JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Huiyu Zhao,Feng Wu,Qingwen Han,Chen Wang,Sibei Cao,Jiayu Ma
The solubility of potassium hexafluorosilicate (K2SiF6) in pure water and acid solutions (HCl and H3PO4) was conducted within a temperature range of 5–70 °C by the isothermal method. The stability of K2SiF6 in the systems above was also investigated by analyzing the equilibrium solids obtained in different conditions using X-ray diffraction (XRD), energy dispersive X-ray fluorescence (XRF), scanning electron microscope (SEM), and Fourier transform infrared (FT-IR). The results revealed that the solubility always increases with increasing temperature in all investigated systems. In the presence of hydrochloric acid and phosphoric acid, the solubility first increases and then decreases with the increase of acid concentration due to the increase of H+ concentration in hydrochloric acid, the effect of the stepwise dissociation of phosphoric acid, and the changed average ionic activity in solutions. K2SiF6 is stable in pure water and acid solutions. In addition, the experimental data were successfully correlated by the Apelblat empirical equation.
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Catalysts
·
2023
·Vol. 13
·期 7
·1080
·
IF 3.9
Shiyuan Lin,Ruosong He,Wenhang Wang,Yang Wang,Yongqiang Gu,Qiang Liu,Mingbo Wu
The abundant C1 source CO2can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3and acidic zeolite ZSM-5 was designed for the direct conversion of CO2+ H2into valuable aromatics, especially para-xylene (PX), via the methanol-mediated pathway. The twin structure of ZSM-5 (ZSM-5T), with sinusoidal channels that are predominantly exposed to the external surface, enhances the possibility of the transformation of methanol into PX due to the favorable diffusion dynamic of PX in the sinusoidal channels. Via the bifunctional catalyst Cr2O3&ZSM-5T, a PX selectivity of 28.7% and PX space-time yield (STY) of 2.5 gCH2h−1kgcat−1are achieved at a CO2conversion rate of 16.5%. Furthermore, we rationally modify the ZSM-5Tzeolite via Cu species doping and amorphous SiO2shell coating (Cu-ZSM-5T@SiO2). After combining with the Cr2O3catalytic component, the CO2conversion (18.4%) and PX selectivity (33.8%) are increased to some extent, which systematically increases the STY of PX to 3.0 gCH2h−1kgcat−1. The physicochemical property of the acidic zeolite and the corresponding structure-function relationship in enhancing the PX productivity are discovered. Our work provides a novel catalyst design idea to boost PX synthesis performance from CO2hydrogenation.Keywords:CO2hydrogenation;bifunctional catalysts;para-xylene;H-ZSM-5 zeolites
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ANALYTICAL CHEMISTRY
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2022
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IF 8.008
Jun Xiong,Ke-Ke Chen,Neng-Bin Xie,Tong-Tong Ji,Si-Yu Yu,Feng Tang,Conghua Xie,Yu-Qi Feng,Bi-Feng Yuan
DNA methylation (5-methylcytosine, 5mC) is the most prevalent epigenetic modification that is predominantly found in CG dinucleotides in mammalian genomes. In-depth investigation of the functions of 5mC heavily relies on the quantitative measurement of 5mC at single-base resolution in genomes. Here, we proposed a methyltransferase-directed labeling with APOBEC3A (A3A) deamination sequencing (MLAD-seq) method for the single-base resolution and quantitative detection of 5mC in DNA. In MLAD-seq, a mutant of DNA methyltransferase, M.MpeI-N374K, is utilized to selectively transfer a carboxymethyl group to the 5 position of cytosine in the CG dinucleotide to form 5-carboxymethylcytosine (5camC) using carboxy-S-adenosyl-l-methionine (caSAM) as the cofactor. After A3A treatment, 5camC is resistant to the deamination and base pairs with guanine. Thus, the cytosines in CG sites are read as C in sequencing. On the contrary, the methyl group in 5mC inhibits its carboxymethylcytosine by M.MpeI-N374K and therefore is readily deaminated by A3A to produce thymine that pairs with adenine and is read as T in sequencing. The differential readouts from C and 5mC in the MLAD-seq enable the single-base resolution mapping of 5mC in CG sites in DNA. With the developed MLAD-seq method, we observed the hypermethylation in the promoter region of retinoic acid receptor β (RARB) gene from human nonsmall cell lung tumor tissue. Compared to harsh reaction conditions in bisulfite sequencing that could lead to significant degradation of DNA, the whole procedure of MLAD-seq is carried out under mild conditions, which will avoid DNA damage. Thus, MLAD-seq is more suitable in the scenario where only limited input DNA is available. Taken together, the MLAD-seq offers a valuable tool for bisulfite-free, single-base resolution and quantitative detection of 5mC in limited DNA.
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PubMed
高影响因子
CORROSION SCIENCE
·
2022
·
IF 7.72
Youmin Qiu,Jie Li,Yifeng Bi,Xiaopeng Lu,Xiaohui Tu,Junjie Yang
A novel mixture, comprising sodium fluoride (NaF) and 3-amino-1,2,4-triazole-5-thiol (ATT), was reported as an effective hybrid corrosion inhibitor for magnesium alloy in pH neutral NaCl solution. The highest efficiency (95.8%) was achieved when 50 mM NaF and 5 mM ATT were mixed. Both experimental and theoretical approaches were employed for addressing the synergism. The synergism was proposed as the formation of a double-layered inhibitors film, in which the lower layer is a uniform fluoride-enriched precipitate layer and the upper one is a hydrophobic adsorption layer. These two layers were mutually strengthened to produce an excellent inhibition effect as a whole.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2022
·
IF 6.51
Yue-Ming Yu,Fan-Zhi Bu,Su-Su Meng,Cui-Wei Yan,Zhi-Yong Wu,Yan-Tuan Li
In order to highlight the advantages of cocrystallization technique in perfecting in vitro / vivo natures of marine drug cytarabine (ARC), and fill the gap of the research of marine pharmaceutical cocrystals with synergistic antitumor effects, the first dual-drug cocrystal simultaneously containing ARC and antitumor drug 5-fluorouracil (FU), viz. ARC-FU, is successfully designed and assembled. The accurate structure is perfectly resolved by single-crystal X-ray diffraction and other approaches. The analytical outcomes demonstrate that the codrug cocrystal consists of ARC and FU with a molar ratio of 1:1, in which FU molecule plays an important role by participating in the formation of both “pyrimidine-pyrimidine” and “pyrimidine-sugar” cyclic hydrogen-bonding systems with ARC molecules. In the cocrystal, there are twofold hydrogen-bonding helixes of ARC molecules and a whole three-dimensional hydrogen-bonding network which also contains the aromatic stacking interaction between pyrimidine rings of both components. Such structural feature and aggregation model have crucial influences on the improvements of in vitro/vivo properties, which is methodically verified by the combination of theoretical analyses and experimental measurements. The in vitro studies exhibit the suitably reduced solubility and obviously increased permeability for the cocrystal that is in accord with the theoretical prediction. Importantly, the ameliorated in vitro peculiarities realize in vivo pharmacokinetic optimization including the extended residence time and enhanced relative bioavailability. Of greater significance, ARC exerts synergistic antitumor effects in association with FU that brings about potentiation of cell growth inhibition with lower IC 50 . Thus, this research not only provides a novel crystalline form for ARC with forward-looking development value, but also breaks new ground for the development of synergistic antitumor pharmaceutical cocrystals with marine characteristics.
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高影响因子
RSC Advances
·
2022
·Vol. 12
·期 50
·32534-32551
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IF 4.036
Huanli Yin,Qi Yan,Yuan Liu,Lan Yang,Yang Liu,Yujie Luo,Tianyu Chen,Ningxi Li,Min Wu
A dual-loaded multi-targeted drug delivery nanosystem was constructed to simultaneously load paclitaxel (PTX) and 5-fluorouracil (5-FU) for targeted delivery and sustained release at tumor sites. Hollow mesoporous silica nanoparticles (HMSNs) were prepared by the inverse microemulsion method, then modified with folic acid and pH- and temperature-responsive materials, co-loaded with PTX and 5-FU, and finally encapsulated into lipid membranes. The obtained nanosystem was selectively internalized by human breast cancer MCF-7 cells that overexpress folate receptors through an energy-dependent process, and it released both drugs in vitro in a simulated tumor microenvironment. Moreover, the inhibitory effect of the dual-loaded nanoparticles was significantly better than that of the free drugs, suggesting that the composite nanosystem has the potential to selectively target tumor sites and perform the synergistic effect of PTX and 5-FU, while reducing their toxic effects on normal tissues.
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高影响因子
FUEL
·
2022
·
IF 8.035
Yan Cui,Bin Chen,Leilei Xu,Mindong Chen,Cai-e Wu,Jian Qiu,Ge Cheng,Ning Wang,Jingxin Xu,Xun Hu
Hollow ZSM-5 zeolites prepared using different alkaline solutions were employed as Ni based catalyst supports for the methanation of CO 2 . The catalysts were thoroughly characterized, and in-situ DRIFTS were used to study the CO 2 methanation intermediates. Using the hollow Ni-based catalysts led to enhanced CO 2 conversion as well as CH 4 selectivity compared with the traditional Ni/ZSM-5, which was mainly due to the strong basicity of the hollow supports as well as the presence of silicon hydroxyls. Meanwhile, the 15Ni/H-ZSM-5-T catalyst prepared with TPAOH solution had higher catalytic performance than 15Ni/H-ZSM-5-NT and 15Ni/H-ZSM-5-N. The introduction of the hollow zeolite morphology led to enhanced diffusion behavior in the catalyst, which inhibited catalyst deactivation. Therefore, the hollow structure of the support with alkaline treatment was an important consideration for the design and preparation of high-performance Ni-based catalysts for CO 2 methanation.
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FOOD RESEARCH INTERNATIONAL
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2022
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IF 7.425
Yingjie Ma,Hairong Huang,Yan Zhang,Feng Li,Bei Gan,Qiang Yu,Jianhua Xie,Yi Chen
This study investigated the impact of soluble dietary fiber (SDF) from untreated (U-SDF), fermented (F-SDF) and high temperature cooked (H-SDF) from tea residues on formation of acrylamide (AA) and 5-hydroxymethylfurfural (5-HMF) in biscuits. Both 3% F-SDF and 2% H-SDF can simultaneously inhibit AA and 5-HMF and SDFs increased the types of volatile compounds in biscuits. After the determination of the bound polyphenol compositions in SDFs by LC-QTOF-MS/MS, six polyphenols with different structural characteristics were selected to explore their contributions on the inhibitory effect of SDFs and structure-inhibitory capacity relationships in the “glucose-asparagine-linoleic acid” model system. It showed that the inhibitory activities of those polyphenols were greatly affected by the number of hydroxyl groups and methoxy groups on the benzene ring. Almost all polyphenols were also found to scavenge hydroxyl radicals generated in reactions. Thus, this study suggests that the bound polyphenols of SDFs play a key role in the inhibition of AA and 5-HMF.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Yongfang Zhou,Yi Shen,Hongying Li
Electrocatalytic oxidation of biomass such as 5-hydroxymethylfurfural (HMF) is a green route to produce value-added chemicals. However, in-depth understanding of the electrocatalytic process is still lacking. Herein, the mechanism of HMF electro-oxidation was studied by operando surface-enhanced Raman spectroscopy (SERS) coupled with an Fe 3+ probe. A multicomponent platform consisting of titanium plates integrated with a gold film and uniform nickel, cobalt and copper nanoparticles (NPs) was employed as an electrode as well as a SERS substrate, enabling operando SERS study on the electrocatalytic process with simultaneous evaluation on catalytic activity and visualization on the variations of active sites. Fe 3+ was intentionally added into the electrolyte as a probe to correlate the nature of active sites with catalytic activity and product selectivity in virtue of its strong interaction with the active sites of the electrocatalysts. Electrodes integrated with Ni and Cu NPs exhibited excellent HMF oxidation performance but their activity were suppressed by adding 1 ppm Fe 3+ . Conversely, the activity towards water oxidation was significantly enhanced by Fe 3+ addition. Fe 3+ inhibits the oxidation of Ni 2+ to Ni 3+ and promotes the formation of more CuO and Cu III . Cu III is better active sites for water oxidation. The presence of Fe 3+ also inhibits the transformation of Co 3+ to Co 4+ , but it has no pronounced effects on HMF oxidation performance. A highest 2,5-furandicarboxylic acid yield (94.0%) and a maximum HMF conversion (98%) are obtained from the electrode integrated with Cu NPs at a potential of 1.47 V. HMF oxidation on Cu NPs follows the aldehyde oxidation pathway, which is not affected by Fe 3+ addition. This work could afford a feasible route to explore mechanisms of electrocatalytic processes.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Xin-Xin Fu,Jian-Peng Li,Zhuo-Qian Li,Yan Liu,Chen-Xiao Feng,Hai-Yang Wang,Zhi-Peng Zhao,Qiao-Yun Liu,Zhong-Yi Liu,Zhi-Kun Peng
Biomass is a promising renewable carbon resource, and bio-based platform molecules such as furan derivatives play an important role in the green manufacturing of high value-added chemicals. Of these, the conversion of 2-methylfuran (2-MF) to 3-acetyl-1-propanol (3-AP) over a bifunctional catalyst has attracted significant interest. However, bifunctional catalysts prepared by traditional method suffer from poor catalytic performance and limited stability due to the agglomeration of metal NPs. Here, Pd@HZSM-5, in which Pd NPs were encapsulated in HZSM-5 in situ showed improved stability and 3-AP yield. The highest yield of 3-AP (90.6%) to date was obtained with a nearly 100% conversion of 2-MF. The catalytic performance over a series of Pd@Zeolite confirms the superiority of the encapsulation effect, which is ascribed to the optimal adjustment of metal/acid balance. The Pd@HZSM-5 catalyst displayed excellent stability due to the encapsulation structure, which restricts the Pd NPs agglomeration. The highest yield of 3-AP was obtained at a high concentration of 2-MF (60%), which implies a promising strategy for the green industrial manufacture of 3-AP. This work reports a new bifunctional catalytic system for the green synthesis of 3-AP from 2-MF, thus stimulating the downstream biomass market.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Xin Ning,Junwen Chen,Qi Zuo,Wenlin Li,Jiajun Zheng,Ruifeng Li
Light alkenes oligomerization , performed in the presence of solid acid catalysts , is an important alternative for the production of clean jet fuels. For 1-hexene oligomerization, the current catalyst often suffers from low activity and selectivity. The developed process is upgraded by zeolite catalyst, targeting high-concentration of jet-range hydrocarbons. An efficient and selective IM-5 zeolite-derived catalytic system has been developed for the oligomerization of 1-hexene. The treatment in an aqueous NH 4 F solution led to dealumination without structure degradation. The IM-5 zeolite with a unique two-dimensional IMF structure and 2.5 nm nanoslab showed rapid diffusion ability than ZSM-5 zeolite. Enhance acidities were observed in the NH 4 F-treated IM-5 zeolites owing to fluoride residue and the removal of Al atoms. The strong Brønsted acid sites exerted a positive effect on both the cracking and the oligomerization reactions with the increasing of the yields of dimers. The contact time and partial pressure between the 1-hexene and the IM-5 zeolites were used to analyze the competition of cracking reactions. High 1-hexene conversion (62%), optimal oligomerization to C 3 -C 5 ratio (O/C = 32), and reasonable stability were obtained over the etched IM-5 catalyst at 240 °C, 4 MPa, and the flow rate of N 2 was 50 mL/min.
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Molecular Catalysis
·
2022
·
IF 5.089
Yiqiang Liu,Yimei Qiu,Wenlong Jia,Zhiliang Shen,Zheng Li,Jiaren Zhang,Yong Sun,Xing Tang,Xianhai Zeng,Lu Lin
In this work, a porous Zirconium based coordination polymer (Zr-ATMP) was facilely synthesized at room temperature with amino tris(methylene phosphonic acid) (ATMP) as ligand, and the surface acidic sites could be adjusted in different solvents. Specifically, the coordination polymer with equivalent content of Bronsted and Lewis acid sites was synthesized in aqueous system, showing high-efficiency catalytic activity for fructose dehydration to 5-hydroxymethylfurfural (HMF). In comparison, the coordination polymer containing an abundance of Lewis acid sites was synthesized in DMF solvent, which efficiently catalyzed the transfer hydrogenation of HMF. Compared to the catalysts preparation in organic solvents, the coordinatively unsaturated Zr 4+ could be hydrated in water during catalyst preparation, resulting in the generation of additional Bronsted acid sites at the cost of Lewis acid sites. This contribution proposed a facile approach to prepare Zr-based coordination polymer with tunable acid properties for biomass valorization.
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