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POLYMER INTERNATIONAL · 2021 ·Vol. 70 ·期 9 ·1344-1355 · IF 2.99

Preparation of ordered macroporous molecularly imprinted polymers and their applications in purifying cinchona alkaloids from cinchona extract

Zhi-Yuan Zhang,Li-Li Rui,Ya-Li Lin,Hui-Dan Zhang,Ji-Ming Ou,Jian-Feng He,Quan-Zhou Wu

Three-dimensionally ordered macroporous molecularly imprinted polymers (3DOM MIPs) were prepared for the direct purification of cinchona alkaloids from crude cinchona extract. The 3DOM MIPs were easily prepared by grafting quinine-MIPs on the pore walls of 3DOM thiol-group-functionalized silica. The materials were characterized using various techniques. The results showed that the 3DOM MIPs had a more regular macroporous structure, a greater surface area and a greater porosity than traditional bulk MIPs (TBMIPs). The 3DOM MIPs could reach a high MIP content of 69.9%. And the 3DOM structure could improve intraparticle adsorption and provide more accessible adsorption sites. Consequently, in both static adsorption experiments and solid-phase extraction (SPE), the actual adsorption capacity of the imprinted polymers of the 3DOM MIPs was about 83% higher than that of TBMIPs. Moreover, the 3DOM MIPs exhibited high affinity for quinine, quinidine and cinchonine. Using the quinine-3DOM MIPs as SPE sorbent, quinine, quinidine and cinchonine could be effectively purified from crude cinchona extract with high elution recoveries. Control experiments also showed that the 3DOM MIPs were superior to commercially available adsorbents in terms of the purification of cinchona alkaloids from crude extract. © 2021 Society of Chemical Industry

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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 45 ·25488-25494 · IF 12.732

A confined thermal transformation strategy to synthesize single atom catalysts supported on nitrogen-doped mesoporous carbon nanospheres for selective hydrogenation

Zhengbin Tian,Wenquan Wang,Yan Zheng,Guang-Hui Wang

Carbon-supported single-atom catalysts (SACs) have brought considerable attention to heterogeneous catalysis, but they, however, often suffer from low activity due to the mass transfer limitation. Herein, we report a soft-templating method to synthesize core–shell mesostructured polymer nanospheres with metal nanoclusters (M-NCs, M = Pd, Pt) as the core, which can be easily converted into nitrogen-doped mesoporous carbon nanosphere (NMCS) supported SACs (M1/NMCS) after a confined thermal transformation process. Through this strategy, Pd1/NMCS and Pt1/NMCS are successfully prepared with rich porosity and high N content. The abundant N species in M1/NMCS can be employed as anchoring sites to capture and stabilize the single metal atoms. In addition, the mesoporous structure of M1/NMCS is beneficial for the mass transfer and the exposure of active sites. Benefiting from such a unique structure, the as-obtained Pd1/NMCS exhibits excellent activity, selectivity, and long-term stability in the selective hydrogenation of quinoline.

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POLYMERS FOR ADVANCED TECHNOLOGIES · 2021 ·Vol. 32 ·期 9 ·3740-3749 · IF 3.665

Synthesis and thermal degradable property of novel tertiary ester-containing four-functional epoxy resin

Tianwen Dai,Shuaiwei Yuan,Huawei Zou,Pengbo Liu

A kind of four-functional epoxy resin containing tertiary ester groups (FETE) was designed and synthesized by two-step reaction: first, the nucleophilic substitution reaction between linalool and isophthaloyl chloride, and then epoxidation. The chemical structure of obtained product was determined by infrared (IR) spectroscopy and nuclear magnetic resonance spectroscopy. Unlike traditional thermosetting epoxy resins, the cured FETE could degrade rapidly at low temperature (200–300°C). Dynamic mechanical analysis analysis showed that through copolymerization of FETE with (4,5-epoxycyclohexane-1,2-dicarboxylic acid diglycidyl ester) epoxy resin (TDE-85), the glass transition temperature (Tg) of copolymer system could be adjusted in the range of 136–179°C; FETE had good miscibility with TDE-85. The thermal degradation behavior of the copolymer system was studied by theoretical calculation, thermogravimetric (TG), and TG coupled with FTIR analysis, the results showed the thermal decomposition performance of the copolymer system could be adjusted in the range of 200–400°C. The tertiary ester groups in FETE were easy to thermally degrade and caused the network skeleton of the copolymer system to collapse. The FETE would have good prospects in reworkable electronic packaging, recycling or degradable epoxy resin area.

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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 42 ·14886-14894 · IF 7.059

Comprehensive properties study of low-temperature imidized polyimide with curing accelerators

Chao Huang,Jinhui Li,Deliang Sun,Rui Xuan,Yuying Sui,Tingyu Li,Liang Shang,Guoping Zhang,Rong Sun,Ching Ping Wong

Over the last few years, low-temperature curing polyimide (PI) has turned out to be a significant target for the advanced electronic package. Although the curing accelerators have been confirmed to be capable of significantly decreasing the curing temperature, their effects on properties have not been comprehensively examined. In this study, polyamide acid is synthesized by pyromellitic dianhydride (PMDA) and 4,4′-oxydianiline (ODA), and the process of low-temperature imidization is investigated by introducing six accelerators, i.e., quinoline (QL), isoquinoline (IQL), 2-methyl quinoline (2-QL), 4-methyl quinoline (4-QL), 8-methyl quinoline (8-QL), as well as 5,6,7,8-tetrahydroquinoline (THQL). As revealed from the results, the polyimide films formed using 4-QL and QL have exhibited prominent mechanical, thermal, and electrical properties. For the PI-4-QL, the tensile strength is 151.87 MPa, elongation-at-break reaches 161.36%, and the weight loss of 5% is observed at 533 °C; for the PI-QL, the tensile strength is 134.82 MPa, elongation-at-break reaches 145.16%, and the weight loss of 5% reaches 545 °C. As indicated from the results, the boiling point, acidity and molecular structure of the low-temperature curing accelerators show significant effects. Lower acidity and steric hindrance between the accelerator and amide bond facilitate the low-temperature imidization of polyamide acid. Furthermore, the as-prepared low-temperature cured PIs of 4-QL and QL would exhibit wide applications in advanced packaging industry.

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Molecular Catalysis · 2020 · IF 3.687

Reversible aerobic oxidative dehydrogenation/hydrogenation of N-heterocycles over AlN supported redox cobalt catalysts

Zhen-Hong He,Yong-Chang Sun,Kuan Wang,Zhong-Yu Wang,Pan-Pan Guo,Chong-Shan Jiang,Man-Qing Yao,Zhu-Hui Li,Zhao-Tie Liu

N -heterocycles with quinoline and tetrahydroquinoline structures are highly important in pharmaceutical and chemical industries, and their highly efficient mutual transformations are vital but still challenging. In the present work, AlN supported redox cobalt catalysts (Co 3 O 4 /AlN and Co/AlN) were prepared, which could achieve the reversible aerobic oxidative dehydrogenation/hydrogenation of N -heterocycles with good performances. The catalytic performances were stem from the strong interaction between Co species with AlN support, which were confirmed by the characterizations of Raman, XPS, UV–vis DRS, and H 2 -TPR etc . Both of the catalysts showed good stabilities and reusabilities for the titled reactions. Besides, the gram-scale experiments achieved with good yields to corresponding products, revealing the present protocol possesses great potential applications in industry. The strategy of using redox Co-based catalyst not only provides a potential catalyst for the reversible hydrogenation/oxidative dehydrogenation reactions but also replenishes methods for constructing of other redox catalyst, especially with AlN as a carrier.

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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Excellent quinoline additive in perovskite toward to efficient and stable perovskite solar cells

Guodong Li,Jihuai Wu,Jing Song,Chao Meng,Zeyu Song,Xiaobing Wang,Xuping Liu,Yuqian Yang,Deng Wang,Zhang Lan

The ionic nature of the perovskite material results in a great number of defects in the perovskite film which limits the efficiency and stability of perovskite solar cells . The passivation of the defects can effectively suppress the non-radiative recombination of carriers and improve the photovoltaic performance and stability of perovskite solar cells. In this paper, quinoline is introduced into the perovskite precursor solution . By adjusting the addition amount, it is found that quinoline can effectively induce the growth and orientation of perovskite crystals, consequently, improving the film quality and reduce defect density . The optimized device shows higher V OC (1.142 V) and FF (0.792), and achieved a champion power conversion efficiency of 20.87%. In addition, the hysteresis of the device is suppressed and the stability is improved. The results demonstrate that quinoline is an effective perovskite additive.

CAS / MDL: 91-22-5
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ENVIRONMENTAL POLLUTION · 2021 · IF 8.071

Rapid formation of pyrogenic char (biochar) with high and low sorption capacity towards organic chemicals

Zaiming Chen,Jianfei Wang,Yuefeng Wang,Bing Li,Meizhen Wang

Pyrogenic char (biochar) with a high sorption capacity (B-HSC) can sequester hazardous chemicals (e.g., phenanthrene). However, when sorption inhibits bioavailability of some functional chemicals (e.g., the herbicidal efficacy of diuron in soil), biochar with a low sorption capacity (B-LSC) is required to prevent sorption effects. The pyrolytic B-HSC generation has been reported, but information on B-LSC formation is scarce. How fast B-HSC and B-LSC could be generated is unknown until now. Here, biochars were rapidly prepared (the shortest heating time reached 5 min and the cooling time reached < 30 min) by a direct-pyrolysis method by directly exposing packaged rice straw and pine wood to 350 °C, 500 °C and 700 °C and out-of-furnace cooling at room temperature. The sorption of diuron, phenanthrene , and twelve other chemicals was investigated. B–HSCs were obtained within 30 min of rice straw pyrolysis , and the biochar K d values quickly increased to 7-730-fold that of the raw biomass as –OH and C–O–C in (hemi)cellulose of rice straw rapidly degraded, increasing hydrophobic interactions between the char and chemicals (solubility ≤ 82.8 g/L). In contrast, B-LSCs were generated within 30 min of PW pyrolysis, and the K d values of the biochars were 0.2–3.0-fold that of the raw biomass, as the surface area development and hydrophobicity-driven sorption were probably delayed by the late degradation of lignin aromatic C–O and phenolic –OH. Biochar amendment revealed an enhancement effect of B-HSC but not of B-LSC on soil sorption. The fast formation of B-LSC and B-HSC provides a guide to develop time- and cost-effective technique in pyrolytically producing weakly or strongly sorbing biochars for organic chemical management.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Highly efficient separation of indole from model wash oil using tetraethyl ammonium amino acid ionic liquids

Youan Ji,Yucui Hou,Shuhang Ren,Weize Wu

Indole is an important chemical that can be directly obtained from wash oil mixtures. In this work, several tetraethyl ammonium amino acid (TAAA) ionic liquids (ILs) were designed to separate indole from model wash oil through forming hydrogen bonds. The effects of important factors, such as stirring time, TAAA type, indole concentration, temperature, and TAAA:indole mole ratio, on indole separation were investigated. It is found that these TAAAs can separate indole from model wash oil with separation efficacy up to 98.0% (for tetraethylammonium L-alanine ionic liquid), and the ultimate indole concentration is 1.6 g/dm 3 . This separation process takes less than 5 min. Also, for one kind of TAAA, the ultimate indole concentrations are almost constant despite different initial indole concentrations. The maximum distribution coefficients of indole are 200.9 at the studied conditions. We have also found that water content in TAAA shows a negative effect on indole separation, which inspired us to design a process for TAAA regeneration using water. After regeneration, TAAA can be reused, and the separation efficacy of indole is not significantly reduced. The FT-IR results show that there are hydrogen bonds between TAAAs and indole. Finally, we compared the TAAA method to other methods and demonstrated the advantages.

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CHEMICAL ENGINEERING SCIENCE · 2020 · IF 3.871

Adjusting surface acidity of hollow mesoporous carbon nanospheres for enhanced adsorptive denitrogenation of fuels

Zimeng Li,Hongwei Liang,Xiaoling Li,Chen Yang,Bingqing Ge,Shaohui Xiong,Hongwei Zhang,Tinghai Wang,Pei Yuan

Mesoporous carbons are widely utilized as adsorbents for adsorptive removal of nitrogen-containing compounds in fuel. Herein, hollow mesoporous carbon nanospheres (HMCNs) were successfully synthesized via a facile silica-assisted sol–gel strategy and further oxidized by different acids (HNO 3 , H 2 SO 4 , and (NH 4 ) 2 S 2 O 8 ) to adjust their surface chemistry. The HMCNs oxidized with (NH 4 ) 2 S 2 O 8 contain the most oxygen-containing groups and exhibit the strongest acidity, resulting in high adsorption capacities towards quinoline (QUI, 29.78 mg N ·g −1 ) and indole (IND, 26.59 mg N ·g −1 ) in model fuel. The superior performance is attributed to the acid-base interaction and hydrogen bonding interaction between the adsorbent and QUI/IND molecules. Remarkably, the adsorption capacity towards nitrogen-containing compounds in real diesel is as high as 19.19 mg N ·g −1 at 50 °C. Our work has paved the way to the rational design and synthesis of high-performance adsorbents for the removal of nitrogen-containing compounds in real diesel on a large scale.

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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 18 ·7490-7500 · IF 3.288

Ultrafast synthesis of magnetic hollow carbon nanospheres for the adsorption of quinoline from coking wastewater

Yan Cui,Weiwei Kang,Lei Qin,Jinghong Ma,Xuguang Liu,Yongzhen Yang

Magnetic hollow carbon nanospheres (MHCNSs) with a uniform particle size (40 nm) were ultrafast synthesized in 80 s by a novel microwave-assisted solvothermal method. MHCNSs exhibited an abundant pore structure and high surface activity. Further, their growth mechanism and adsorption property towards quinoline in coking wastewater were discussed. The results indicate that the surfactant P123 plays a template role in inducing the growth of MHCNSs. At 298 K, MHCNSs exhibited a saturated adsorption amount of 155.23 mg g−1 towards quinoline in coking wastewater. Also, they showed excellent regeneration and magnetic separation properties. Through investigating the effect of pH, it was found that MHCNSs realized their best adsorption capacity at pH = 7, and they possessed a relatively stable adsorption capacity in slightly alkaline coking wastewater. The adsorption kinetics, isotherm and thermodynamics results demonstrate that the pseudo-second-order and Langmuir–Freundlich are the most suitable models for quinoline adsorption on MHCNSs, and the process belongs to spontaneous and exothermic chemisorption. In general, MHCNSs could be a potential adsorbent for the effective adsorption of quinoline from coking wastewater.

CAS / MDL: 91-22-5
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CATALYSIS LETTERS · 2020 ·Vol. 151 ·期 1 ·194-211 · IF 2.482

Steric Hindrance of Methyl Group on the Reaction Pathway of Hydrodesulfurization in the Presence of Quinoline

Chen Xilong,Dong Yanzeng,Yu Xiaohang,Wang Zhiheng,Liu Yanyan,Liu Jiankun,Yao Songdong

Abstract Steric hindrance of methyl on reaction pathway of hydrodesulfurization in presence of quinoline was investigated over a NiMo/Al 2 O 3 catalyst at 4.0 MPa and 320 °C. The results show that steric hindrance of methyl changed the main pathway of HDS while presence of quinoline further exacerbated this transformation. Changes in inhibitory factor curve show that quinoline poisoning on DBT HDS is a relatively mild. When adjacent methyl is present, even at low concentration, the inhibitory factor of quinoline on 4,6-DMDBT HDS is still greater than 85%. At high levels, the inhibitory factor of quinoline on DDS pathway even exceeds 99%. Quinoline poisons HYD pathway of DBT HDS to a stable level in a short time (30 to 60 min). However, after 6 h of reaction, HYD pathway yield of 4,6-DMDBT HDS is still increasing. Quinoline simultaneously poisons HYD and DDS pathways of 4,6-DMDBT HDS to a stable level within 120 min, and then DDS pathway will continue to be poisoned, thereby increasing HYD pathway yield. Regardless of presence of adjacent methyl in sulfur-containing molecules, an increase in quinoline concentration will lead to an increase in HYD/DDS pathway yield ratio. Addition of quinoline inhibits conversion of hydrogenated intermediates to DDS products by poisoning C–S bond dissociation center (such as CUS active site) and leads to formation of deep hydrogenated products. Graphic Abstract

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Micro & Nano Letters · 2019 ·Vol. 14 ·期 13 ·1287-1292 · IF 0.975

Magnetic composites Fe3O4@SiO2@PILs as sorbents for efficient denitrogenation of fuel oil

Feng Wang,Jie Li,Long Xu,Feng Jiang,Jianfeng Zhang

In this work, the study of synthesis and denitrogenation of magnetic polymeric ionic liquids (PILs) for N-compounds in simulated oils and diesel are reported. Three functionalised magnetic particles, Fe 3 O 4 @SiO 2 @PILs with side alkyl chain of C2, C4 and C6, respectively, were prepared by grafting PILs on the surface of silica-coated Fe 3 O 4 . Fourier transform infrared spectra, thermogravimetric analysis, X-ray diffraction and scanning electron microscopy were carried out to characterise the structure of Fe 3 O 4 @SiO 2 @PILs. It has shown that Fe 3 O 4 @SiO 2 @ PILs possess precious merits for sorbents, such as regular morphology, good stability and magnetic properties. Denitrogenation experiments of simulated oils demonstrate that Fe 3 O 4 @SiO 2 @ PILs show better denitrogenation efficiency of basic N-compounds than neutral N-compounds. The effects of temperature, reaction times, ratio of reagent to oil on denitrogenation for simulated oils were explored, and 92.1% denitrogenation efficiency was obtained to remove quinoline from simulated oils. Denitrogenation of Fe 3 O 4 @SiO 2 @PILs in diesel leads to 84.3% denitrogenation efficiency, and it can remain 82.5% denitrogenation efficiency after five times of recycles. Compared with other similar sorbents, Fe 3 O 4 @SiO 2 @PILs show competitive performances to eliminate organic N-compounds. It is hopeful that Fe 3 O 4 @SiO 2 @PILs can be promising sorbents for purification of liquid fuel by adsorptive denitrogenation.

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