HZSM-5 and HZSM-5 were investigated with focus on the influence of hydrogen pressure and catalyst deactivation. It is found that doped MoO3could prolong the catalyst activity due to the suppression of coke formation. The influence of hydrogen pressure on catalytic HDO of acetone was further studied. Hydrogen pressure of 30 bar effectively prolonged catalyst activity while decreased the coke deposition over catalyst. The coke formation over the HZSM-5 and Mo/HZSM-5 under 30 bar hydrogen pressure decreased 66% and 83%, respectively, compared to that under atmospheric hydrogen pressure. Compared to the test with the HZSM-5, 35% higher yield of aliphatics and 60% lower coke were obtained from the Mo/HZSM-5 under 30 bar hydrogen pressure. Characterization of the spent Mo/HZSM-5 catalyst revealed the deactivation was mainly due to the carbon deposition blocking the micropores and Bronsted acid sites. Mo/HZSM-5 was proved to be potentially enhanced production of hydrocarbons.Keywords:hydrodeoxygenation;biomass;hydropyrolysis;MoO3;bifunctional catalysts

CAS / MDL: 12054-85-2
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Reaction Kinetics Mechanisms and Catalysis · 2021 ·Vol. 134 ·期 2 ·1003-1015 · IF 2.081

Preparation of a zinc-based metal–organic framework (MOF-5)/BiOBr heterojunction for photodegradation of Rhodamine B

Chen Anna,Zhang Jin,Zhou Yi,Tang Haiqin

In this study, the MOF-5/BiOBr photocatalyst with microsphere structure was synthesized by hydrothermal method for the first time. The crystal structure, morphology, photoelectric performance and photocatalytic activity of the samples were characterized by XRD, SEM, TEM, XPS and electrochemistry. The results show that the synthesized MOF-5/BiOBr photocatalyst exhibits better photocatalytic performance than pure MOF-5 and BiOBr under simulated sunlight. The efficiency of Rhodamine B (RhB) removal based MOF-5/BiOBr composite (MOF-5 with mass ratio of MOF-5/BiOBr = 20 wt% of) reached 99.7%. The possible photocatalytic mechanism is discussed through the capture experiment of active species. The enhanced photocatalytic performance of the MOF-5/BiOBr composite may be related to the interaction between BiOBr and MOF-5 and the type II charge transfer path. The catalyst has simple preparation process, low cost, high activity under natural light, and high efficiency, and is expected to play a role in the treatment of environmental wastewater. This work provides a new insight for designing MOF-5 based photocatalyst.

CAS / MDL: 10035-06-0 81-88-9
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CHEMOSPHERE · 2021 · IF 7.086

Catalytic co-pyrolysis of oil sludge and biomass over ZSM-5 for production of aromatic platform chemicals

Jinyu Hou,Daoxu Zhong,Wuxing Liu

Hazardous oil sludge (OS) poses a great challenge to the environment, whereas conventional treatment methods (i.e., incineration or pyrolysis-incineration) are relatively less value-added and will bring about air pollution problems. To realize the high-value utilization of OS, catalytic co-pyrolysis with waste biomass to produce platform chemicals was studied using TG-FTIR and Py (pyrolyzer)-GC/MS methods. Results showed that for the non-catalytic co-pyrolysis of RH (rice husk) and OS, the main synergy on weight loss was the greatly lowered initial pyrolysis temperature of RH (for ∼55 °C) at the lower temperatures and the reduced weight loss ratio of OS (∼10–18 wt%) within the higher temperature range. ZSM-5 catalyst promoted the degradation of OS and RH mixtures at < 150 °C, yet showed minor effects on their weight loss at higher temperatures. The oxygenated and aliphatic compounds from non-catalytic co-pyrolysis were efficiently converted, resulting in an increased relative yield of aromatics to the highest of 46% and an elevated selectivity to BTX (as high as 60%). Despite the relatively short carbon chain length of OS components, ZSM-5 was proved effective to activate the OS pyrolysis products, thus enhancing the further aromatization reactions with biomass pyrolysis intermediates. This study provides a novel method for value-added co-utilization of hazardous OS waste and abundant biomass waste, and thus is beneficial to producing renewable chemicals while reducing the environment pollutant.

✓ 已验证 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Design and preparation of AP/M(5-ATZ)4Cl2 (M = Cu, Co) self-assembled intermolecular energetic materials

Wei Liu,Taixin Liang,Jiangbo Zhang,Fei Xiao,Houhe Chen

Intermolecular energetic materials (IEMs) have become the focus of attention due to their excellent performance in combustion, ignition, energy release and sensitivity. In this paper, two IEMs were successfully designed and prepared by the self-assembly of 5-aminotetrazole (5-ATZ) and transition metal ions on the surface of ammonium perchlorate (AP) particles. The scanning electron microscope, infrared spectroscopy, powder X-ray diffraction, thermogravimetric analyses, and differential thermal analyses were employed to characterize the prepared samples. The results show that the surface of AP particles is completely covered by a uniform and dense M(5-ATZ) 4 Cl 2 (M = Cu, Co) self-assembled layer. Thermal analyses show that the high-temperature decomposition peak temperatures of AP/Cu(5-ATZ) 4 Cl 2 (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 (10 wt%) are decreased by 93.3 °C and 127.1 °C compared to the case of pure AP, while the heat releases of them are increased by 539 J∙g −1 and 580 J∙g −1 . In addition, the burning rates of AP/Cu(5-ATZ) 4 Cl 2 /Al (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 /Al (10 wt%) are increased by 6.8 mm∙s −1 and 7.8 mm∙s −1 compared with the case of AP/Al. Moreover, the hygroscopicity tests show that the prepared samples do not agglomerate aftter being placed in the atmosphere with a relative humidity of 79% for 66 h. This research shows considerable application prospects in improving the combustion and energy performance of solid propellants, it is also a reference for the design and preparation of other novel IEMs.

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FOOD SCIENCE AND BIOTECHNOLOGY · 2023 · IF 2.9

Characterization of a novel ribose-5-phosphate isomerase B from Curtobacterium flaccumfaciens ZXL1 for D-allose production

Zheng Qian,Long Si,Chen Zhi,Fu Jiaolong,Ju Xin,Li Liangzhi

Enzymatic preparation of rare sugars as an alternative to traditional sweeteners is an effective strategy to achieve a low-calorie healthy diet. Ribose-5-phosphate isomerase B (RpiB) is a key enzyme in the non-oxidative branch of the catalytic pentose phosphate pathway. Here, we investigated the potential of Curtobacterium flaccumfaciens ZXL1 ( C. flaccumfaciens ZXL1) derived RpiB (CfRpiB) in D-allose preparation. The optimal reaction conditions for recombinant CfRpiB were found experimentally to be pH 7.0, 55 °C, and no metal ions. The kinetic parameters K m , k cat , and catalytic efficiency k ca t / K m were 320 mM, 4769 s −1 , and 14.9 mM −1  s −1 respectively. The conversion of D-allulose by purified enzyme (1 g L −1 ) to D-allose was 13% within 1 h. In addition, homology modeling and molecular docking were used to predict the active site residues: Asp13, Asp14, Cys72, Gly73, Thr74, Gly77, Asn106, and Lys144.

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CHEMICAL ENGINEERING SCIENCE · 2026 · IF 5.1

Enhancing light olefin production by pre-cracking and acidity tuning over hierarchical La/ZSM-5@ASA composites

Shuang Liu,Lei Ye,Shaokai Huang,Peng Zhou,Mingxuan Ma,Miao Hu,Xujin Ren,Xin Pu,Xin Han,Jichang Liu

La/ZSM-5@ASA composites were developed by a stepwise assembly strategy. • La 3+ displaced the acidic protons and generated new BAS [Si-OLa(OH) 2 -Al]. • ASA overcoat passivated external surface acid sites and enabled pre-cracking. • Hierarchical La/ZSM-5@ASA shows high light-olefin selectivity in n -paraffin cracking. Catalytic cracking of surplus automotive fuels, heavy oil and waste plastics into light olefins is an efficient resource-reutilization strategy. Conventional ZSM-5 zeolites, however, suffer from limited light-olefin selectivity and coke-induced deactivation due to strong acidity and microporous constraints. Herein, a stepwise assembly strategy involving La modification and subsequent amorphous silica-alumina (ASA) overcoating was developed to construct core–shell catalysts with optimized acidity and diffusion. La modification modulated acid strength and distribution, and DFT calculations revealed it lowered the energy barrier of the rate-determining protonation step, promoting propylene formation. The ASA overcoat, applied via co-gelation, passivated external strong Brønsted acid sites and introduced open interfacial diffusion channels. This architecture enabled pre-cracking of reactants, promoting efficient C-C bond cleavage and suppressing secondary reactions. The optimized hierarchical La/ZSM-5@ASA(1:1) achieved 63.10% total ethylene and propylene selectivity in n -heptane cracking, outperforming ZSM-5 and 0.50La/ZSM-5 by 5.12% and 1.38%, respectively. This advantage is more pronounced for longer linear hydrocarbons, and the suppression of methane and coke precursors boosts atom utilization efficiency, indicating a carbon-economic cracking pathway.

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APPLIED ORGANOMETALLIC CHEMISTRY · 2023 · IF 3.9

Transformation of glucose to 5-hydroxymethylfurfural with Al and Sn mixed-metal metal–organic frameworks as catalyst

Yongzhao Zhang,Xuzheng Chen,Zhenya Zhu,Luping Lv

5-hydroxymethylfurfural (5-HMF) has been considered as an important biomass-based platform chemical for its wide applications. Currently, the production of 5-HMF from the catalytic dehydration of glucose is preferred, in which the Brønsted and Lewis acids in catalysts play an important role. Here, it was found that MIL-53(Al) modified with tin was an active, selective, and reusable catalyst for the transformation of glucose to 5-HMF in dimethyl sulfoxide (DMSO) solvent. Around 42.3% yield of 5-HMF with 93% glucose conversion was achieved, when the prepared metal-organic frameworks (MOFs) was used as the catalyst, showing superior catalytic performance compared with most of other MOFs. Moreover, the catalyst possessed inert catalytic properties in water with almost no any influence on the conversion of glucose, suggesting a compelling opportunity to act as a support material.

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ELECTROANALYSIS · 2023 ·Vol. 36 ·期 3 ·e202300324 · IF 3

A facile ratiometric electrochemical sensing platform with in-situ electropolymerized thionine on effective sensing of 5-hydroxytryptamine

Kankan Chen,Jiawei Xu,Jingjing Song,Zhonggang Liu,Zheng Guo

The ratiometric electrochemical sensors have been highly explored to minimize system errors and environmental interference. However, it is extremely desirable on the development of an effective ratiometric electrochemical sensor in a facile approach without the complicated assembly process. In this work, an effective internal reference probe was coupled based on the polymerized thionine (pTh) via a one-step electrodeposition method. The ratiometric electrochemical sensing platform was applied for 5-hydroxytryptamine (5-HT) detection, where the internal reference probe, Th, presented the robust redox signal and can be clearly distinguished from the oxidation signal of 5-HT. The proposed pTh modified GCE presented the outstanding electrochemical performance on sensing 5-HT in a wide concentration range with a detection limit of 8.4 nΜ. Further, the fabricated sensor was efficiently employed for the detection of 5-HT in various human serum samples and the obtained results were consistent with the reported range in serum samples. This work offers the great possibility on the fabrication of efficient ratiometric sensors in a facile approach and presents great application prospects in clinical diagnosis.

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