ACS Catalysis
·
2024
·
IF 11.3
Zaixiang Xu,Fengcang Zhou,Hanchi Chen,Jianguo Wang
The regeneration of NAD(P)H and its analogues is crucial for biocatalytic processes. However, despite the efficiency of enzymatic catalysis in regenerating NAD(P)H, the sustainability of enzymes is often compromised, particularly under extreme catalytic conditions. Moreover, artificial cofactors may present advantages in certain reactions due to their stability and versatility, yet the substrate specificity of enzymes poses significant challenges to their regeneration through the enzymatic method. Therefore, it is imperative to develop a highly stable regeneration method that can be adapted to both natural and artificial cofactors. In this work, employing potassium-ion-doped carbon nitride (ionCN-0.2) as a catalyst not only achieves high-efficiency photocatalytic regeneration of NAD(P)H, comparable to that of glucose dehydrogenase (GDH), but also a remarkable ability to regenerate nicotinamide analogues. This enhanced performance stems from the tunable negative ζ-potential, which effectively adsorbs the positively charged [Cp*Rh(bpy)H2O]2+ mediator, resulting in enhanced regeneration kinetics of the nicotinamide moiety. The catalyst demonstrates superior performance compared to the reported systems; the optimal regeneration rate reaches 0.55 mmol L–1 gcat–1 min–1 and approaches enzymatic regeneration efficiency. Expanding the reaction conditions to a wider temperature and pH range also confirms the effectiveness and sufficient stability of this photocatalytic system, offering a promising strategy for stable cofactor regeneration in biocatalytic processes.
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ChemistrySelect
·
2025
·Vol. 10
·期 7
·e202405464
·
IF 2
Kun Jia,Peng Jia
Graphical The asymmetric activation of anhydrous methanol molecules is realized by exogenous protons, the position and protonation position of asymmetric activation are determined, and the C─H bonding energy and reaction activation energy of some methanol molecules are reduced, and the asymmetric regulation of the non-oxidation dehydrogenation reaction process of anhydrous methanol molecules was realized. The activation of C─H bonds under mild conditions is a crucial step in the conversion of organic molecules. However, the simultaneous activation of C─H bonds in methanol can result in excessive oxidation, thereby diminishing the selectivity for formaldehyde production. We achieved selective activation of the C─H bonds in methanol under mild conditions by adjusting the proton concentration in an anhydrous methanol solution, which significantly enhanced the dehydrogenation rate of methanol. Additionally, we constructed related molecular models to identify the sites of asymmetric oxidation, providing new insights for further studies on C─H bond activation.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Jianning Zhang,Yanpei Dang,Tianhao Li,Yangzhong Zhao,Liantai Duan,Ke Chen,Xiao Zhang,Hengli Duan,Wensheng Yan,Sihua Feng,Gang Shao,Zhaoju Yu,Qing Huang,Yujie Song
Silicon boron carbonitride (SiBCN) ceramics have garnered significant attention due to their exceptional high-temperature stability, resistance to creep, and favorable electrical properties. However, the ceramicization mechanism of covalently bonded boron atoms in polyborosilazane (PBSN), which is crucial in determining the structural and crystalline phase evolution of silicon boron carbonitride (SiBCN) ceramics through the polymer-to-ceramic process, still needs further clarification for the design of advanced ceramics. Therefore, PBSN precursors constructed with B–C bonds were systematically investigated in the polymer-to-ceramic conversion process. B–C bonds were transformed into B-N bonds between 300°C and 600°C, ultimately resulting in the formation of h-BN at high temperatures. Meanwhile, higher levels (8.11–14.12%) of B facilitated the formation of SiC at equivalent temperatures but hindered the formation of Si 3 N 4 crystal nuclei. That is due to the formation of B–N and NB 3 units, which inhibited the formation of Si–N bonds and SiN 4 units, thereby interfering with the nucleation process of Si 3 N 4 and facilitating the crystallization of SiC. This study offers valuable insights for regulating the microphase evolution and properties of PDC nanocomposites.
研究领域:
材料科学
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陶瓷材料
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聚合物衍生陶瓷
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固态化学
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高温材料
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Lu Wang,Hong Li,Yue Dai,Erzhu Sun
Dopamine (DA) can self-polymerize to form polydopamine (PDA) under weak alkaline conditions in the presence of oxygen, creating vibrant structures at the gas–liquid interface. However, the issue of the polydopamine film cracking and easily peeling off from the fabric surface remains unresolved. In this article, we report the rapid polymerization of dopamine in a CuSO 4 /H 2 O 2 system, resulting in the preparation of polydopamine-structured colored cotton fabrics through the stepwise addition of 3-aminopropyltriethoxysilane (KH550) and polyethyleneimine (PEI). Structured color cotton fabrics were hydrophobically treated by a simple impregnation technique using the hydrophobic agent cetyltrimethoxysilane (HDTMS). This improvement suggests that the covalent bonding of PEI with PDA, along with its assembly on the fabric surface, enhanced the homogeneity and continuity of the structural color film, resulting in a brighter and more uniform fabric surface color. After HDTMS treatment, the structural color film on PDA/KH550/PEI-Cotton was converted from a hydrophilic to a hydrophobic state, with a static water contact angle averaging approximately 152.375°. The hydrophobic treatment provided the structural color fabrics with good film stability and resistance to washing, while their surface coloration remained largely unaffected. This method provides a new research idea for eco-dyeing of cotton fabrics.
研究领域:
材料科学
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纺织功能材料
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表面化学
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纳米结构色
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绿色染整技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Yujia Xie,Fengyong Zhang,Pingle Liu,Fang Hao,Hean Luo
Direct functionalization of saturated C–H bonds by metalloporphyrin catalysts is among the topical and challenging areas within the chemical industry and synthetic chemistry. In this work, supported CoD(p-Cl)PPCl metalloporphyrin catalysts were prepared and characterized. It has been found that the CoD(p-Cl)PPCl/ZnO catalyst shows better catalytic activity than the supported catalyst (ZrO2, MCM-41, kaolin, Zr(OH)2, and boehmite (BM)) in cyclohexane oxidation with dioxygen. The effects of the reaction pressure, reaction temperature, and reaction time on the catalytic activity were considered by the supported CoD(p-Cl)PPCl/ZnO catalyst. The CoD(p-Cl)PPCl/ZnO catalyst can be facilely recovered and was recycled up to seven times without a significant decrease in catalytic performance. The average cyclohexane conversion and selectivity to KA oil are 10.98% and 84.34%, respectively, and the turnover number is 2.10 × 107.
研究领域:
催化化学
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有机合成
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工业化学
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材料化学
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绿色化学
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INTERNATIONAL JOURNAL OF FOOD SCIENCES AND NUTRITION
·
2019
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IF 2.792
Yuanfeng Wu,Yuke Shen,Ye Zhu,Jothame Mupunga,Ligen Zou,Chao Liu,Shiwang Liu,Jianwei Mao
After consuming broccoli, isothiocyanates can be produced by the hydrolytic action of myrosinase from plant and/or microbiota. Using male C57BL/6 mice, the present study investigated the effects of broccoli ingestion on the myrosinase-like activity, NAD(P)H:quinone oxidoreductase 1 (NQO1) activity, diversity and composition of the gut microbiota. Compared with the control group, continuously feeding raw or hydrolysed broccoli increased the myrosinase-like activities of the colon and caecum contents, and also improved the NQO1 activity of the colon mucosa. Significant difference between the broccoli and control feeding groups were found. 16S rRNA gene sequencing indicated that broccoli ingestion profoundly affected the composition of the gut bacteria community. The correlation between the gut bacterial community composition and microbiota myrosinase-like activity was also studied. However, one type of glucosinolate, sinigrin, had no effect on these activities, indicating that broccoli component(s), other than glucosinolate, had increased the NQO1 and myrosinase-like activities.
研究领域:
营养学
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微生物学
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分子生物学
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Libin Wang,Ting Shu,Songtao Guo,Shi Chen,Yingjun Jiang,Xianluo Hu
ABSTRACT Owing to sluggish ionic mobility at low temperatures, supercapacitors , as well as other energy-storage devices, always suffer from severe capacity decay and even failure under extreme low-temperature circumstances. Solar-thermal-enabled self-heating promises an attractive approach to overcome this issue. Here, we report a unique H-bonding charge-transfer complex with a high photothermal conversion efficiency of 79.5% at 405 nm based on chloranilic acid and albendazole . Integrated with a microsupercapacitor, the chloranilic acid-albendazole complex (CAC) film prompts an apparent temperature increase of 22.7 °C under 1 sun illumination at −32.6 °C, effectively elevating the working temperature of devices. As a result, the rate capability of the microsupercapacitor has been significantly improved with a 17-fold increase in capacitance at a current density of 60 μA cm −2 , leading to outstanding low-temperature performances. Importantly, the integrated device is capable of working at a low temperature of −30 °C in the open air, which demonstrates the potential of CAC in practical applications for low-temperature ultracapacitive energy-storage devices.
研究领域:
材料科学
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能源存储技术
·
光电化学
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Journal of Materials Research and Technology-JMR&T
·
2025
·
IF 6.6
Zhijun Liu,Junxiang Lu,Meng Xu,Shaochun Li,Anjie Zhou,Yongjuan Geng,Sai Zhang
This study presents the development of h-BN/PDMS composite coatings through hydroxylation treatment and modification of hexagonal boron nitride (h-BN) using a vinyl silane coupling agent. The study aims to address the limitations of conventional PDMS coatings, specifically their inadequate mechanical strength and poor resistance to weathering. The innovation lies in the improved dispersion of h-BN within the PDMS matrix, which was achieved via the surface grafting of vinyl groups. This approach, combined with the intrinsic layered structure and high thermal conductivity of h-BN, led to a synergistic enhancement in the mechanical performance and protective functionality of the coating. Experimental results demonstrated that incorporating 8% modified h-BN increased the tensile strength of the coating to 5.206 MPa, an improvement of 110.6% over pure PDMS, and reduced erosion depth to 2.7 μm. Furthermore, the coating exhibited minimal adhesive strength loss after UV aging (from 1.085 to 1.012 MPa). Under acidic conditions (pH = 2), the composite coating reduced the mortar strength loss by 53.1%. In seawater immersion and 25 freeze-thaw cycles, the mass loss rates of the test blocks decreased by 55.9% and 90.4%, respectively. In addition, the high UV reflectance (97.6%) and oxygen barrier properties of h-BN significantly mitigated the photo-oxidative degradation of the PDMS matrix. This study proposes a theoretical foundation and process optimization strategy for designing high-performance protective coatings suitable for use on concrete and electronic components in extreme environments.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Yuan-Yang Guo,Ze-Hua Tian,Yu-Chen Han,Dandan Ma,Tianju Shao,Zhiyong Jiang
Graphical Chemically stable Hantzsch ester is discovered to be an efficient and economical NAD(P)H mimic as sacrificial electron source in in vitro bioconversions. Biocatalysis has emerged as a valuable and reliable tool for industrial and academic societies, particularly in fields related to bioredox reactions. The cost of cofactors, especially those needed to be replenished at stoichiometric amounts or more, is the chief economic concern for bioredox reactions. In this study, a readily accessible, inexpensive, and bench-stable Hantzsch ester is verified as the viable and efficient NAD(P)H mimic by four enzymatic redox transformations, including two non-heme diiron N -oxygenases and two flavin-dependent reductases. This finding provides the potential to significantly reduce the costs of NAD(P)H-relying bioredox reactions.
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高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 6
Peng Chu,Lindong Ma,Hongli Liu,Zongwei Zhang,Yuhao Liu,Weiqiang Xie,Wenshuo Cao,Mingwei Li,Yuanhang Zhou
Aluminum borate fibers are promising candidates for high-temperature thermal insulation owing to their excellent thermal stability, good chemical resistance, and relatively low density. Herein, we report a simple method for preparing porous Al 18 B 4 O 33 /h-BN composite fibers via electrospinning and stepwise heat treatment, using an aluminum isopropoxide/aluminum nitrate (AIP-AN) complex as the aluminum source and nanoscale h-BN as the boron source. The incorporation of h-BN not only promotes the in-situ formation of the Al 18 B 4 O 33 phase but also affects the fiber's pore structure. Meanwhile, the heterogeneous interface formed between h-BN and the Al 18 B 4 O 33 may introduce additional interfacial thermal resistance, thereby synergistically reducing thermal conductivity and improving thermal insulation performance. The resulting composite fibers exhibited a highly porous structure, with a high specific surface area of 53.9175 m 2 g −1 , a low density of 0.025 g cm −3 , and a low thermal conductivity of 0.0417 W m −1 K −1 . The porous Al 18 B 4 O 33 /h-BN composite fibers demonstrate significant potential for thermal insulation in extreme environments, offering a viable approach to developing high-performance ceramic fiber insulation materials.
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MOLECULES
·
2026
·Vol. 31
·期 15
·2595
·
IF 5.1
Jie Chen,Ying Zhou,Yishao Wang,Fujing Huang,Fangming Zou,Shunmei He,Xianwen Song
Small-molecule blending is an effective strategy for improving the mechanical properties of poly(vinyl alcohol) (PVA). However, the influence of structural differences among phenolics on the toughening mechanism remains unclear. In this study, we systematically investigated the reinforcing effects of three trihydroxy-phenolics (apigenin, galangin, and baicalein) on PVA hydrogels by combining molecular simulations with experimental validation. Molecular simulations predicted that H-bonding crosslinking between phenolics and PVA chains is the central reinforcement mechanism, and that the spatial arrangement of hydroxyl groups and the competition between intermolecular H-bonding ultimately determine the performance. Structural characterization and experimental validation showed that apigenin, owing to the dispersed spatial distribution of its three hydroxyl groups, exhibits stronger H-bonding crosslinking ability and achieves the most significant reinforcement. After a single freeze–thaw cycle, all trihydroxy-phenolics/PVA composite hydrogels exhibited markedly better mechanical properties than pure PVA hydrogels, with the following strength order: apigenin/PVA > galangin/PVA ≈ baicalein/PVA. This study provides a rapid and efficient theoretical model and a reference case for small-molecule toughened PVA hydrogels.
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CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Yiwei Zhao,Zuhang Jin,Cheng Tao,Rui Du,Yongzheng Shi,Chao Zhang
The synthesis of KA oil (a cyclohexanone-cyclohexanol mixture) from guaiacol through mild electrocatalytic approach represents a sustainable strategy for biomass valorization. Herein, we report the electrocatalytic conversion of guaiacol to KA oil over the reduced Pt/TiO 2 catalysts. The TiO 2 -induced hydrogen spillover effect facilitates strategic modulation of H ads (H*) coverage on Pt surfaces, thereby effectively suppressing competitive aromatic ring hydrogenation and excessive hydrogen evolution reactions. Comparative studies of electrocatalysis and thermocatalysis have demonstrated that Pt active sites serve as the dominant catalytic centers. However, H spillover significantly influences reactivity and selectivity, particularly in the electrocatalytic pathways. The electrocatalytic system demonstrates preferential C–O bond cleavage with KA oil selectivity around 70%. This work provides valuable insights into the regulation of metal-support interactions in the design of electrocatalysts.
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