ChemSusChem
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2017
·Vol. 11
·期 4
·672-680
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IF 7.226
Yang Li,Rui Zhu,Junting Wang,Ze-Sheng Li,Niansheng Xu,Jidong Zhang,Peng Wang
Graphical It's only lateral : Two N -annulated perylene-based hole transporters were reported for perovskite solar cells. In comparison to the bulky 2-hexyldecyl, the methoxyphenyl lateral substituent can induce stronger intermolecular π–π stacking and better connectivity of the intermolecular aggregate domains in the solid films, leading to improved hole mobility and power conversion efficiency of the perovskite solar cells. Perylene derivatives are a family of well-known organic electron-transporting materials with excellent photochemical and thermal stabilities, and have been widely used in various optoelectronic devices. In this work, two diphenylamine functionalized N -annulated perylenes are reported as hole-transporting materials (HTMs) for perovskite solar cells. Through joint theoretical and experimental studies, the HTM employing a methoxyphenyl lateral substituent is found to feature a closer stacking distance and better aggregate connectivity in the solid film than its analogue with the bulky 2-hexyldecyl lateral substituent, contributing to a higher hole mobility and a remarkably enhanced device performance of perovskite solar cells. This work demonstrates the significant influence of lateral substituents of HTMs on the intermolecular packing and solid microstructure, giving a clear insight on the molecular design of high-performance organic semiconductors.
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DALTON TRANSACTIONS
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2017
·Vol. 47
·期 1
·180-189
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IF 4.029
Dandan Yang,Jie Dong,Baiquan Wang
A series of new pincer-type tridentate o-aryloxide-N-heterocyclic carbene nickel complexes Ni1–Ni3 were synthesized, and the molecular structure of Ni3 was confirmed by X-ray crystallography. In comparison with the above tridentate complexes, the bidentate bis(aryloxide-NHC) nickel complex Ni4 was also synthesized. On activation with either Et2AlCl or Me2AlCl, all nickel complexes showed low activity toward norbornene (NB) homopolymerization. Surprisingly, Ni1–Ni3 catalysts exhibited moderate to high activity toward the homopolymerization (up to 3.21 × 106 g PNB (mol of Ni)−1 h−1) and copolymerization of norbornene with 1-octene (up to 1.39 × 105 g polymer (mol of Ni)−1 h−1) with B(C6F5)3 as the cocatalyst even at 100 °C, showing that tridentate nickel catalysts have high thermal stability. Notably, the tridentate Ni1–Ni3 complexes showed better activities than the corresponding bidentate bis(aryloxide-NHC) nickel complex Ni4. The obtained poly(NB-co-1-octene)s were confirmed to be vinyl-addition copolymers, which exhibited high 1-octene insertion ratio (9%–17%), good thermal stability (Td > 400 °C), high molecular weight (up to 105), and narrow molecular weight distribution (PDI ≤ 1.91).
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Guoxu Wang,Meng Liu,Juan Du,Lei Liu,Yifeng Yu,Jitong Sha,Aibing Chen
The membrane carbon materials with hierarchical porous architecture are attractive because they can provide more channels for ion transport and shorten the ions transport path. Herein, we develop a facile way based on “confined nanospace deposition” to fabricate N-dopi-ng three dimensional hierarchical porous membrane carbon material (N-THPMC) via coating the nickel nitrate, silicate oligomers and triblock copolymer P123 on the branches of commercial polyamide membrane (PAM). During high temperature treatment, the mesoporous silica layer and Ni species serve as a “confined nanospace” and catalyst respectively, which are indispensable elements for formation of carbon framework, and the gas-phase carbon precursors which derive from the decomposition of PAM are deposited into the “confined nanospace” forming carbon framework. The N-THPMC with hierarchical macro/meso/microporous structure, N-doping (2.9%) and large specific surface area (994m 2 g -1 ) well inherits the membrane morphology and hierarchical porous structure of PAM. The N-THPMC as electrode without binder exhibits a specific capacitance of 252 F g -1 at the current density of 1 A g -1 in 6 M KOH electrolyte and excellent cycling stability of 92.7% even after 5000 cycles.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Huihui Wang,Qian Zhao,Daiqiang Li,Zhilin Zhang,Yuan Liu,Xueli Guo,Xiaotong Li,Zhi Liu,Lian Wang,Jinzhu Ma,Hong He
Photothermal catalysis is extremely promising for the removal of various indoor pollutants owing to its photothermal synergistic effect, while the low light utilization efficiency and unclear catalytic synergistic mechanism hinder its practical applications. Here, nitrogen atoms are introduced, and Pt nanoparticles are loaded on TiO2 to construct Pt/N-TiO2-H2, which exhibits 3.5-fold higher toluene conversion rate than the pure TiO2. Compared to both photocatalytic and thermocatalytic processes, Pt/N-TiO2-H2 exhibited remarkable performance and stability in the photothermocatalytic oxidation of toluene, achieving 98.4% conversion and 98.3% CO2 yield under a light intensity of 260 mW cm–2. Furthermore, Pt/N-TiO2-H2 demonstrated potential practical applicability in the photothermocatalytic elimination of various indoor volatile organic compounds. The synergistic effect occurs as thermocatalysis accelerates the accumulation of carboxylate species and the degradation of aldehyde species, while photocatalysis promotes the generation of aldehyde species and the consumption of carboxylate species. This ultimately enhances the photothermocatalytic process. The photothermal synergistic effect involves the specific conversion of intermediates through the interplay of light and heat, providing novel insights for the design of photothermocatalytic materials and the understanding of photothermal mechanisms.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Ting Zhang,Weitao Wang,Meng He,Huan Wang,Zhen-Hong He,Yang Yang,Kuan Wang,Zhao-Tie Liu
Imines as valuable chemical intermediates can be synthesized by aerobic photocatalytic oxidation of amines, which is recognized as a promising and green route for imines synthesis. It is attractive to develop solvent-free photocatalytic oxidation of amines with high efficiency, especially with high activity and selectivity, but it is challenging. In the present work, flower-like BiOX/TiO 2 (X = Cl, Br, I) heterojunction was designed for solvent-free photocatalytic oxidation of benzylamine to N-benzylidenebenzylamine. Type II heterojunction of BiOCl/TiO 2 with 67.3 wt% of BiOCl achieved the high formation rate of 6316 µmol∙g −1 ∙h −1 and selectivity of 99 % on BiOCl/TiO 2 . To the best of our knowledge, the activity and selectivity are the highest for solvent-free photocatalytic system. The reason for the varied photocatalytic performances were investigated. The solvent-free photocatalytic mechanism was revealed and proposed. Moreover, the BiOCl/TiO 2 photocatalyst can be used for photocatalytic oxidation of varied benzylamines to imines.
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ANALYTICA CHIMICA ACTA
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2024
·
IF 5.7
Jun-Yi Zhou,Yan-Qing Chen,Guang Hu,Haiyu Zhao,Jian-Bo Wan
Background N-acylethanolamines (NAEs) are a class of naturally occurring bioactive lipids that play crucial roles in various physiological processes, particularly exhibiting neuroprotective and anti-inflammatory properties. However, the comprehensive profiling of endogenous NAEs in complex biological matrices is challenging due to their low abundance, structural similarity and the limited availability of commercial standards. Here, we propose an integrated strategy for comprehensive profiling of NAEs that combines chemical derivatization and a three-dimensional (3D) prediction model based on quantitative structure-retention time relationship (QSRR) using liquid chromatography coupled with high-resolution tandem mass spectrometry (LC-HRMS). Results After acetyl chloride (ACC) derivatization, the detection sensitivity of NAEs was significantly improved. We developed a QSRR prediction model to construct an in-house database for 141 NAEs, encompassing information on RT, MS 1 ( m/z ), and MS/MS spectra. Propargylamine-labeled fatty acids were synthesized as RT calibrants across various analytical conditions to enhance the robustness of the RT prediction model. NAEs in biological samples were then in-depth profiled using parallel reaction monitoring (PRM) acquisition. This integrated strategy identified and annotated a total of 50 NAEs across serum, hippocampus and cortex tissues from a 5xFAD mouse model of Alzheimer's disease (AD). Notably, the levels of polyunsaturated NAEs, particularly NAE 20:5 and NAE 22:6, were significantly decreased in 5xFAD mice compared to WT mice, as confirmed by accurate quantitation using ACC- d 0 / d 3 derivatization. Significance Our integrated strategy exhibits great potential for the in-depth profiling of NAEs in complex biological samples, facilitating the elucidation of NAE functions in diverse physiological and pathological processes.
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TRANSACTIONS OF TIANJIN UNIVERSITY
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2024
·
IF 6.7
Liu Weihao,Liu Qingtao,Wan Xin,Shui Jianglan
Non-precious metal electrocatalysts (such as Fe–N–C materials) for the oxygen (O 2 ) reduction reaction demand a high catalyst loading in fuel cell devices to achieve workable performance. However, the extremely low solubility of O 2 in water creates severe mass transport resistance in the thick catalyst layer of Fe–N–C catalysts. Here, we introduce silicalite-1 nanocrystals with hydrophobic cavities as sustainable O 2 reservoirs to overcome the mass transport issue of Fe–N–C catalysts. The extra O 2 supply to the adjacent catalysts significantly alleviated the negative effects of the severe mass transport resistance. The hybrid catalyst (Fe–N–C@silicalite-1) achieved a higher limiting current density than Fe–N–C in the half-cell test. In the H 2 –O 2 and H 2 –air proton exchange membrane fuel cells, Fe–N–C@silicalite-1 exhibited a 16.3% and 20.2% increase in peak power density compared with Fe–N–C, respectively. The O 2 -concentrating additive provides an effective approach for improving the mass transport imposed by the low solubility of O 2 in water.
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JOURNAL OF MOLECULAR CATALYSIS B-ENZYMATIC
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2012
·
IF 2.735
Xinjiong Fan,Xiaolong Liu,Yuhuan Liu
A novel gene (designated as est816 ) encoding an esterase was isolated from a Turban Basin metagenomic library with a functional screening method. Sequence analysis revealed that est816 encoded a protein of 271 amino acids with a predicted molecular mass (Mr) of 29.9 kDa and was expressed in Escherichia coli BL21 (DE3) in soluble form. The optimum pH and temperature of the recombinant Est816 were 7.5 and 60 °C, respectively. The enzyme was stable in the pH range of 5.0–9.0 and at temperatures below 50 °C. The residual activity of Est816 was 47.7% when stored at 25 °C for 5 months. The enzyme could hydrolyze a wide range of ρ-nitrophenyl esters, but its best substrate is ρ-nitrophenyl acetate with the highest activity (364 U/mg). It could also degrade medium to long-chain AHLs at the concentration of 1 mM in half an hour with more than 90% degradation efficiency. This is the first report to construct one metagenomic library from Turban Basin to obtain one esterase, which belongs to family V esterases/lipases and has AHL-lactonase activity. The recombinant enzyme displayed broad substrate spectrum, high activity and thermostability. These excellent properties make it an attractive enzyme for quorum quenching.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2012
·
IF 2.237
Rulong Li,Huabin Xing,Qiwei Yang,Xu Zhao,Baogen Su,Zongbi Bao,Yiwen Yang,Qilong Ren
This paper presents an extensive study on the feasibility of ionic liquids (ILs) for the extractive separation of a 1-hexene/n-hexane mixture. Seventeen ILs were tested at 313 K. The extraction selectivities of 1-hexene to n-hexane were in the range 1.5–3.0. The chemical structures of anion and cation in ILs greatly affected the extraction, and the functional groups, such as carbon–carbon double bond, nitrile, ester, and amide, in the ILs led to higher selectivities. The increase of alkyl chain length in cation led to the increase of extraction capacity of 1-hexene. To increase the distribution of 1-hexene in IL phase, silver salt was added to the ILs. It was found that ILs containing silver salt had a high distribution of 1-hexene, as well as high selectivity of 1-hexene against n-hexane. The extraction efficiency increased with the concentration of silver salt in ILs. When the initial feed concentration of 1-hexene was smaller, the selectivity of 1-hexene to n-hexane was higher. A simple mathematical model has been developed to describe the total 1-hexene content in the reaction media under study, on the basis of the formation of complexes between silver and 1-hexene with different stoichiometry. This work proves that the ILs can act as effective extractants in 1-hexene/n-hexane separation.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yang Li,Xuemei Diao,Peicheng Li,Panpan Liu,Yan Gao,Zhiyong Zhao,Xiao Chen,Ge Wang
To cope with the complex and changeable extreme environments, extending multifunctionality is crucial for potable smart wearable composite phase change materials (PCMs). Herein, we developed advanced Co/N co-doped carbon foam-based multifunctional “five-in-one” composite PCMs integrating dual-temperature thermal management, light-triggered heating, waterproof, flame retardant, and microwave absorption through high-temperature calcination of melamine foam@ZIF67 and melting encapsulation of paraffin wax (PW). Benefiting from the strong full-spectrum absorption, fast photon and phonon transport, and local surface plasmon resonance effect, our designed foam-based composite PCMs exhibited an ultrahigh photothermal conversion efficiency of 95.17 %. More importantly, foam-based composite PCMs demonstrated excellent thermal management, structural stability and thermal storage stability after undergoing 300 heating–cooling cycles. Furthermore, foam-based composite PCMs showed superior microwave absorption (RL min = -57.93 dB), good flame retardancy and satisfactory hydrophobicity (contact angle > 100°). Thus, our developed multifunctional foam-based composite PCMs provide great potential for personalized thermal management and anti-radiation smart wearables even in harsh environments (e.g., rain, snow, sweat, fire, extreme cold, extreme heat and electromagnetic interference), creating a versatile platform for smart wearable light-triggered phase change heater with on-demand properties.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Lei Cai,Xiyu Mou,Jieshee Hong,Chun Cui
With the improvement of people's living standards and health awareness, reducing salt, sugar, and fat is gradually becoming the mainstream trend. In this work, we delved into the development of an innovative taste enhancer, N-lauroyl theanine (NLT), and its taste presentation mechanism. NLT was synthesized in the aqueous phase by enzyme-catalyzed and direct-heating methods using food-grade enzymes in yields of up to 64.33 % and 49.11 %, respectively. Sensory evaluation and molecular docking techniques revealed the potential of NLT to enhance salty, umami, sweet, and kokumi taste sensations and its taste presentation mechanism. Results revealed significant taste enhancement of saltiness, umami, sweetness, and kokumi and prolonged their duration in the oral cavity by 0.25–1 mg/L NLT. Molecular docking analyses showed that NLT had a strong binding affinity for a variety of taste receptors. These findings highlight the potential of NLT as a potent taste enhancer for the development of healthier salt/sugar-reduced foods.
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JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Hu Wang,Zhifeng Yao,Yong Chen,Bing Li,Xin Zhong,Mengnan Zhang,Longbin Xia,Zunqing Zheng,Mingfa Yao
Experimental and kinetic studies on the blending of ethers or diesters with larger alkanes at low temperatures are enormously scarce. In this paper, the low-temperature oxidation (LTO) kinetics model of polyoxymethylene dimethyl ether 3 (OME 3 )/ n -heptane (500 K–950 K) was established by using the jet-stirred reactor (JSR) to conduct the LTO experiments of OME 3 / n -heptane with different blending ratios. GC/MS was used to detect and quantify 17 kinds of stable products in the LTO process of OME 3 / n -heptane. The detailed OME 3 / n -heptane kinetic model was fully verified experimentally. The interaction mechanism of OME 3 / n -heptane was discussed based on the experiments and corresponding chemical kinetic analysis . Results show that the oxidative decomposition processes of OME 3 and n -heptane were significantly different, the LTO and NTC process of OME 3 were significantly weaker than those of n -heptane, but the high-temperature reactivity of OME 3 was much stronger. In addition, n -heptane significantly promoted the intermediate species CH 3 OCHO and COCOC*O of OME 3 , mainly because n -heptane significantly prolonged the LTO of OME 3 in the fuel blends. And the NTC process of the fuel blends was mainly dominated by OME 3 , while the LTO process was more influenced by n -heptane, which resulted in the weakened NTC of n -heptane and the significantly enhanced LTO process of OME 3 .
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