Surfaces and Interfaces
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2024
·
IF 5.7
Hao Zhang,Zhengyuan Tao,Ziqi Yu,Tiantian Zhu,Hanlin Rao,Badusha Mohamad Ali,Jianli Wang
Pickering interfacial catalysts (PICs) have emerged as a promising solution for simultaneously enhancing and catalyzing liquid-liquid biphasic reactions. In this study, we successfully synthesized dumbbell-shaped Janus structured polymeric nanoparticles with one side anchored imidazolium-TEMPO (im-C 4 -TEMPO@JPP) as Pickering interfacial catalyst for the oxidation of alcohols using the Anelli-Montanari reaction system. In the Pickering emulsion system, the im-C 4 -TEMPO@JPPs particles are assembled at the W/O interface due to the hydrophilicity of imidazolium-TEMPO anchored lobe which enables excellent amphiphilic character of the polymeric Janus dumbbell. Moreover, the im-C 4 -TEMPO@JPPs particles reduce the interfacial tension from 27.82 to 18.43 mN/m. This excellent interfacial adsorption capacity of im-C 4 -TEMPO@JPPs strongly stabilizes the water/dichloromethane Pickering emulsion over two months (emulsion volume fraction >90 %), thus providing an efficient reaction platform for liquid-liquid biphasic reactions. As a result, the constructed Pickering emulsion system efficiently catalyzes the oxidation of cinnamyl alcohol to cinnamaldehyde under static conditions. After 1 hour of reaction, the conversion of cinnamyl alcohol achieved 97.1 % with a selectivity of 99 %, nearly the same level relative to stirring intensified biphasic reaction. Hence, this novel PIC effectively improves the efficiency and sustainability of liquid-liquid biphasic catalytic reactions .
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MOLECULES
·
2024
·Vol. 29
·期 7
·1554
·
IF 4.2
Haorui Gong,Sai An,Weilong Qin,Yongbo Kuang,Deyu Liu
In order to expand the application of bismuth vanadate (BiVO4) to the field of photoelectrochemistry, researchers have explored the potential of BiVO4in catalyzing or degrading organic substances, potentially presenting a green and eco-friendly solution. A study was conducted to investigate the impact of electrolytes on the photocatalysis of benzyl alcohol by BiVO4. The research discovered that, in an acetonitrile electrolyte (pH 9) with sodium bicarbonate, BiVO4catalyzed benzyl alcohol by introducing saturated V5+. This innovation addressed the issue of benzyl alcohol being susceptible to catalysis in an alkaline setting, as V5+was prone to dissolution in pH 9 on BiVO4. The concern of the photocorrosion of BiVO4was mitigated through two approaches. Firstly, the incorporation of a non-aqueous medium inhibited the formation of active material intermediates, reducing the susceptibility of the electrode surface to photocorrosion. Secondly, the presence of saturated V5+further deterred the leaching of V5+. Concurrently, the production of carbonate radicals by bicarbonate played a vital role in catalyzing benzyl alcohol. The results show that, in this system, BiVO4has the potential to oxidize benzyl alcohol by photocatalysis.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hui Wang,Hongtu Zhao,Wenbo Wu,Shifan Xu,Na Wang,Ting Wang,Xin Huang,Lina Zhou,Ying Bao,Hongxun Hao
The solubility performance of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane has been investigated by the combination of experimental measurement, solvent parameter analysis, and molecular simulation methods. The solubility in 10 pure solvents at 293.15 K to 343.15 K was determined. It was found that the solubility in nine solvents increased with temperature, except for isoamyl propionate. However, it has the largest solubility in isoamyl propionate (4.36 × 10 −2 ∼ 5.39 × 10 −2 ). Additionally, a correlation analysis was performed using four equations, which showed that the NRTL equation provided the best fit (overall average relative deviation = 3.74 %, overall coefficient of determination = 0.991). Moreover, the solvent effect was analyzed by Hansen solubility parameters, predicting good solubility in solvents with R a(V) ≤ 12.47 MPa 0.5 or Δ δ t ≤ 7.77 MPa 0.5 , indicating weak polarity of solvent and weak solvent–solvent intermolecular hydrogen bonds enhance dissolution. Furthermore, molecular electrostatic potential surface and radial distribution function analyses provided that weak hydrogen bonding C-H···O promotes dissolution.
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AICHE JOURNAL
·
2024
·
IF 3.5
Tong Luo,Qi Liu,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Aqueous amine solution is a promising absorbent for CO 2 capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO 2 for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high-performance CO 2 absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti-degradation CO 2 absorbent.
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EUROPEAN POLYMER JOURNAL
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2024
·
IF 5.8
Zedong He,Hao Zhang,Ju Xie,Ti Zhou,Jie Zhang
Silicon-containing polyesters represent a novel class of polymers that integrate silicone and polyester units within their main chain. Polysiloxanes typically consist of flexible chain segments, while polyesters are characterized by their rigidity. The combination of these two components in the main chain offers the potential for tunable properties across a broad range. For the first time, a new organosilicon cyclic ester monomer (Si-Mon) was synthesized using a pseudo-high dilution condensation method. Both theoretical and experimental studies confirm that the ring-opening reaction site of Si-Mon is the ester group, rather than the Si-O-Si bond. Silicon-containing polyesters (SiPET-Series 1) with molecular weights exceeding 20,000 Da were efficiently and rapidly synthesized at room temperature, utilizing benzyl alcohol as the initiator and t-BuP 4 as the catalyst. Organosilicon polyester diols (SiPET-Series 2) with varying molecular weights were produced using 1,4-benzenedimethanol as the initiator. Additionally, a new type of organosilicon polyester elastomer (SiPET-E) was developed by employing SiPET-Series 2 as the base gum and (2,4,6-trioxotriazine-1,3,5(2H,4H,6H)- triyl)tris(hexamethylene)isocyanate (THDI) as the crosslinking agent. The stress–strain behavior of SiPET-E is influenced by the molecular weight of SiPET-Series 2. Notably, SiPET-E exhibits remarkable properties; for instance, it demonstrates superelastic characteristics when the molecular weight of SiPET-Series 2 is 13,000 g/mol, achieving a tensile strength of 2.56 MPa and an elongation at break of 776 % without the use of reinforcing fillers.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Li Suiqin,Wang Shibin,Wang Yuhang,He Jiahui,Li Kai,Gerken James B.,Stahl Shannon S.,Zhong Xing,Wang Jianguo
Electrochemical alcohol oxidation (EAO) represents an effective method for the production of high-value carbonyl products. However, its industrial viability is hindered by suboptimal efficiency stemming from low reaction rates. Here, we present a synergistic electrocatalysis approach that integrates an active electrode and aminoxyl radical to enhance the performance of EAO. The optimal aminoxyl radical (4-acetamido-2,2,6,6-tetramethylpiperidine 1-oxyl) and Ni 0.67 V 0.33 -layered double hydroxide (LDH) are screen as cooperative electrocatalysts by integrating theoretical predictions and experiments. The Ni 0.67 V 0.33 -LDH facilitates the adsorption and activation of N -(1-hydroxy-2,2,6,6-tetramethylpiperidin-4-yl)acetamide (ACTH) via interactions with ketonic oxygen, thereby improving selectivity and yield at high current densities. The electrolysis process is scaled up to produce 200 g of the steroid carbonyl product 8b (19-Aldoandrostenedione), achieving a yield of 91% and a productivity of 243 g h -1 . These results represent a promising method for accelerating electron transfer to enhance alcohol oxidation, highlighting its potential for practical electrosynthesis applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Jinbo Hu,Wenbo Wang,Xinyan Liu,Yeqi Du,Hao Zhang,Ranlong Duan,Xinchao Bian,Yanlong Liu,Xuesi Chen
The lower melt strength of poly(lactide) (PLA) limits its broader applications. Here, a strategy combining copolymerization with multi-arm branching was propose to enhance the melt strength of PLA. Initially, stereoisomeric cyclic ester monomers (CEM) synthesized via zeolite catalysis were copolymerized into PLA chains. Subsequently, rheological testing revealed that the zero-shear viscosity ( η 0 ) of linear PLA increased by 467 % with only 1 mol% of CEM units. Our study further systematically explored the relationship between the side group structure and chirality of the comonomers and the rheological properties of the copolymers. CEMs with long-chain branched structures and opposite chirality had the best enhancement effect. In order to further enhance the melt strength, we successfully achieved alterations in polymer topology by employing trimethylolpropane as an initiator, corresponding three-arm copolymers achieve up to a 67-fold increase in η 0 (1.0 kPa∙s to 68.1 kPa∙s). Tensile tests indicated that the mechanical properties of the copolymers were comparable to those of PLA, with a tensile strength of approximately 65 MPa. Additionally, due to the high melt strength, we successfully produced closed-cell PLA-based foam materials with uniform pore sizes. In summary, this study furnishes a feasible method for designing polymer materials possessing the desired melt strength.
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CHEMISTRY OF MATERIALS
·
2024
·
IF 7.2
Yufen Xiao,Jiamin Zhang,Tong Wu,Shuai Chen,Zhixiong Huang,Jianzhong Du
Natural modulators, such as insulin, play a significant role in modulating molecule levels. Inspired by the role of natural modulators, herein, we propose a glucose modulator that is composed of a glycopolymersome only to regulate glucose levels. This insulin- and drug-free strategy can smartly take in and snap out glucose according to the surrounding blood glucose levels (BGLs) by reversible sugar substituting. The glycopolymersome is self-assembled from a biodegradable glycopolymer that is composed of sugar and phenylboronic acid derivative, poly(ε-caprolactone)-block-poly[(3-acrylamidophenylboronic acid-stat-N-acryloyl glucosamine] [PCL-b-P(AAPBA-stat-AGA)]. It exhibits excellent long-term hypoglycemic effects toward type 1 diabetic mice for at least 3 days upon one shot without observed side effects, which is the longest effective sugar-regulation time for the insulin and drug-free strategy. Most notably, we explored the effect of the molecular structure of the glycopolymers on the BGL regulating efficacy, where the glucosyl moiety was polymerized with PBA either randomly or separately. Block-statistical glycopolymersomes exhibited lower binding energy to glucose, better glucose responsiveness, and prolonged hypoglycemic effect due to the abundant intramolecular and intermolecular dynamic covalent bonds between AAPBA and AGA. Our finding confirmed the importance of a block-statistical copolymer structure and the key role of sugar in regulating BGLs without involving medication, which may provide guidance and open new avenues for design blood glucose regulating materials.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Hao Wu,Xian Jiang,Jingyu Lu,Yibo Li,Xinyan Li,Guidong Ju,Rengui Li,Jing Zhang
The hydrogen evolution reaction (HER) in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production. Herein, we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H Inc -PdRu electrocatalyst, thereby modulating its electronic structure and enhancing its alkaline HER performance. We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity, achieving a remarkably low overpotential of 25 mV at 10 mA cm –2 compared with the Pd, Ru and PdRu catalysts while maintaining robust catalyst stability. Operando spectroscopic analysis indicates that H insertion into the H Inc -PdRu electrocatalyst enhances the availability of H 2 O* at the surface, promoting water dissociation at the active sites. Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices, effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics. This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2024
·
IF 4.2
Xiangyang Chen,Shun Gong,Biao Zhao,Kai Pan
Biobased thermoplastic polyamide elastomers (TPAEs) have received increasing attention in both academia and industry. Here, a series of semi-biobased long-chain TPAEs are successfully synthesized via one-step melt polymerization, employing polyamide 1210 (PA1210) and polyetheramines (PEAs) as hard and soft segments, respectively. The prepared TPAEs demonstrate excellent mechanical properties, energy dissipation capabilities, low density, good damping, high resilience, and low melting temperature. More interestingly, the properties of the TPAEs can be customized by adjusting the content and molecular weight of PEA. By varying the molecular weights of the PEAs, two different thermal behaviors can be observed in the prepared TPAEs. Specifically, PEA with low molecular weight has good compatibility with PA1210, leading to an increase in the conformation of the crystalline region and a significant decrease in melting temperature. Meanwhile, high molecular weight PEA causes strong phase separation with PA1210, leading to limited crystalline regions and inadequate physical cross-linking, further resulting in suboptimal mechanical properties. This work provides new insights into the design and preparation of PEA-type biobased long-chain TPAEs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Luotian Lv,Yao Liu,Yankai Huang,Tong Li,Han Feng,Yongqing Wang
Since the intensification of global environmental pollution and energy shortages, photocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as a promising strategy to convert solar energy into clean chemical energy. Herein, we construct a robust and efficient heterojunction construction photocatalyst for CO 2 RR, composed of the highly reactive CeNi quantum dots (CeNi QDs) and nickel metal–organic layer (Ni-MOL) ultrathin nanosheets. This design facilitates the rapid separation of photogenerated charge carriers, as confirmed by X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and other characterizations. Mechanistic studies with in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and the d-band center calculation indicate that the propensity of photocatalyst for CO 2 absorption and CO desorption, leading to high performance and selectivity. The optimized loading amount of CeNi quantum dots and modified structure result in a CO yield of 30.53 mmol·g −1 within 6 h under irradiation. This work not only paves a new and convenient way for developing high-activity quantum dot materials for CO 2 RR but also exploits novel avenues to fabricate more heterojunction composites for solar energy conversion.
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Foods
·
2024
·Vol. 13
·期 11
·1593
·
IF 4.7
Fangying Xian,Lin Yang,Huaqing Ye,Jinlin Xu,Xiaoping Yue,Xiaolan Wang
Douchi is a Chinese traditional fermented food with a unique flavor. Methyl anthranilate (MA) plays an important role in formation of this flavor. However, the complicated relationship between the MA formation and the metabolic mechanism of the key functional microorganisms remains unclear. Here, we elucidated the response mechanism of aroma production driven by high salt stress inTrichomonascus ciferriiWLW (T. ciferriiWLW), which originates from the douchi fermentation process. The highest production of MA was obtained in a 10% NaCl environment. The enhanced expression of the key enzyme genes of the pentose phosphate pathway and shikimic acid pathway directed carbon flow toward aromatic amino acid synthesis and helped sustain an increased expression ofmetKto synthesize a large amount of the methyl donorS-adenosylmethionine, which promoted methyl anthranilate yield. This provides a theoretical basis for in-depth research on the applications of the flavor formation mechanisms of fermented foods.
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