CATALYSIS LETTERS
·
2024
·
IF 2.3
Shao Yulin,Xie Ping,Han Yuning,Zhong Tianhao,Li Tao,Yu Yingmin,Zhao Qingshan,Li Zhongtao
In response to the problem that the conventional concentrated sulfuric acid catalyst for esterification reactions are prone to corrosion and generate large amounts of acid-containing wastewater, highly efficient gel resin-loaded ionic liquid solid acid (SA-ILs) catalysts were prepared by a one-pot method of loading ionic liquids onto gel resins. It is shown that the gel resin carrier has a strong water-absorbing structure, and the ionic liquids are covalently loaded on the gel resin carrier through chemical bonding, leading to SA-ILs catalysts with excellent acidity and good structural stability. With an optimal ionic liquid loading of 11% and acid density of 3.25 mmol·g −1 ,the synthesized SA-ILs catalysts showed good catalytic performance in the transesterification reaction between acetic acid and ethanol at 80 °C for 1.5 h. The catalyst dosage was 10 wt% of the total mass of acetic acid and ethanol, and the ethanol to acetic acid addition was at a molar ratio of 1.5:1. Ethyl acetate yields of up to 81% were achieved after the reaction. The catalyst also showed slightly decrease of the catalytic performance after reused for five cycles. The lower activation energy of the catalyst is proved to be the key to facilitate the catalytic transesterification reaction. Graphical Abstract
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Cong Peng,Yutong Sui,Chaohua Fang,Hongxu Sun,Wenxin Liu,Xinying Li,Chen Qu,Wenhui Li,Jiemin Liu,Chuandong Wu
Recently, various biosensors based on odorant-binding proteins (OBPs) were developed for the detection of odorants and pheromones. However, important data gaps exist regarding the sensitive and selective detection of aldehydes with various carbon numbers . In this work, an OBP2a-based electrochemical impedance spectroscopy (EIS) biosensor was developed by immobilizing OBP2a on a gold interdigital electrode, and was characterized by EIS and atomic force microscopy . EIS responses showed the OBP2a-based biosensor was highly sensitive to citronellal , lily aldehyde, octanal , and decanal (detection limit of 10 −11 mol/L), and was selective towards aldehydes compared with interfering odorants such as small-molecule alcohols and fatty acids (selectivity coefficients lower than 0.15). Moreover, the OBP2a-based biosensor exhibited high repeatability (relative standard deviation: 1.6%–9.1 %, n = 3 for each odorant), stability (NIC declined by 3.6 % on 6th day), and recovery (91.2%–96.6 % on three real samples). More specifically, the sensitivity of the biosensor to aldehydes was positively correlated to the molecular weight and the heterocyclic molecule structure of the odorants. These results proved the availability and the potential usage of the OBP2a-based EIS biosensor for the rapid and sensitive detection of aldehydes in aspects such as medical diagnostics, food and favor analysis, and environmental monitoring.
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MACROMOLECULES
·
2024
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IF 5.1
Hai Li,Yang You,Chun Hui Xie,Yun Qi Li,Hai Bo Xie
Despite the significant attention that biobased polymers have garnered, the potential value of the intrinsic structural characteristics inherited from biomass in the molecular design of these polymers remains underexplored. In this study, a noncoplanar triaryl-imidazole was designed to serve as a curing agent for high-performance epoxy adhesives. The curing behavior can be modulated through the conjugative effects of the aryl groups and the electron-donating properties of the methoxy groups, both of which are inherited from lignin. Furthermore, both theoretical and experimental results indicate that π–π stacking interactions involving the aromatic rings, cation–π interactions involving the imidazolium cation, and hydrogen bonds involving the methoxy groups coexist within the cured resins, thereby forming a multivalent supramolecular network centered around the lignin-derived noncoplanar triaryl-imidazolium. As a result, the system demonstrates a high glass transition temperature (TgDMA = 230.85 °C), enhanced strength and toughness, strong adhesion, and a wide working temperature range (−196 to 200 °C). These findings contribute to the establishment of structure–property relationships for lignin-based polymers and provide valuable insights for the rational design of biobased chemicals and polymers.
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Small Methods
·
2024
·
IF 10.7
Aiping Zhang,Shujie Tie,Xiaojuan Lu,Wanjia Tian,Zhenghui Fan,Siyin Dong,Ruihan Yuan,Congcong Wu,Xiaojia Zheng
Perovskite X-ray detectors are recognized as the most promising candidates for low-dose detectors due to their superior performance. However, it is still full of challenging in the fabrication of flat-panel X-ray imagers (FPXIs), primarily due to the absence of large area thick films that exhibit high uniformity and long-term performance stability. A general synthesis route is urgently needed to grow large-scale halide perovskite thick films directly on a pixeled thin-film transistor (TFT) backplane with high uniformity, closing the gap between the great potential of perovskite X-ray detectors and their entry into the market. In this work, an advanced precursor paste suitable for blade coating is developed to enable high-throughput manufacturing of FPXIs. Highly uniform perovskite films with a thickness of 300-micrometers are directly deposited onto pixeled TFT substrates by the blade-coating method using the above paste, which governs a stable dark current and minimal noise of the X-ray detectors. As a result, (BA) 2 (MA) 9 Pb 10 I 31 perovskite X-ray detectors achieved a high sensitivity of 15200 µC Gy air −1 cm −2 and a limit of detection (LoD) of 26.8 nGy air s −1 . Moreover, FPXIs with a spatial resolution of 0.95 lp mm −1 (0.475 lp pixel −1 ) are obtained, which exhibits negligible signal crosstalk and excellent X-ray imaging performance.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
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IF 5.7
Chen-Lu Xu,Chen-Yuan Zhu,Yang-Nan Li,Jian Gao,Ye-Wang Zhang
A novel heparinase III from Pedobacter schmidteae (PsHep-III) with high activity and good stability was successfully cloned, expressed, and characterized. PsHep-III displayed the highest specific activity ever reported of 192.8 U mg–1 using heparin as the substrate. It was stable at 25 °C with a half-life of 323 h in an aqueous solution. PsHep-III was employed for the depolymerization of heparin, and the enzymatic hydrolyzed products were analyzed with gel permeation chromatography and high-performance liquid chromatography. PsHep-III can break glycosidic bonds in heparin like →4]GlcNAc/GlcNAc6S/GlcNS/GlcNS6S/GlcN/GlcN6S(1 → 4)ΔUA/ΔUA2S[1 → and efficiently digest heparin into seven disaccharides including N-acetylated, N-sulfated, and N-unsubstituted modification, with molecular masses of 503, 605, 563, 563, 665, 360, and 563 Da, respectively. These results indicated that PsHep-III with broad substrate specificity could be combined with heparinase I to overcome the low selectivity at the N-acetylated modification binding sites of heparinase I. This work will contribute to the application of PsHep-III for characterizing heparin and producing low-molecular-weight heparin effectively.
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ChemistrySelect
·
2024
·Vol. 9
·期 40
·e202403878
·
IF 1.9
Haifeng Liao,Jianwei Guo
Graphical Three kinds of heteropoly acid-based ionic liquids with different Hammett acidity were prepared for the catalytic conversion of cellulose to levulinic acid, and the effects of different solvent systems on the catalytic reactions were investigated. The results showed that higher Hammett acidity was beneficial to increase the yield of levulinic acid, and GVL/H 2 O bi-phase solvent system was helpful to extract the product to the organic phase and promote the formation of levulinic acid. Levulinic acid is an important chemical intermediate, which has many applications in organic synthesis, industry, agriculture, and medicine. In this word, three kinds of heteropoly acid based ionic liquids ([IMPS]H 2 PW 12 O 40 、[PyPS] H 2 PW 12 O 40 [TEAPS] H 2 PW 12 O 40) were used to catalyze the one-pot conversion of cellulose to levulinic acid. [IMPS]H 2 PW 12 O 40 has the highest catalytic activity due to its strong Hammett acidity ( H 0 ). In addition, the effect of biphasic solvent systems on the conversion of cellulose to levulinic acid was also studied. The results showed that the GVL/H 2 O system could effectively promote the conversion of cellulose and increase the yield of levulinic acid. The yield of levulinic acid could reach 52.6% and the conversion rate of cellulose was 91.2% at 180 °C for 180 min under the GVL/H 2 O volume ratio of 1:1 with [IMPS]H 2 PW 12 O 40 as a catalyst at 1 Mpa N 2 and cellulose as raw material. And [IMPS]H 2 PW 12 O 40 can be recycled up to five times without significant performance loss. This study provides a promising method for efficiently converting cellulose and other biomass resources to levulinic acid extraction.
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JOURNAL OF ORGANOMETALLIC CHEMISTRY
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2025
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IF 2.4
Ke Yang,Sisi Cheng,Shijia Li,Kun Zhu,Ziqin Yao
The influencing factors of ZIF-8 synthesis were systematically investigated by the green synthesis method and the samples were also compared with ZIF-8 synthesized in other ways, and an optimal synthesis route was found by exploring the synthesis conditions. On this basis, the synthesis mechanism of ZIF-8 was analyzed. The research results show that the key influencing factors in the reaction process are the amount of NaOH and the pH value of the system. Different amounts of NaOH will produce different intermediates, and these intermediates further affect the pH value of the entire reaction system. The pH value of the system plays a decisive role in the deprotonation process of the ligand in the reaction, and this process is the key to whether the ZIF-8 structure can be formed. It is worth mentioning that the ZIF - 8 synthesized in this study demonstrates varying removal performances for different dyes under different conditions. Under specific conditions, it exhibits the maximum removal rate for Rhodamine B (RhB), reaching 99.97 %. This excellent removal performance is closely associated with the pore - structure characteristics of the synthesized material, which fully indicates that the ZIF - 8 synthesized through the green route has certain application potential and promising application prospects in related fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yuanyuan Cui,Jianmin Sun
Developing a highly efficient catalyst for the conversion of CO 2 into cyclic carbonate is crucial for achieving carbon neutrality. Incorporating target-specific active sites into solid catalysts represents a novel and promising strategy for enhancing the chemical conversion of CO 2 . In this study, the original UiO-66-NH 2 was post-synthetically modified by replacing the H atom of –NH 2 functional group in UiO-66-NH 2 with the Br group in 1-bromobutylimidazole (BIm) under alkaline conditions. Subsequently, the imidazole group in UiO-66-NH 2 -BIm was quaternized with bromoalkyls (including 3-bromopropionic acid, 2-bromoethanol, and 2-bromoethylamine hydrobromide), resulting in the synthesis of UiO-66-NH 2 modified by ionic liquids (ILs) containing hydrogen bond donors, denoted as IL-R@UiO-66-NH 2 (where R OH, NH 2 , COOH). The catalytic performance was assessed in the absence of cocatalyst and solvent at 100 °C, 5 h and 1.0 MPa CO 2 . Notably, IL-COOH@UiO-66-NH 2 exhibited the highest catalytic performance, achieving propylene carbonate yield of 96.1 %. This outstanding performance was attributed to the synergistic interactions between the Lewis acidity of the MOF node, the strong nucleophilicity provided by the Br − of the IL, and the hydrogen bonding interaction facilitated by the carboxyl group, Lewis basic N site from the IL cation. Additionally, IL-COOH@UiO-66-NH 2 demonstrated compatibility with a wide range of epoxy substrates and exhibited good recyclability.
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Journal of Materials Chemistry C
·
2025
·
IF 5.1
Taoli Deng,Zan Ding,Shuang Zheng,Rong-Jun Xie
Ce3+-doped nitride phosphors are promising color converters in laser-driven lighting and display technologies, but they suffer from serious loss in luminescence efficiency caused by the interfacial reaction between phosphor powders and glass powders during the fabrication of phosphor-in-glass bulks or films. In this work, the oxygen-free organic–inorganic hybrid glass (OIHG) Zn(Im)3(HbIm) (ZIF-62) was used instead of the traditional oxide glass to prepare an La3Si6N11:Ce3+ (LSN) phosphor converter by cofiring LSN with the ZIF-62 glass. The LSN phosphor-in-ZIF-62 glass converter well maintains the internal quantum efficiency of the original phosphor powders, showing a luminescence loss of only ∼1%. The sandwich-structured LSN-in-ZIF-62 glass converter, constructed by cofiring it with sapphire substrates, enables the generation of white lighting with a maximum luminous flux of 872.2 lm and a luminous efficacy of 291 lm W−1 when pumped by a blue laser diode at a powder density of 5.99 W mm−2. The use of the oxygen-free ZIF-62 glass provides a viable method to design nitride phosphor-based color converters for low-power laser-driven lighting, high-power LED lighting or projection applications.
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MACROMOLECULES
·
2025
·
IF 5.2
Yuming Deng,Jiahui Zhou,Mengjie Si,Gaopeng Wang,Yueman Tang,Zi Rong Zhang,Jiayu Hu,Yan-jie Wang,Jintao Yang,Si Yu Zheng
Polyzwitterionic gels possess a high density of ionic groups and present great potential in ionotronics. However, zwitterionic chains are easy to be highly hydrated, leading to weak interchain interactions and a poor mechanical performance. Although metal ions like Fe3+ show great effectiveness in toughening hydrogels, they usually weaken the zwitterionic gel inversely due to the anti-polyelectrolyte effect. Herein, a special co-ion effect of Fe(ClO4)3 is found, which is adopted to toughen the zwitterionic hydrogel. In contrast to the weak effect of Fe(NO3)3, FeBr3, and FeCl3 salts on gel toughness, Fe(ClO4)3 can toughen the imidazolium-based polyzwitterion (pVBIPS) effectively. The Fe(ClO4)3-treated pVBIPS gel exhibits a high ultimate tensile stress of 1.34 MPa, a Young’s modulus of 1.2 MPa, and tensile work of 2.29 MJ/m3, surpassing many existing pure zwitterionic hydrogels. It is found that the ClO4– ions can effectively bind to the imidazolium moiety of pVBIPS and promote the formation of SO3––Fe3+ interactions; the trivalent Fe3+ ions can then bridge multiple sulfonate groups to impart the strength. This work should offer a new strategy for developing tough zwitterionic hydrogels.
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TALANTA
·
2025
·
IF 6.1
Yifei Ma,Lijie Zhang,Hong Yang,Shanshan Zhu,Jinhua Liu
Highly selective and sensitive determination of dopamine (DA) from multiple sources remains a persistent and significant challenge. Here, we develop an imidazole-triggered in situ fluorescence reaction system for highly selective and sensitive determination of DA from various sources (human, horse, dog, rabbit, and mouse). The system operates by catalyzing the oxidation of DA with 1,5-Dihydroxynaphthalene (1,5-DHA) through a Lewis base formed by imidazole, leading to the rapid generation of yellow azamonardine fluorescent compounds (AFC). Notably, the system demonstrates minimal background noise and a high signal-to-noise ratio of up to 300-fold with a determination limit of 33.33 pM, making it 10-100 times more sensitive than conventional enzyme-linked immunosorbent assay (ELISA) methods. Moreover, selectivity tests reveal that our system can effectively distinguish between several common interfering substances, even at concentrations as low as 10 nM. The developed system shows promising results in detecting DA from diverse sources (humans, horses, dogs, rabbits, and mice), including urine samples from clinical patients, exhibiting good agreement with traditional ELISA kits. Therefore, the established in situ fluorescence reaction system holds great potential for the determination of DA-related disorders due to its impressive analytical capabilities.
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NANOTECHNOLOGY
·
2024
·
IF 2.9
Yuhai He,Chen Wang,Qiuhua Wu,Guolin Zhang
In this paper, a new Janus-structured nano drug delivery carrier Fe3O4@TiO2&mSiO2 was designed and synthesized, which consisted of a spherical head and a closely connected rod. The head was a nanocomposite of core/shell structure with magnetic spinel ferric tetraoxide core and anatase titanium dioxide shell (Fe3O4@TiO2), and the rod was ordered mesoporous silica (mSiO2). The nanocarriers showed excellent magnetic targeting capability (saturation magnetization, 25.18 emu g-1). The core/shell heads endowed the carriers with fine microwave responsiveness. The pore volume of mesoporous nanocarriers was 0.101 cm3 g-1, and the specific surface area was 489.0 m2 g-1. Anticancer drug doxorubicin could be loaded in the mesoporous of the carriers to form Fe3O4@TiO2&mSiO2-DOX. The drug loading capacity was 10.4%. Fe3O4@TiO2&mSiO2-DOX exhibited acid-sensitive and microwavesensitive release properties along with good bio-compatibility. Fe3O4@TiO2&mSiO2 Janus nanoparticles are expected to be ideal drug carriers.
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