Journal of Flow Chemistry
·
2022
·Vol. 12
·期 3
·317-325
·
IF 3.264
Xu Qilin,Li Guosi,Zhu Fucheng,Chen Naidong,Chen Cuiwu,Yu Zhiqun
N -(3-Amino-4-methylphenyl)benzamide ( 1 ) is a crucial building blocks of many drug candidates. In this paper, a continuous flow microreactor system was developed to synthesize 1 and determine intrinsic reaction kinetics parameters. By screening the acylating reagents and reaction conditions, 1 was obtained by the selective acylation of 4-methylbenzene-1,3-diamine ( 2 ) with benzoic anhydride ( 3 ). Since the two amine groups in 2 are in different chemical environments, parallel by-products and serial by-products coexist, which makes the selective monoacylation process relatively complicated. To reveal the reaction process clearly, reaction rate constants and their 95% confidence intervals, activation energies, pre-exponential factors were acquired by kinetics study in microflow system. The established kinetic model can calculate the selectivity and conversion of the acylation reaction, which are in good agreement with the experimental results. Subsequently, the kinetic model was used to optimize reaction conditions, as a result, 1 was synthesized in the microreactor with a yield of 85.7% within 10 min.
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高影响因子
Science China-Materials
·
2022
·Vol. 65
·期 12
·3368-3381
·
IF 8.64
Bai Le,Yao Fang,Wang Rui,Liu Baibai,He Dongmei,Zhou Qian,Wang Wenqi,Xu Cunyun,Hu Xiaobo,Chen Shaoqiang,Song Qunliang,Zhou Tingwei,Lee Donghwa,Zhao Pengjun,Chen Cong,Yang Hua,Lin Qianqian,Zang Zhigang,Chen Jiangzhao
The deep-level traps at grain boundaries (GBs) and halide ion migration are quite challenging for further enhancement of the stability and efficiency of perovskite solar cells (PSCs) as well as for the elimination of notorious hysteresis. Herein, we report a large-sized strongly coordinated organic anion GB anchoring strategy for suppressing ion migration and passivating defects in planar PSCs. The practical implementation of this strategy involves the incorporation of potassium salts containing a large-sized organic counter anion (4-sulfobenzoic acid monopotassium salt, SAMS) into the perovskite precursor. It has been found that anions within SAMS can be firmly anchored at GBs due to the strong coordination interaction between C=O and/or S=O at both ends of bulky anion and undercoordinated Pb 2+ and/or halide vacancies, along with the hydrogen bond between −OH and formamidinium. SAMS can not only passivate shallow-level defects but also cause more effective passivation of the deep-level defects. The GB manipulation strategy results in a reduced defect density, an increased carrier lifetime as well as suppressed ion migration, which in turn contributed to enhanced efficiency and stability of PSCs together with a thorough elimination of hysteresis. As a result, the SAMS-modified device with an outstanding fill factor of 0.84 delivers a significant improvement in efficiency (22.7%) in comparison with the control device (20.3%). The unencapsulated modified device demonstrates only little degradation after 1320 h at 60°C.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Xin Deng,Lihua Zhu,Huan Zhang,Liqing Li,Ning Zhao,Jiexiang Wang,Sameh M. Osman,Rafael Luque,Bing Hui Chen
A covalent organic framework (COF) was used as the support of the catalyst in this work in order to obtain an environmentally friendly catalyst with high catalytic performance, selectivity and stability for 4-nitrophenol hydrogenation. Pd tiny particles are fixed in the cavity of COF to obtain Pd/COF catalysts, which has a quite narrow particle size distribution (5.09 ± 1.30 nm). As-prepared Pd/COF catalysts (Pd loading-2.11 wt%) shows excellent catalytic performance (conversion - 99.3%, selectivity >99.0% and turnover frequency (TOF)-989.4 h −1 ) for 4-nitrophenol hydrogenation under relatively mild reaction conditions of reaction temperature-40 °C and reaction pressure-3.0 MPa H 2 , and Pd/COF catalysts have high stability. Pd/COF catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscope energy-dispersive X-ray spectroscopy (SEM-EDS), transmission electron microscope (TEM), high resolution TEM (HRTEM), Brunauer-Emmett-Teller (BET), scanning TEM energy-dispersive X-ray spectroscopy (STEM-EDS) elemental analysis techniques to prove that the Pd nanoparticles are highly dispersed on the COF. Pd/COF catalysts have good stability and reusability hence with certain industrial application value.
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PubMed
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 26
·2201049
·
IF 6.389
Yun Zhao,Qianqian Bai,Liqiang Chai,Xiaofei Dong,Jiangtao Chen,Jianbiao Chen,Yan Li,Xiuxun Han
Aiming at the current bottleneck of Cu 2 ZnSn(S,Se) 4 (CZTSSe) thin film solar cells, an experimental analysis of the performance and loss mechanism of CZTSSe thin film solar cells upon proton radiation exposure is presented. In order to deduce the important cell parameters, the environment of the cells is simulated by subjecting the devices to 200 keV proton irradiation with fluences from 1 × 10 10 to 1 × 10 17 cm -2 . It is found that the damage constants are sensitive to the elemental diffusion at heterojunction and Na redistribution in device. The incidence of the proton can lead to bandgap, tails fluctuations, and Urbach energy changes in the cells those directly impact defects and structural disorder in CZTSSe material thereby the device performance. The time-resolved photoluminescence results show that the carrier lifetime is also very sensitive to the distribution of interface elements, especially Na, Cd, and S. These findings may provide new ideas for solving the V OC deficit of CZTSSe solar cells. From this work, it can be also suggested that the CZTSSe thin film solar cells are robust to proton irradiation and have the potential for future space applications.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2022
·
IF 4.119
Jiaqi Yang,Guorui Qu,Cuiping Liu,Shiwei Zhou,Bo Li,Yonggang Wei
The high lithium content in spent lithium ion batteries (LIBs) and a large number of spent LIBs generation shift the target of lithium recovery to solid waste. Adsorption separation is of great application value for lithium recovery. There is still a lack of a lithium adsorption material with excellent properties. Herein, an environmental hydrolytic polymerization to prepare lithium ion-imprinted membranes (LIIMs) with high adsorption capacity and selectivity is presented. The LIIMs can reach adsorption equilibrium in 40 min, showing fast adsorption kinetics . The optimal adsorption capacity of the LIIMs for Li + was 132.00 mg g −1 after immersing in a 300 mg L −1 LiCl solution based on ample binding sites and a strong affinity force. Langmuir isothermal adsorption results proved that the imprinting sites on LIIMs were homogeneous. The selective separation factors (α) of Li + to Mg 2+ , K + , Ca 2+ , Na + were 6.80, 17.00, 21.30, and 24.60, respectively, which implies the superior selectivity LIIMs toward Li + . The adsorption capacity of LIIMs remained about 97 % after six cycles. Due to the suitable cavity, abundant rebinding sites, and strong affinity, the LIIMs have a good selective adsorption ability to Li + . Therefore, the LIIMs would have potential applications for separating Li + from spent LIBs.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 16
·7896-7908
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IF 4.682
Xu Tianye,Lu Shun,Wang Yajie,Gan Xiaoyan,Guo Liling,Liu Hanxing
Two-dimensional (2D) perovskite formed by introducing various organic spacer cations into 3D perovskite is considered to be one of the most effective methods to improve the humidity stability of perovskite materials. In order to solve the phase inhomogeneity and phase distribution nonuniformity of two-dimensional perovskites, additive engineering technique is widely used during their fabrication processes. Although many additives are proved to be effective in improving the quality of perovskite films, the mechanism of additive engineering has not been fully understood. In our work, we prepare 2D Ruddlesden–Popper perovskites based on 4-bromophenylethylammonium (BPEA) using a new additive of ionic liquids MAAc (methylammonium acetate). The (BPEA) 2 (MA) 4 Pb 5 I 16 perovskite prepared with the assistance of MAAc exhibits a stable photoelectric conversion efficiency (PCE) of 8.47%, which is much higher than the one without MAAc additive (4.79%). Besides a nearly tenfold increase in electron mobility, the unencapsulated (BPEA) 2 (MA) 4 Pb 5 I 16 -based device with MAAc additive remains 88% of its initial efficiency after 960 h exposure to air with a humidity of 20 ± 5% at room temperature, while the device without additive decreases to 63% of its initial efficiency. Meanwhile, the interactions between PbI 2 and MAAc at different temperatures and molar ratios are investigated and the formation mechanism of 2D perovskites in the presence of MAAc is proposed. It is found that an intermediate perovskite with distorted [PbI 6− x Ac x ] 4− octahedron is formed with the addition of MAAc, making the quality and photoelectric properties of the resultant films greatly enhanced.
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高影响因子
WORLD JOURNAL OF MICROBIOLOGY & BIOTECHNOLOGY
·
2022
·Vol. 38
·期 6
·1-10
·
IF 4.253
Liang YaoYao,Luo Juan,Yang Chenhao,Guo Shuning,Zhang Bowen,Chen Fengqianrui,Su Kairui,Zhang Yulong,Dong Yi,Wang Zhihao,Fu Hongda,Sui Guangchao,Wang Pengchao
Hydroxy-mandelic acid (HMA) is widely applied in pharmaceuticals, food and cosmetics. In this study, we aimed to develop an allosteric transcription factors (aTFs) based biosensor for HMA. PobR, an aTF for HMA analog 4-hydroxybenzoic acid, was used to alter its selectivity and create novel aTFs responsive to HMA by directed evolution. We established a PobR mutant library with a capacity of 550,000 mutants using error-prone PCR and Megawhop PCR. Through our screening, two mutants were obtained with responsiveness to HMA. Analysis of each missense mutation indicating residues 122–126 were involved in its PobR ligand specificity. These results showed the effectiveness of directed evolution in switching the ligand specificity of a biosensor and improving HMA production.
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PubMed
高影响因子
TALANTA
·
2022
·
IF 6.556
Ya-Qin Liu,Wei Zhu,Quan Yuan,Ji-Ming Hu,Xin Zhang,Ai-Guo Shen
Developing a rapid, low cost and sensitive sensing strategy for undifferentiated detection and fast killing of bacterial pathogens are critical to alleviating bacteria infections. Here, we propose a direct photoreduction method to synthesize the SERS tag by integrating poly(4-cyanostyrene) nanoparticles (NPs) and silver ions , which are applied as bio-sensing system for bacteria sensing and fast killing. Under a focused laser spot, silver ions on the surface of the poly(4-cyanostyrene) NPs could be photoreduced into Ag NPs, thereby causing the Raman signal amplification of poly(4-cyanostyrene) NPs up to 40 times, and there is a good linear correlation between the Raman intensity of poly(4-cyanostyrene) NPs and different concentrations of Ag + . Moreover, 4-mercaptophenylboronic acid, performing the same recognition function for both the Gram-positive and Gram-negative bacteria, is used as bridge between the bacteria and Ag + by the inherent chemical bonding. Based on further constructed bio-sensing system, we achieved the quick count and killing of both Gram-positive bacteria, e.g. , Staphylococcus aureus ( S. aureus ), and Gram-negative bacteria, e.g. , Escherichia coli ( E. coli ). Notably, the sensing strategy can detect at least ∼100 cells of E. coli , ∼10 cells of S. aureus and ∼10 cells of their mixture in less than 40 min. The detection accuracy for actual samples can also reach over 80% and the bacteria were entirely killed by Ag + after the detection, avoiding bacterial contamination in the environment. This novel method is anticipated to perform as a simple yet effective tool for fast and sensitive bacteria counting and killing.
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PubMed
高影响因子
EcoMat
·
2022
·Vol. 4
·期 2
·e12164
·
IF 12.213
Chaoyu Lin,Gan Luo,Huiqin Zhou,Anlin Feng,Li Zeng,Qingyang Li
An amorphous Ni nanoparticles-loaded ZnO nanowire array is controllably constructed on stainless steel mesh through combined electrodeposition and hydrothermal reaction. Its nano-arrayed structure not only provides a platform to achieve stable and good dispersion of Ni nanoparticles, but also helps improve their ability to adsorb 4-nitrophenolate ions and to capture hydrogen radicals, thereby accelerating the hydrogen transfer from metal hydride complex to 4-nitrophenol. Benefiting from the abovementioned unique features, it outperforms most Ni-based catalysts. While a 30-s re-electrodeposition of Ni can provide it extra 150 min of high catalytic activity towards the reduction of waste 4-nitrophenol to valuable 4-aminophenol, further demonstrating its outstanding reusability. The highly general methodology reported here paves the way to economically and effectively synthesize various other metal nanoparticles-loaded ZnO nanowire arrays on different conductive substrates, which not only enrich the nanowire-arrayed catalysts, but also significantly promote their practical utilizations in a wide range of environment-related fields.
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JOURNAL OF POLYMER SCIENCE
·
2022
·Vol. 60
·期 9
·1468-1479
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IF 3.046
Ming Duan,Gang Wu,Tianbin Gu,Xiaohui Jiang,Lei Zhao,Limei Zhou,Yunwen Liao,Qiang Pu
Present work reports a new type of poly( N -alkyl-2-[4-hydroxybut-2-ynyl] pyridinium bromides) (designated as Po-n, n = 8, 12, 16 of carbon atoms in the alkyl chain). Po-n were synthesized and characterized by FTIR, GPC, and NMR analysis. The possible polymerization mechanism was proposed and supported by theoretic calculation. A preliminary probe was performed on the conductivity and anticorrosive ability of the conjugated polymer. The results showed that these polymers demonstrated poor conductivity, however the conductivity was enhanced by graphene doping. Po-n are good inhibitors for X70 steel corrosion in HCl solution. So, the conjugated polymers may play important roles in the fields of optoelectronic devices and steel corrosion inhibition. Graphical
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MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Zhenhu Guo,Jingsong Lu,Wensheng Xie,Xuezhong Li,Hong Wu,Lingyun Zhao
The strategic design for fabricating metal phenolic networks (MPNs) at different dimension brings potential possibilities to obtain MPNs-based system with controlled structure, biologically tunable physicochemical properties and high responsiveness behavior. Considering adequate Fe ions within Fe-based materials, self-supplied metal ions for polyphenol to form coating layer on the surface are served as a novel and facile strategies to obtain metal-based phenolic networks composites. Combing these, herein, a simple, green and fast strategy was performed to fabricate recyclable Fe@Fe 3+ -tannic acid-Au (Fe@MPNs-Au) system with high efficiency to catalyze the reduction of 4-nitrophenol. The obtained experimental results showed that the catalytic rate of Fe@MPNs-Au for 4-nitrophenol could be improved from 0.4398 min −1 to 1.5804 min −1 with the increase of Au loading. Additionally, the increased Fe 3+ -tannic acid MPNs layer thickness could also enhance the catalytic rate of Fe@MPNs-Au from 0.2226 min −1 to 2.085 min −1 . More importantly, the superior magnetic properties contributed by Fe core make it possible to be easily separated and collected by a magnet from the solution after multiple catalytic reduction reaction. Finally, we hope this strategy can provide a novel paradigm for fabricating metal-based phenolic networks system by in situ coordinating reaction between self-supplied Fe sources and phenolic molecules.
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Separation Science Plus
·
2022
·Vol. 5
·期 6
·237-246
·
IF 0
Min Lu,Hao Zhang,Shi-Jun Yin,Hui Jiang,Xu Wang,Feng-Qing Yang
In this study, the poly (sodium 4-styrenesulfonate)-mediated calcium carbonate magnetic microspheres were prepared by a simple spontaneous biomimetic mineralization method to immobilize kallikrein. The immobilized kallikrein can be easily separated from the reaction mixture by an external magnet. The structural properties of the materials were studied by several characterization techniques. Subsequently, the immobilized kallikrein enzyme activity and stability were studied. Moreover, the inhibitory potency of ten natural compounds on kallikrein was evaluated by combining with capillary electrophoresis analysis. The immobilized kallikrein exhibited optimum pH and temperature at 7.5 and 75°C, respectively. After seven successive cycles, the immobilized kallikrein retained 82% of its initial activity. Furthermore, the Michaelis–Menten constant ( K m ) and the half-maximal inhibitory concentration (IC 50 ) of serine protease inhibitor on the immobilized kallikrein were determined to be 3.30 mM and 67.04 μM, respectively. In addition, berberine, evodine, coptisine, and jatrorrhizine among the ten natural compounds showed good inhibitory activity on the immobilized kallikrein, and their % of inhibition were (43.1 ± 1.7), (34.4 ± 1.9), (38.0 ± 1.7), and (28.5 ± 1.0)%, respectively. These results indicate that the biomimetic mineralization synthetic magnetic microsphere is an efficient method for kallikrein immobilization.
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