Green Energy & Environment
·
2025
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IF 14.6
Xiang Hui,Jianhui Shi,Jiajun Zhang,Yan Cao,Huiquan Li,Peng He,Liguo Wang
The carbonylation of amines offers a promising route for synthesizing N-substituted carbamates with high atom economy. However, conventional catalysts exhibit limited catalytic efficiency, and the underlying proton transfer mechanism remains elusive. Herein, we reported a metal-free, room-temperature strategy utilizing 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) as a dual hydrogen bond catalyst to synergistically activate propylamine (PA) and dimethyl carbonate (DMC). This green catalytic system achieves a 10-fold acceleration in reaction rate compared to other hydrogen bonding catalysts under mild conditions. This is enabled by dual hydrogen bonding of TBD with PA and DMC, which facilitates rapid proton transfer and stabilizes tetrahedral intermediates. Theoretical calculations confirm that the dual hydrogen bond system significantly lowers activation energy compared to single hydrogen bond analogs. Furthermore, it was revealed that the hydrogen bonding network within the product is the primary factor responsible for the sluggish reaction rate. This study demonstrates the effectiveness of a dual hydrogen bond system in accelerating the carbonylation of amines and provides a green route to access carbamates.
研究领域:
化学
·
催化科学
·
有机合成
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产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Liu Yang,Shang Huishan,Zhang Bing,Yan Dongpeng,Xiang Xu
The C–C bond cleavage of biomass-derived glycerol to generate value-added C1 products remains challenging owing to its slow kinetics. We propose a surface fluorination strategy to construct dynamic dual hydrogen bonds on a semiconducting BiVO 4 photoelectrode to overcome the kinetic limit of the oxidation of glycerol to produce formic acid (FA) in acidic media. Intensive spectroscopic characterizations confirm that double hydrogen bonds are formed by the interaction of the F–Bi–F sites of modified BiVO 4 with water molecules, and the unique structure promotes the generation of hydroxyl radicals under light irradiation, which accelerates the kinetics of C–C bond cleavage. Theoretical investigations and infrared adsorption spectroscopy reveal that the double hydrogen bond enhances the C=O adsorption of the key intermediate product 1,3-dihydroxyacetone on the Bi–O sites to initiate the FA pathway. We fabricated a self-powered tandem device with an FA selectivity of 79% at the anode and a solar-to-H 2 conversion efficiency of 5.8% at the cathode, and these results are superior to most reported results in acidic electrolytes.
研究领域:
材料科学
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光电化学
·
催化反应
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产品关联
DOI
PubMed
高影响因子
ACS Applied Polymer Materials
·
2021
·
IF 4.089
Qilong Zhou,Lisong Dong,Jian Wu,Yijun Shi,Xin Feng,Xiaohua Lu,Jiahua Zhu,Liwen Mu
From one to more, the same raw materials giving rise to multifarious products is one of the goals of researchers to pursue industrial efficiency. Herein, we designed a formula (controlling the content of the matrix) to prepare two functional ionic gels, integrating the excellent lubrication, thermal conductivity, and self-healing ability to meet different industrial demands of the lubrication and biomedical fields. Deep eutectic solvents (DESs) of urea/choline chloride (UCC) and glycerol/choline chloride (GCC) were locked in polyacrylamide (PAM) ionic gel formed by acrylamide (AM) and a photoinitiator by free-radical polymerization. The unique dual hydrogen bond network in the ionic gel causes the material to exhibit a low wear rate, which can effectively reduce the wear of metal contact. With the addition of PAM, the ionic gel has excellent mechanical strength and good recovery performance. Unexpectedly, this dense hydrogen bond network enhances thermal conductivity by optimizing phonon and electron transfer. The versatile ionic gel has a good application prospect as a substitute for industrial lubricants and medical device materials.
研究领域:
材料科学
·
生物医学工程
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DOI
高影响因子
Progress in Natural Science-Materials International
·
2025
·
IF 7.1
Lingke Li,Fangli Xiao,Wenqiang Ai,Shilong Dong,Ruiqi Wang,Yanan Zheng,Hongyu Ji,Yang Liu,Lei Zu,Huiqin Lian
Black phosphorus (BP) has advantages over silicon and graphite in high-capacity fast charging. However, BP faces challenges such as low conductivity and volume expansion. Although composites of BP and graphite (G) can alleviate these problems to a certain extent, it is difficult to maintain the high performance of batteries at high current densities with conventional single binder systems. In this study, an innovative dual hydrogen bonding cross-linking strategy is proposed. The study used a cost-effective ball milling method to prepare BP-G composites and a hydrogen-bonded crosslinked polyacrylic acid (PAA)-poly(ethylene oxide) (PEO) binder to form hydrogen bonds with the BP. Hydrogen bonding cross-linking allows the binder to form a network structure, which effectively disperses the stresses. Hydrogen bonding exists between the binder and the BP. Ether bonds in the binder improve ionic migration. The degree of hydrogen bond crosslinking was optimized by adjusting the binder composition. The electrode material with the optimal binder ratio exhibited a discharge capacity of 1186 mAh g −1 at 8 A g −1 . After 900 cycles, a reversible capacity of 771.8 mAh g −1 was maintained, with a capacity retention rate of 65.1 %, significantly outperforming electrodes using polyvinylidene fluoride (27.9 %) and PAA (19.3 %).
研究领域:
材料科学
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电化学
·
能源存储
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangyu Wang,Mingwei Zhao,Xuhao Wang,Peng Liu,Mengyao Fan,Xiaowei Yan,Zhenfeng Ma,Yanfang Zhang,Caili Dai
Petroleum remains the main source of energy consumption over the past decade. The development of rich unconventional oil reservoirs is a huge challenge. Clean fracturing fluids (CFFs) have gained considerable attention for the unconventional reservoir development, owing to their integrated capabilities of fracturing and oil expulsion. Performance of CFFs is a vital factor in enhancing oil recovery. In this work, a ternary deep eutectic solvent (DES) with dual hydrogen donors (HBDs) was developed as a novel and green medium for improving CFF performance. With the hydrogen-bonding interactions, the ternary DES enable a robust micelle network, thereby strengthening the rheological property, temperature resistance and drag reduction performance of CFFs. The salt resistance performance was improved due to the ion–dipole interaction between HBDs and salt cations, decreasing the interactions between salt cations and surfactants. The DES also increase the imbibition efficiency from 30.7 % in 98 h to 43.7 % in 62 h. Besides, the gel breaking performance and reusability of gel-breaking fluid were enhanced in the presence of DES. The ternary DES showed more effective reinforcement for CFF properties as compared with binary DES, due to the synergistic effect of dual HBDs. This work will provide a promising alternative for intensifying CFF performance.
研究领域:
石油工程
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绿色化学
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产品关联
DOI
高影响因子
Polymer Chemistry
·
2020
·Vol. 11
·期 34
·5463-5474
·
IF 5.342
Wuhou Fan,Yong Jin,Liangjie Shi
Achieving the room-temperature self-healing of polymer materials with mechanically robust and tough features is a challenging project due to their conflicting attributes. Herein, a novel design concept of dynamic but mechanically robust and tough polymer networks was proposed derived from dynamic diselenide bonds and dual H-bonds, in which flexible fluorinated siloxane units and H-bonded urethane and urea groups are embedded simultaneously. Through adjustment of the mass fraction of fluorinated siloxane units incorporated, waterborne polyurethanes with good mechanical performances (tensile strength: 16.31 MPa; toughness: 69.8 MJ m−3) could be constructed. Meanwhile, this optimized sample could also be healed at room-temperature within 2 h under visible light. Therefore, the fast room-temperature self-healing of our elaborated polymers with mechanically robust and tough features is achieved, which has never been achieved for the contemporary polymer materials. The reconstruction of dual H-bonding interactions of urethane and urea moieties is responsible for the prophase healing after reconnecting the fracture surfaces, and macromolecular chains containing fluorinated siloxane units with excellent flexibility could promote the visible-light-triggered diselenide metathesis in a highly efficient manner subsequently. Moreover, much improved water resistance properties could also be achieved. The elaborated strategy will provide inspiration for developing mechanically robust and tough water-dispersed polymer materials with fast room-temperature self-repairing performance and desirable water resistance properties, which are of vital importance to the next generation of smart materials.
研究领域:
材料科学
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高分子化学
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DOI
高影响因子
MACROMOLECULES
·
2015
·
IF 5.8
Huajun Huang,Yunbin Yuan,Jianping Deng
Optically active polymer particles constitute a unique type of polymer particle. However, nearly all the particles of this kind so far reported in the literature were prepared from chiral monomers. On the other hand, helix-sense-selective polymerization (HSSP) techniques were majorly applied in solution polymerization systems for preparing helical polymers adopting predominant one-handed helicity. In the present study, we report the first HSSP in precipitation polymerization systems, by which optically active helical polymer particles were constructed from an achiral monomer. Achiral acetylenic monomer with bulky adamantyl group smoothly underwent helix-sense-selective precipitation polymerization (HSSPP) with (nbd)Rh+B–(C6H5)4 as catalyst in the presence of Boc-l- or Boc-d-alanine as chiral additive. The HSSPPs provided optically active polymer particles consisting of helical polymer forming predominantly one-handed screw sense. SEM images show that the resulting polymer particles were obtained in high yield (80 wt %, average diameter approximately 300 nm) with regular spherical morphology. CD spectra clearly demonstrated that HSSP occurred in the course of precipitation polymerizations. The induced helical structures with preferential screw sense exhibited relatively high thermostability. We further proposed a possible mechanism for the occurrence of HSSPPs and the formation of stable helical structures: Double hydrogen bonds formed between each chiral additive molecule and the neighboring two amide structures in the polymer pendant groups; the double hydrogen bonds played essential roles for controlling the screw sense of the helical polymer chains and the stability. Based on this mechanism, a “chiral-lock effect” was further put forward. The preparative strategy opens new routes for preparing optically active polymer particles and even novel superhelical architectures for significant uses as chiral stationary phase for HPLC, chiral catalysts, enantioselective recognition probes, etc.
研究领域:
高分子化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2025
·
IF 12.5
Ruihuan Gu,Weiwei Chen,Yanrui Zou,Tingting Yang,Zirui Liu,Ning Yu,Jin Huang,Lin Gan
Multi‑hydrogen bond networks have been introduced into hydrogels to enhance responsiveness, self-healing, and processability, but low interaction density and weak bond force limit their strength and tear resistance. In this study, we construct a multiple-crosslinked interpenetrating network system of dynamic covalent bond, dual‑hydrogen bond, and percolation around cellulose nanocrystals (CNCs) to resolve the function-plasticity trade-off. This design enhances strength and toughness without sacrificing the hydrogel's electromechanical sensing and self-healing performance. The resulting hydrogel demonstrates improved tensile strength (25.54 kPa), toughness (246.09 kJ/m 3 ), and self-healing (93.3 %). Meanwhile, based on ionic conductivity and excellent mechanical plasticity, the hydrogels achieve quick linear response sensing under a wide strain region and high sensitivity (4.36). The mechanism study for the multiple-crosslinked interpenetrating network system reveals that although dual‑hydrogen bonds are weak, they dissipate impact energy over long distances, reducing stress concentration. The percolation network, enabled by the rod-like filler particles of CNCs, enhances strength at a low filler concentration, allowing the dynamic covalent bond crosslinking to maintain flexibility and function. Since the CNCs also present high biocompatibility, the hydrogel must be able to offer promising solutions for applications in wearable electronics and wound dressings.
研究领域:
材料科学
·
生物医学工程
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产品关联
DOI
PubMed
高影响因子
MACROMOLECULES
·
2021
·
IF 5.985
Huanhuan Yang,Shilong Wu,Quan Chen
This study focuses on the stretchability of brittle ionomers after introducing three types of hydrogen bonds, i.e., dual, triple, and quadruple hydrogen bonds. The introduction of dual or triple hydrogen bonds that are weaker than the ionic association improves the stretchability, and better improvement has been achieved for the triple hydrogen bonds. In comparison, the introduction of quadruple hydrogen bonds that are equally strong as the ionic association does not show this type of improvement. This result strongly indicates that there is an optimized strength ratio between the first (the stronger ionic) network and the secondary (the weaker hydrogen-bonding) network, i.e., the secondary network should be considerably weaker but still not too weaker than the first network. When this condition is satisfied, continuous dissociation and association of the secondary network weaken the chain retraction after the strain-induced breakup of the first network, thereby suppressing the formation of defects or microscopic cracks that potentially grow into the macroscopic fracture.
研究领域:
聚合物科学
·
材料科学
✓ 已验证
DOI
高影响因子
ORGANIC ELECTRONICS
·
2020
·
IF 3.31
Caixia Liu,Mengdi Li,Baisheng Lu,Ying Huang,Yangyang Zhang,Ping Liu,Xiaohui Guo,Yuanming Ma,Yugang Zhang,Shenyang Li,Wei Chen,Yunjian Ge
Owing to their ultrahigh sensitivity, crack-based flexible strain sensors have garnered considerable attention in recent years. In this study, a practical, and reliable chemical bonding-based dip-coating method is proposed to fabricate high sensitivity and high stability crack-based flexible strain sensor with dual hydrogen bond-assisted structure. The strain sensor has a sandwich structure, which is composed of graphene nanoplatelets (GNPs)/poly (sodium-p-styrenesulfonate) (PSS) conductive layer, ultra-violet (UV) adhesive substrate layer, and UV adhesive covering layer. The fabrication process, principle of dual hydrogen bond-assisted structure, strain sensing mechanism, and various properties of the proposed sensor are examined. It is demonstrated that the cracks and the dual hydrogen bond-assisted structure facilitate a practical strain sensor with high sensitivity (gauge factor of 19.65 in the strain range of 0–30%), long-term stability (over 10,000 cycles), good linearity, negligible drift, fast response time (~50 ms), and low detection limit (0.10%). Meanwhile, the proposed crack-based flexible strain sensor can be used as a wearable device , which can be directly mounted on human skin to monitor tiny human motions and writing behavior. Consequently, it exhibits immense potential for wearable applications including artificial skin, human-machine interfaces, and medical healthcare.
研究领域:
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Mengqian Fu,WeiLu Ding,Qianmeng Zhao,Zhenyang Xu,Wei Hua,Yunong Li,Zifeng Yang,Li Dong,Qian Su,Weiguo Cheng
CO 2 capture and conversion to high-value-added products is critical for the purposes of environmental preservation and carbon resource utilization. In this study, a novel class of porous poly(ionic liquid)s has been synthesized, incorporating dual hydrogen bond donors (amide and hydroxyl groups) and nucleophiles (Br - ) as multiple effective active sites for the cycloaddition reaction between CO 2 and epoxides. The presence of dual hydrogen bond donors not only provides two active sites for synergistic catalysis with epoxides but also enhances the capacity for CO 2 adsorption. Comprehensive characterization has been conducted to elucidate the structural features and properties of these innovative materials. By regulating the ratio between ionic liquid monomer and divinylbenzene, a hierarchical porous structure favorable for the reaction was constructed, resulting in optimized catalytic activity comparable to that of bulk ionic liquid monomers. Furthermore, this catalyst exhibits remarkable structural stability with minimal activity loss even after five consecutive use cycles. Combining density functional theory calculations with in-situ Fourier transform infrared spectroscopy analysis, the catalytic mechanism was proposed that the dual hydrogen bond donors and Br - synergistically promote ring-opening reactions of epoxides, while amide groups serve as basic sites to enhance CO 2 adsorption during the reaction process.
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Ya Liu,Yaqi Ren,Jing Huang,Hongsheng Lu,Zhiyu Huang,Li Wang
Shape-memory gel materials are widely used in smart drives and biological tissues due to their excellent flexibility and diverse stimuli responsiveness. In particular, shape-memory organohydrogel materials have rose intense interest recently owing to their sophisticated shape memory behavior. However, conventional mechanical enhancement strategies, either by introducing nanoparticles or double-network structure, employed in the preparation of organohydrogels require high energy input, leading to difficulties in emulsification for emulsion precursors of organohydrogels. These strategies are not suitable for large-scale production of high-strength organohydrogels. Herein，a high-strength shape-memory organohydrogel NL-H was prepared based on dual hydrogen bonding and gelator-induced solidification effect. The precursor was easily emulsified, as the aqueous phase involved no nanoparticles or highly viscous polymers. Moreover, the dual hydrogen bonds among the dual amide groups of N -acryloyl glycinamide (NAGA) monomers can endow the organohydrogel with high mechanical properties . Owing to the oil-solidification effect of gelator HSA, the mechanical properties could be greatly enhanced, showing a high Young's modulus of 188.04 kPa. Furthermore, by integrating a high elastic hydrogel matrix and reversible oil domains, the organohydrogel showed a thermo-softening and favorable shape-memory properties. Consequently, this work provides a new enhancement strategy for the preparation of organohydrogel with high mechanical properties and excellent shape memory capabilities. And the simple preparation process can also facilitate the large-scale fabrication.
研究领域:
材料科学
·
生物医学工程
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
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