ACS Applied Polymer Materials
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2025
·
IF 4.7
Yu Han,Qiang He,Yuqun Fang,Jingkai Nie,Weinan Qin,Hao Liu,Kai Zhu
Phase change materials (PCMs) offer great potential for realizing zero-energy thermal management due to superior cold storage and stable phase change temperatures. However, the widespread use of PCMs is consistently impeded by issues such as liquid leakage and solid rigidity. Here, we present a simple yet effective strategy for developing highly flexible polymer-based phase change materials. Our approach involves creating a dual three-dimensional (3D) cross-linked network of acrylamide (AM) and sodium alginate (SA) within a poly(vinyl alcohol) (PVA) matrix. The synergy between H-bonds and AM-SA networks significantly enhances the mechanical strength, thermal stability, and leakage resistance of PVA@AM-SA. Our research offers a promising approach to designing phase change materials with both high latent heat capacity and exceptional mechanical strength, making them ideal for use in wearable thermal management applications.
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ORGANOMETALLICS
·
2020
·
IF 3.804
Liangwei Zhang,Long Liu,Tianzeng Huang,Qizhi Dong,Tieqiao Chen
A palladium-catalyzed cyclobutanation of aryl sulfonates with strained alkenes has been developed. The methodology is featured to achieve the cleavage of both C–O and C–H bonds of phenol derivatives in one pot. Under the reaction conditions, in addition to reactive triflates, the relatively inactive tosylates and mesylates can also be transformed into the corresponding benzocyclobutanes in high yields. This reaction can be carried out in gram-scale experiments with a low loading of the palladium catalyst and is applicable to the cyclobutanative modification of bioactive molecules, highlighting its synthetic value in organic synthesis.
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JOURNAL OF ORGANIC CHEMISTRY
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2023
·
IF 3.6
Huanhuan Song,Jingwen Li,Yinbin Zhang,Ke Chen,Le Liu,Junjie Zhang,Xin-Hua Duan,Mingyou Hu
Difluoromethylated heterocyclic compounds have found broad applications in numerous bioactive molecules. Herein, we report photoredox catalysis-induced direct C–H difluoromethylation of heterocycles by using bis(difluoromethyl) pentacoordinate phosphorane (PPh3(CF2H)2, 1) as the reagent. A variety of heterocycles, such as quinoxalin-2(1H)-one, thiophene, indole, and coumarin, are readily tailored with a difluoromethyl group. The method is featured as transition-metal-free by using an organic compound Erythrosin B as the catalyst and O2 as the oxidant.
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PubMed
高影响因子
PROGRESS IN ORGANIC COATINGS
·
2021
·
IF 5.161
Beibei Chen,Zhe Dong,Jiaye Li,Mengjie Zhang,Kan Zhang
Hexagonal boron nitride (h-BN) is a promising additive used in tribology ; however, its application is limited due to its poor interfacial combination with polymer matrices induced by its inert and smooth surface. In order to tackle this problem, an innovative ZnO nanowires-decorated h-BN hybrid was first prepared, which was then applied onto epoxy (EP) to enhance its tribological properties. The results demonstrated that ZnO nanowires were in-situ grown uniformly on the exterior of the hydroxylated h-BN, which strengthened the physical and chemical interaction between h-BN and EP, since the EP chains were prone to wrap around the ZnO nanowires. When the h-BN/ZnO content was 0.5 wt%, the friction coefficient and wear rate were decreased by 81.5% and 95.4%, respectively, and the corresponding composite coating possessed superior tribological properties under harsh conditions, which was mainly because of the synergistic reinforcing and lubricating effect between the ZnO nanowires and h-BN, as well as the good interfacial compatibility between h-BN/ZnO hybrid and EP. Moreover, the corresponding enhancement mechanisms of h-BN/ZnO were proposed.
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Surfaces and Interfaces
·
2024
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IF 5.7
Zhiwei Zou,Hongxiang Zhang,Xuefeng Pan,Hui Shen,Jianying Yu,Tengfei Guo,Yonghao Wang
Electrocatalytic reduction of nitrate (NO 3 - ) to ammonium (NH 4 + ) is an environment friendly approach for treating nitrogen-containing wastewater. Consequently, electrocatalysts capable of effectively and selectively reducing NO 3 - to NH 4 + receives growing attention. However, Cu-based catalysts demonstrate limited efficiency and the drawback of generating toxic NO 2 - though it is prevalent in the field of electrocatalytic reduction of NO 3 - (NO 3 RR). In this work, a CuNi alloy was synthesized on a Co foil through electrodeposition (marked as CuNi@Co) and its electrocatalytic performance for NO 3 RR was evaluated. XRD, EDS mapping and XPS characterization indicate CuNi exists with alloy state. Electrocatalytic experiments demonstrate that CuNi@Co exhibits an exceptional FE NH3 of 99.12% at -0.64 V (vs. RHE). Importantly, no detrimental NO 2 - generated during NO 3 RR process because the reduction rate from NO 2 - to NH 4 + is faster than that from NO 3 - to NO 2 - . Mechanistic analysis suggests that Cu serves as a ‘reservoir’ to provide electrons to facilitate the reduction of NO 3 - to NO 2 - during NO 3 RR process and the synergistic effect of Ni and Cu promotes more active hydrogen (H*) to participate the reduction process of NO 2 - to NH 4 + not H 2 generation, ultimately improving FE NH3 . This work elucidates the role of electrons and H* in electrocatalytic nitrate reduction to ammonium for CuNi alloy, providing new insights into the reduction process of NO 3 RR for Cu-based materials.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Ling Ding,Lou Gao,Di Pan,Ke Du,Jiayu Yu,Wanyi Li,Yahong Zhang,Yi Tang
The utilization of racemic lactic acid (rac-LA) produced via chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (meso-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of meso-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L2A) in a one-step catalytic conversion of rac-LA to LD. Experimental results from various LA solutions with different L2A content indicate that the L2A content is critical for maximizing the selectivity of racemic lactide (D/L-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L2A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease meso-LD formation, and a LD yield of 60% with a D/L-LD/meso-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of D/L-LD and meso-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from rac-LA derived from chemical conversion.
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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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RENEWABLE ENERGY
·
2024
·
IF 9
Huajing Zhou,Tiancheng Li,Fawen Zhang,Faze Chen,Zilian Liu,Rongrong Miao,Qingqing Guan,Lingxiang Zhao,Liang He
Intrinsic point defects in metal core-shell materials can regulate electron redistribution, thereby reducing catalytic energy barriers and enhancing their ORR activity. However, their specific contributions to electron transfer and mass transport pathways remain unclear. In this study, defect-rich hollow O Co @Co 3 O 4 nanoparticles were successfully synthesized using ZIF-67(Co) as a sacrificial template through controlled annealing and internal electric field substitution reactions. High-resolution electron microscopy analysis and density functional theory (DFT) calculations co-revealed the growth mechanism of Co and O vacancies, as well as antisite defects. The formation of oxygen vacancies significantly lowered the energy barrier for Co vacancy formation, playing a crucial bridging role in the development of antisite defects. The electric field polarization induced by Co-O atomic displacement resulted in asymmetric charge distribution, optimizing the adsorption of active hydrogen (H*) and oxygen atoms and facilitating the generation and release of reactive oxygen species (ROS). Electrocatalytic experiments demonstrated that under the combined action of singlet oxygen ( 1 O 2 ) and H*, bisphenol A (BPA) can be efficiently degraded. This study successfully bridges the knowledge gap between atomic defects and advanced electrocatalysis, providing a new perspective and insight for the in-depth analysis of the structure-performance relationship of electrocatalyst materials in the future.
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Joule
·
2020
·
IF 29.155
Anyi Mei,Yusong Sheng,Yue Ming,Yue Hu,Yaoguang Rong,Weihua Zhang,Shulin Luo,Guangren Na,Chengbo Tian,Xiaomeng Hou,Yuli Xiong,Zhihui Zhang,Shuang Liu,Satoshi Uchida,Tae-Woong Kim,Yongbo Yuan,Lijun Zhang,Yinhua Zhou,Hongwei Han
Summary The stability of perovskite solar cells (PSCs) has been considered as the largest obstacle to their commercialization. Herein, we observed that the main failure mechanism for MAPbI 3 perovskite is the escape of methylammonium (MA) iodide at the grain boundaries in an open space or the reconstruction of crystal in a confined small space, as well as the irreversible long-distance ionic migration under the multiple actions of light, heat, and electrical bias. Strengthened with bifunctional organic molecular of 5-ammoniumvaleric acid (5-AVA) iodide at the grain boundaries, the MAPbI 3 crystal was localized in the nanoscale, and thus, the decomposition or reconstruction was inhibited and the ionic migration became reversible. As a result, we propose a reliable approach to make PSCs meet stability standards of IEC61215:2016 qualification tests. A printable PSC filled with (5-AVA) X MA 1-X PbI 3 has been working for more than 9,000 h at a maximum power point of 55°C ± 5°C without obvious decay.
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ACS Catalysis
·
2025
·
IF 13.1
Yu-Yang Liu,Shan Xu,Xiao-Xin Li,Run-Han Li,Xin-Ting Cai,Hui-Zhen Zhong,Jiang Liu,Qing Huang,Lei Zhang,Shun-Li Li,Ya-Qian Lan
Developing strategies and photocatalysts for C(sp3)-H bond functionalization under simple and mild conditions is important but challenging. Here, we report two redox heterocluster-based frameworks, named Ni5-PW12 and Ni5-V16, in which the terminal oxygen atoms of polyoxometalates are directly coordinated to metal atoms in metal–organic clusters. Due to the coexisting strong oxidation and reduction capacities, both of these photocatalysts achieve photocatalytic C(sp3)-H bond oxidative imination through combining oxidation of methyl aromatics and reduction of nitro aromatics reactions. The experimental and theoretical results reveal that benefiting from the short distance between the clusters, the rapid charge transfer and mass transfer processes would enhance the photocatalytic reactivity and inhibit side reactions. More importantly, all of the photocatalytic reactions are carried out in mild conditions at room temperature without any additional solvents, photosensitizers, oxidizing or reducing agents, or cocatalysts.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2024
·Vol. 149
·期 23
·13759-13771
·
IF 3
Li Wenjie,Long Jiangfeng,Liu Sijia,Wang Peng,Xu Linglin,Lai Yong
To assess the feasibility of using C-S–H seeds to boost the anti-mechanical vibration capabilities of concrete, this work evaluated the mechanical properties, hydration kinetics, phase assemblage of hydrates, and pore structure of Portland cement (PC) and slag cement mortars, at varying dosages of C-S–H seeds. Results reveal that the incorporation of C-S–H seeds negatively affects the vibration resistance of neat PC, while it effectively enhances the vibration resistance of slag cement. The addition of these seeds facilitates cement hydration and improves the early mechanical properties, which is evident in the shortened appearance time of the hydration exothermic peak by almost 50%. The remarkable vibration resistance observed in slag cement primarily stems from the synergistic effect between C-S–H seeds and slag. However, the premature formation of the internal microstructure in neat PC due to C-S–H seeds disrupts the stability of mutual construction between hydration products. The findings indicate that C-S–H seeds can be used in engineering to enhance concrete lifespan, reduce road repair expenses, and enhance construction efficiency.
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