JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Lei Yuan,Cai Xu,Shaoyong Zhang,Mincheng Yu,Xiaozhong Wang,Yingqi Chen,Liyan Dai
The selective C H bond oxidation of aromatic hydrocarbon is an interesting but challenging task, it is desirable to develop efficient heterogeneous non-noble metal catalyst for this reaction. Herein, two kinds of spinel (FeCoNiCrMn) 3 O 4 high entropy oxides were fabricated via two different methods (i.e., c-FeCoNiCrMn, prepared by a co-precipitation method, and m-FeCoNiCrMn, prepared by physically mixing method). Different from traditional environmentally-unfriendly Co/Mn/Br system, the prepared catalysts were employed for the selective C H bond oxidation of p-chlorotoluene to p-chlorobenzaldehyde in a green approach. Compared to m-FeCoNiCrMn, c-FeCoNiCrMn have smaller particles size and larger specific surface area, which were related to the enhanced catalytic activity. More importantly, characterization results disclosed that abundant oxygen vacancies were formed over c-FeCoNiCrMn. Such a result facilitated the adsorption of p-chlorotoluene on the catalyst surface and promoted the formation of *ClPhCH 2 O intermediate as well as the desired p-chlorobenzaldehyde, as revealed by DFT (Density functional theory) calculations. Besides, scavenger tests and EPR (Electron paramagnetic resonance) results indicated that hydroxyl radical derived from H 2 O 2 homolysis was the main active oxidative species for this reaction. This work revealed the role of oxygen vacancy in spinel high entropy oxide and also demonstrated its promising application for the selective C H bond oxidation in an environmentally-benign approach.
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高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Siyuan Chang,Sen Zhang,Tianyi Chen,Lei Xu,Sumin Ge,Bingfeng Li,Chenke Yun,Guoxin Zhang,Xuejun He,Xin Pan
The important bio-based platform chemical 5-Hydroxymethylfurfural (HMF) can be oxidized for use in several products that serve as versatile building blocks of polymers. Previously, we had demonstrated that Pseudomonas aeruginosa PC-1 can selectively produce 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) from 800 mM HMF, with a yield greater than 90%. In this study, an aldehyde dehydrogenase (PaALDH64) was identified from P. aeruginosa PC-1 for selective HMF oxidation to HMFCA. The HMF tolerance level of E. coli /pET- PaALDH64 was over 300 mM, which was greater than the tolerance levels of all other reported enzymes. The proposed biocatalyst could be used to catalyze the biotransformation of other aldehydic furans, with carboxylic acid yields over 92%. Molecular docking revealed that the catalytic active site cleft in PaALDH64 formed more hydrogen bonds with HMF compared to other enzymes, which stabilized the enzyme–substrate interaction and enhanced the catalytic efficiency. In a fed-batch process, 547.8 mM HMFCA was produced from 600 mM HMF by E. coli /pET- PaALDH64 within 19 h only, which showed an excellent HMF conversion rate. Overall, PaALDH64 constitutes a promising enzyme for the industrial production of HMFCA.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaoqing Yuan,Ju Liu,Yanlei Wang,Xingming Jie,Jingyu Qin,Hongyan He
Knoevenagel condensation reaction is important for generating C C double bonds and providing various valuable intermediates in organic chemistry, which always need harsh conditions including high reaction temperature, difficult catalyst recovery, difficult product separation, etc. In this work, a novel class of dual-responsive emulsion reactor was prepared for the Knoevenagel condensation reaction between malononitrile and aromatic aldehyde, where the temperature and CO 2 -responsive ionic liquids (ILs) were used as an emulsifier, responder, and catalyst simultaneously. Driven by temperature or CO 2 , the emulsion reactor undergoes reversible and controllable transformations between emulsification and demulsification, where efficient catalytic reactions, product separation, and reactor recovery are all achieved. The isolated product yield of 2-(4-chlorobenzylidene)-malononitrile remained above 90% after 5 cycles of the emulsion reactor. NMR and molecular dynamics simulations showed that the temperature drives the reversible stretching and curling of the polyether chain on the cation, while CO 2 reacts with the –COO - group on the anion to form carbonates and carboxylic acids in water, leading to changes in the surface activity of ILs, thereby reversibly regulating the demulsification and emulsification of the emulsion. Hence, through the dual stimuli-responsive ILs, the efficient reaction can be performed in the homogeneous phase, and the products and catalysts can be easily separated in the heterogeneous phase. These results on the revisable microreactor can not only help to design the smart and efficient “homogeneous reaction-heterogeneous separation” systems but also support the development of green sustainable chemistry.
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ChemSusChem
·
2022
·Vol. 15
·期 19
·e202201068
·
IF 9.14
Meijiang Liu,Huifang Liu,Ning Li,Chaofeng Zhang,Jian Zhang,Feng Wang
Graphical Selectivity under control : The synergistic action of photogenerated holes and superoxide radicals could selectively oxidize the C−C bond breakage to generate formic acid. And the generation of hydroxyl radicals was inhibited in favor of solving the over-oxidation of formic acid. Photocatalysis is a promising technology for conversion of the glycerol into formic acid, but photocatalytic oxidation of C−C bonds in glycerol exhibits poor selectivity towards formic acid because the photogenerated radicals (e.g., hydroxyl radicals) further oxidize formic acid to CO 2 . In this work, a synergy of photogenerated holes and superoxide radicals that achieved the selective oxidation of glycerol into formic acid over the TiO 2 catalyst was revealed. The charge separation of pristine TiO 2 was improved with the aid of oxygen, which resulted in efficient hole oxidation of the C−C bonds in glycerol to formic acid. Surface active species were controlled to prevent being converted to hydroxyl radicals on TiO 2 by controlling the oxygen and water contents, which solved the problem of formic acid peroxidation without sophisticated catalyst modifications. Mechanism studies suggested that glyceraldehyde and glycolaldehyde were the intermediates to generate formic acid. This work provides a green and efficient approach to produce formic acid as a liquid hydrogen carrier from bio-based alcohols.
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Materials Today Communications
·
2023
·
IF 3.8
Hu Tian,Yuanyuan Zhang,Lin Liu,Jinjuan Xing,Xiaojun Wang
Three triazole Schiff bases [1-(4-Methylphenyl)-N-(1,2,4-triazol-4-yl)methanimine (A1), 4-(1,2,4-triazol-4-yliminomethyl)phenol (A2) and 1-(4-chlorophenyl)-N-(1,2,4-triazol-4-yl)methanimine (A3)] were synthesized in this work. Self-assembled monolayer films (SAMs) were prepared on copper (Cu) surfaces using the compounds mentioned above respectively. The characterization methods such as contact angle (CA), scanning electron microscopy (SEM) and electrochemical measurement were applied to evaluate the inhibition behaviors of the three Schiff bases in 3.5 wt% NaCl solution on coppers. Electrochemical tests proved their prominent corrosion inhibition performances of the three Schiff bases. Adsorption behaviors of the three Schiff bases on the copper surfaces obeyed Langmuir isotherm adsorption model. Quantum chemical calculation and molecular dynamics simulation (MD) further confirmed the relationship between corrosion inhibition performance and molecular structure.
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MACROMOLECULES
·
2023
·
IF 5.5
Yang You,Zheng Yue Wang,Min Zhi Rong,Ming Qiu Zhang
The authors of this work propose the construction of reversibly interlocked macromolecular networks (RILNs) at the interface between immiscible polymers to address the common challenge arising from compounding different polymers together. The proof-of-concept model system is made by stacking cross-linked polyether and styrene–butadiene block copolymer, which, respectively, contain reversible Schiff base and Diels–Alder (DA) bonds. By taking advantage of the synergy between the topological rearrangement of the dynamic networks and migration of the pre-embedded zinc ion catalyst, interdiffusion and interlocking of the temporarily de-cross-linked macromolecular chains can be purposely synchronized. Consequently, the envisaged interfacial RILNs with decent mechanical properties are successfully prepared in the solid state, which is an advancement over traditional RILNs that have to be made with the assistance of solvent. The resulting interfacial binding is tight and reversible because of the massive chain entanglements in the interfacial region and the degradability of dynamic networks as well. It is anticipated that the methodology discussed in the paper would hopefully be developed into a facile technique for the fabrication of high-performance polymer blends regardless of the miscibility of the raw materials.
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CATALYSIS LETTERS
·
2020
·Vol. 151
·期 3
·720-733
·
IF 2.482
Zhu Anlian,Li Qixing,Feng Wanlu,Fan Dongshuang,Li Lingjun
Abstract The synthesis of 2-amino-4H-chromenes through one-pot multicomponent reactions has received great attention due to the high atom efficiency and the broad bioactivities of the products. Here, the catalytic performances of a series of functional ionic liquids towards this type of reaction were investigated and the results showed that the ionic liquid, choline acetate ([Choline][Ac]), could efficiently promote this reactions under room temperature without the necessary of organic solvents. The reaction is easy to be conducted and the following work-up procedures are very simple. The pure products can be obtained through extraction and washing procedures, no column separation procedures are needed. Intriguingly, this reaction system can be easily scaled up to multi-gram, suggesting its perspective in industrial applications. In addition, the ionic liquid [Choline][Ac] can be easily prepared from cheap and biocompatible materials, and it can be feasibly recycled and reutilized for at least five cycles. Graphic Abstract
Various aldehydes, malononitrile and activated phenols could be converted to the
corresponding 2-amino-4H-chromenes with good to excellent isolated yields under
the catalysis of choline acetate at room temperature.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Pengqi Zhu,Mengting Gao,Jin Zhang,Zhiwei Wu,Ruiyi Wang,Yunwei Wang,Eric R. Waclawik,Zhanfeng Zheng
Coordinated Ru species, Ru/LDH, were applied to the reduction of carbonyl compounds via blue light irradiation under mild (45 °C, atmospheric argon pressure), ligand-free, and additive-free conditions. LDH can act as an efficient base catalyst to assist in formation of isopropoxide, requiring no additional base, because basic OH groups form an ordered distribution on LDH surface. The coordinated Ru species containing one OH and three oxygen atoms ligands deriving from the OH groups of LDH are a crucial component, for securing the active electron-deficient Ru species that favours formation of Ru-isopropoxide. The photocatalytic activity is related to the adsorption capacity of isopropyl alcohol near the electron-deficient Ru species and the formation of Ru-isopropoxide. The strong-metal-support interactions between Ru and LDH affect the coordination and the electronic surroundings of the Ru centres and have a significant effect on the photocatalytic activity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Jiuli Han,Lu Bai,Shuangjiang Luo,Bingbing Yang,Yinge Bai,Shaojuan Zeng,Xiangping Zhang
Ionic liquids (ILs) are attractive and prospective materials used in membranes due to the nonvolatility, structure tunability, and the ability to tune the interface compatibility. The cobalt IL Bmim 2 Co(NCS) 4 possesses the porphyrin-like N4-coordinated cobalt center which could selectively and reversibly interact with O 2 . Herein the Bmim 2 Co(NCS) 4 as liquid-phase oxygen carrier was used to fabricate thin-film composite (TFC) membrane with the polymer of intrinsic microporosity (PIM-1). The microstructures, properties and gas separation performance of the membrane were compared with the TFC membrane which takes cobalt porphyrin (T(4-Cl)PPCo) as a carrier. We found that the addition of a small amount of T(4-Cl)PPCo can enlarge the d -spacing of packed chains of PIM-1 and significantly increase the fractional free volume (FFV) and the gas permeability of the membrane, but the selectivity is unsatisfactory. It is worth noting that adding Bmim 2 Co(NCS) 4 into the polymer can increase greatly the O 2 /N 2 selectivity which is higher than that of the membrane with T(4-Cl)PPCo. Although the addition of Bmim 2 Co(NCS) 4 decreases the d -spacing of packed chains of PIM-1, resulting in the slight decline of FFV and gas permeability of the membrane, the Bmim 2 Co(NCS) 4 /PIM-1 TFC membranes exhibit better O 2 /N 2 separation performance than the T(4-Cl)PPCo/PIM-1 TFC membranes in consideration of the Robeson upper bound.
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ADVANCED FUNCTIONAL MATERIALS
·
2019
·Vol. 29
·期 19
·1901101
·
IF 15.621
Zhou Liu,Tiyun Yang,Yuxing Huang,Yang Liu,Liucheng Chen,Libo Deng,Ho Cheung Shum,Tiantian Kong
Miniaturized droplet reactors hold great promise for the development of green and sustainable chemistry. However, handling liquids with small volumes, especially viscous ones, in a convenient and loss-free manner remains a challenge. Here, by electrically controlling the coalescence and mixing of particle-coated droplets, also known as liquid marbles, an effective microreactor is demonstrated for miniaturized chemical reactions involving viscous reagents. By applying an electric voltage to marbles, the induced electromixing of marble microreactors promotes the reaction rate and the product yield. The advantages of electromixed marble reactors are manifested by a series of chemical reactions between aldehydes and 2-methylindole in viscous glycerol solution. The electrically-controlled coalescence and mixing establish liquid marbles as microreactors for rapid, efficient, and miniaturized chemical reactions.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 10
·e5120
·
IF 3.259
Dongdong Li,Luyao Wang,Ernesto Yagüe,Linlin Dai,Xiumei Zhao,Zibo Yang,Shuang Zhi,Yunhui Hu
An innovative ternary copper(II) complex, [Cu(Cl-PIP)(Tyr)Cl] n , has been synthesized and characterized using infrared spectroscopy, elemental analysis and single-crystal X-ray diffraction analysis. X-ray crystallography indicates that the Cu atom is five-coordinated in a square-pyramidal configuration. The unit forms a one-dimensional chain along the crystallographic c -axis. The complex was screened for cytotoxicity against a panel of eight human cancer cell lines, namely MDA-MB-231, CAL-51, K562, HeLa, SGC-7901, A549, MCF-7 and SMMC-7721. The best anticancer activity was obtained with triple-negative breast cancer CAL-51 and MDA-MB-231 cell lines, with IC 50 values in the range 0.035–0.10 μM, and this was better than using carboplatin. The complex inhibits proteasomal chymotrypsin-like activity, and docking studies reveal its interaction with 20S proteasome. In addition, the complex causes accumulation of ubiquitinated proteins, induces apoptosis and inhibits cell proliferation, indicating its great potential as a novel therapy for triple-negative breast cancer.
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Catalysis Science & Technology
·
2015
·Vol. 5
·期 7
·3798-3805
·
IF 5.426
Song Wang,Pingwei Liu,Wen-Jun Wang,Zhiguo Zhang,Bo-Geng Li
A novel hyperbranched polyethylene (HBPE)-supported L-proline has been developed via a bottom-up copolymerization strategy. Copolymerization of ethylene and a protected proline acrylate comonomer with cationic Pd-diimine catalysts was conducted, followed by de-protection of the proline groups. Well-defined HBPE copolymers having molecular weights (MWs) of 10.3–50.3 kDa and 3.2–15.6 L-proline molecules per HBPE polymer chain were synthesized. The effects of the L-proline amount and HBPE MW on the catalyst performance were studied. The HBPE catalysts were efficient in asymmetric aldol reactions of p-nitrobenzaldehyde (p-NBA) or benzaldehyde derivatives with cyclohexanone. High p-NBA conversions of up to 98% and excellent product selectivities with anti/syn = 98/2 and ee > 99% were achieved. Moreover, the HBPE catalysts could be easily recovered by adding water into the product. The recovered catalysts could be reused multiple times with only a slight decline in reactivity and selectivity.
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