Nature Protocols
·
2026
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IF 16
Wu Yongmeng,Liu Xinyu,Huang Yanmei,Meng Nannan,Zhang Bin
The construction of carbon‒nitrogen (C‒N) bonds is an essential transformation for synthesizing value-added organonitrogen compounds, including the raw materials for fertilizers, synthetic materials and pharmaceuticals. Electrocatalytic C‒N bond construction has emerged as an alternative strategy to traditional thermochemical routes, avoiding harsh and energy-intensive processes. This protocol describes an electrocatalytic C‒N bond construction strategy to synthesize organonitrogen from nitrogen oxides in water under ambient conditions, with a focus on several vital chemicals, such as urea, formamide, cyclohexanone oxime, amino acids and 15 N-labeled amino acids. Here, we provide detailed procedures for catalyst and reaction device design, electrosynthesis, product quantification and measurements for investigating the reaction mechanisms. Four catalysts, namely, vacancy-rich ZnO, core-shell Cu@Zn, AgRu alloy and low-coordination Ag, are synthesized as cathode catalysts. Two types of electrolyzers, an H-type cell and a flow cell, are used for the electrocatalytic reaction. Characterization techniques such as electrochemical in situ Raman spectroscopy, in situ attenuated total reflectance–Fourier transform infrared spectroscopy, ex situ electron paramagnetic resonance and scanning flow cell-differential electrochemical mass spectrometry have been adopted to study the reaction mechanism. The synthesis amount of urea is at the micromole level, while the synthesis amounts of formamide, cyclohexanone oxime and amino acids are at the millimole level. The catalyst synthesis protocol requires 0.5–1.5 d, the electrosynthesis requires ≤11 h and the in situ characterization requires 0.5–1.5 h.
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Materials Science & Engineering C-Materials for Biological Applications
·
2014
·
IF 2.736
Xiaomo Li,Hui Zhong,Xiaorong Li,Feifei Jia,Zhipeng Cheng,Lili Zhang,Jingzhou Yin,Litao An,Liping Guo
Environmentally sensitive hydrogels as one of the most potential drug delivery systems have gained considerable interest in recent years. In the present study, we synthesized a newly temperature-responsive composite hydrogel based on attapulgite (ATP) and poly (N-isopropylacrylamide) (PNIPAM) as the localized drug carriers for drug delivery. The as-prepared ATP/PNIPAM hydrogel has large aperture which significantly improved the quantity of adsorption of drugs, exhibiting the excellent properties of drug release. The scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and X-ray diffraction (XRD) were used to characterize the ATP/PNIPAM. The swelling/deswelling behaviors and the release of ciprofloxacin lactate were studied. When the temperature was below the low critical solution temperature (LCST), the swelling property of hydrogels was excellent and the swelling rate was large. And, the drug release rate increased with the increase of the content of attapulgite in the composite hydrogel when it was put in the buffer solution (pH 7.38) at 37.0 °C. Therefore, the composite hydrogels might be very useful for its application in biomedical fields.
研究领域:
材料科学
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药物递送
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高分子化学
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生物医学工程
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智能水凝胶
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
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IF 5.2
Mingwei Zhang,Linlin Liu,Wenjun Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
ZSM-48 is widely used to support Pt nanoparticles (Pt/ZSM-48) for hydroisomerization of long-chain n -paraffin due to its 10-member-ring one-dimensional pore structure . But the yield of target isomers on Pt/ZSM-48 is difficult to be improved due to easily bundled crystal bars and relatively excessive acid sites of ZSM-48, which restricts reactant diffusion and causes cracking. In this study, different types of zeolite growth modifiers (ZGMs) are screened for regulating the physicochemical property of ZSM-48, in which phenolic hydroxyl was found to be the most effective functional group. Quantitative correlations between ZGM structure and the properties of corresponding ZSM-48 crystal are achieved based on appropriate descriptors and multi-parameter regression. Then, the mechanism of ZSM-48 regulation by phenolic ZGMs is revealed. The models predict that polydopamine (PDA) is a superior ZGM for hydroisomerization, which is verified by textural characterization and reaction evaluation. Compared with the conventional catalyst, the isomer selectivity was improved effectively from 92% to over 97% when the feed conversion was lower than 80%, and the maximum yield of isomers was 89.0% as catalyzed by the PDA-regulated catalyst. The as-built models can also be used to design preferred phenolic ZGMs for preparing tailored ZSM-48 in other applications.
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ZEITSCHRIFT FUR KRISTALLOGRAPHIE-NEW CRYSTAL STRUCTURES
·
2023
·Vol. 238
·期 4
·799-800
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IF 0.3
Yu-Pei Xia
C 4 H 13 Cl 2 N 5 , monoclinic, P 2 1 (no. 4), a = 7.1868(6) Å, b = 5.8408(4) Å, c = 12.6534(11) Å, β =
105.134
(
2
)
∘
, V = 512.73(7) Å 3 , Z = 2, R
gt ( F ) = 0.0354, wR
ref ( F
2 ) = 0.0961, T = 298 K.
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JOURNAL OF ORGANIC CHEMISTRY
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2023
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IF 3.6
Xinhan Li,Hengyuan Zhao,Li Meng,Jun Dong,Chunhui Yang,Zixiang Wei,Xianming Wang,Jianbin Xu,Baomin Fan
The ability to selectively synthesize multiple products from the same sets of substrates is a highly appealing and challenging concept in synthetic chemistry. In this manuscript, we describe the visible-light photoredox intermolecular catalysis of N-arylacrylamides that are α-C–H functionalized with aryl tertiary amines. The photocatalyst acts as a chemical switch to trigger two different reaction pathways and to obtain two different products from the same starting material. Simple adjustments to the reaction conditions enable the divergent synthesis of the oxidative cyclizations or the addition products in good to high yields with excellent atom economy.
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Coatings
·
2023
·Vol. 13
·期 2
·431
·
IF 3.4
Chao Liu,Zhenxiang Chen,Ruiqin Kang,Jing Wang,Qingwei Lu,Tao Wang,Dayong Tian,Ying Xu,Zhan Wang,Huiping Ding
The fabrication of a green, high activity and low-cost carbon-based catalyst capable of activating new oxidant (peroxymonosulfate, PMS) for contaminants abatement is needed. In this research, we prepared novel N-doped biochars via one-step pyrolysis of algal sludge without external nitrogen sources. The obtained ASBC800 possessed the largest specific surface area (SBET= 145.596 m2g−1) and thus it displayed the best catalytic performance, as revealed by the effective elimination of sulfadiazine (SDZ, >95% within 70 min) with 0.2 g L−1ASBC800 and 0.5 mM PMS. Both radical species (e.g., SO4•−, and•OH), and nonradical regime (1O2and electron-transfer) contributed to SDZ oxidation, in which ASBC800 played essential roles in activating PMS, accumulating SDZ, and regulating electron shuttle from SDZ to ASBC800-PMS*. Overall, this work not only provides a novel strategy for the synthesis of N-rich and cost-effective biochar but also promotes the development and application of carbon-based functional materials in environmental remediation.Keywords:peroxymonosulfate;pre-adsorption;oxidation;electron-transfer;N doping
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LANGMUIR
·
2022
·
IF 4.331
Hui Zhang,Yi Li,Junping Miao,Xinran Zhu,Jing Yang,Qinglei Zhang,Yanfu Yang,Junqiang Zhao,Yunxia Hu,Yiping Zhao,Li Chen
N-Oxide zwitterionic polyethyleneimine (ZPEI), a new kind of aqueous phase monomer synthesized by commercially branched polyethyleneimine (PEI) via oxidation reaction, was prepared for fabrication of thin-film composite (TFC) polyamide membranes via interfacial polymerization. The main factors, including the monomer concentration and immersion time of the aqueous phase and organic phase, were investigated. Compared with PEI-TFC membranes, the obtained optimal defect-free ZPEI-TFC membranes exhibited a lower roughness (3.3 ± 0.3 nm), a better surface hydrophilicity, and a smaller pore size (238 Da of MWCO). The positively charged ZPEI-TFC membranes (isoelectric point at pH 8.05) showed higher rejections toward both divalent cationic (MgCl2, 93.0%) and anionic (Na2SO4, 96.1%) salts with a water permeation flux of up to 81.0 L·m–2·h–1 at 6 bar, which surpassed currently reported membranes. More importantly, mainly owing to N-oxide zwitterion with strong hydration capability, ZPEI-TFC membranes displayed a high flux recovery ratio (97.0%) toward a model protein contaminant (bovine serum albumin), indicating good anti-fouling properties. Therefore, the novel N-oxide zwitterion functionalized positively charged nanofiltration membranes provide an alternative for water desalination and sewage reclamation.
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Small
·
2023
·
IF 13.3
Shuyang Peng,Di Liu,Keyu An,Zhiqin Ying,Mingpeng Chen,Jinxian Feng,Kin Ho Lo,Hui Pan
Green hydrogen is considered to be the key for solving the emerging energy and environmental issues. The photoelectrochemical (PEC) process for the production of green hydrogen has been widely investigated because solar power is clean and renewable. However, mass production in this way is still far away from reality. Here, a Si photoanode is reported with CoO x as co-catalyst for efficient water oxidation. It is found that a high photovoltage of 350 mV can be achieved in 1.0 m K 3 BO 3 . Importantly, the photovoltage can be further increased to 650 mV and the fill factor of 0.62 is obtained in 1.0 m K 3 BO 3 by incorporating Mo into CoO x . The Mo-incorporated photoanode is also highly stable. It is shown that the incorporation of Mo can reduce the particle size of co-catalyst on the Si surface, improve the particle-distribution uniformity, and increase the density of particles, which can effectively enhance the light absorption and the electrochemical active surface area. Importantly, the Mo-incorporation results in high energy barrier in the heterojunction. All of these factors are attributed to improved the PEC performance. These findings may provide new strategies to maximize the solar-to-fuel efficiency by tuning the co-catalysts on the Si surface.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Zixuan Ou,Xindi Chen,Xinming Wu,Changren Zhou,Kaijie Zhang,Jingyang Luo,Fang Fang,Yinqiang Sun,Ming Li,Qian Feng
While pioneering methods have demonstrated that bacterial N-acyl homoserine lactone (AHL) signaling molecules can influence the growth and self-aggregation of suspended microalgae, whether AHLs can affect the initial adhesion to a carrier has remained an open question. Here we revealed that the microalgae exhibited different adhesion potential under AHL mediation, where the performance was affiliated to both AHL types and concentrations. The result can be well explained by the interaction energy theory, where the energy barrier between the carriers and the cells varied due to AHL mediation. Depth analyses revealed that AHL acted through modifying the properties of the surface electron donor of the cells, which were dependent upon three major components, i.e. , extracellular protein (PN) secretion, the PN secondary structure, and the PN amino acid composition. These findings expand the known diversity of AHLs mediation on microalgal initial adhesion and metabolisms, which may interface with other major cycles and become helpful to theoretically guide the application of AHLs in microalgal culture and harvesting.
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Journal of Coatings Technology and Research
·
2023
·
IF 2.3
Meng Fangfei,Wang Wenjin,Yu Yijia,Xia Wenjuan,Wang Ling,Wu Zhaoqiang,Chen Hong
A simple and convenient strategy for fabricating superhydrophilic multifunctional antifogging coatings was developed by hydrolyzing triethoxysilyl-terminated poly( N -vinylpyrrolidone) (TRES-PVP) with tetraethyl orthosilicate (TEOS) under acidic conditions. These antifogging coatings can be easily obtained by coating TRES-PVP hydrolysates on substrates at room temperature and then curing by thermal treatment. The superhydrophilic transparent coatings exhibited excellent antifogging, self-cleaning and antifouling properties. Additionally, the coatings also have good adhesion against the cross-cut test and remain stable after exposure to the laboratory environment for five months or immersion in water at room temperature for 20 days. Therefore, the present TRES-PVP hydrolysate coatings are promising for practical multifunctional antifogging applications.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 37
·e54400
·
IF 3
Xiaowei Jiang,Zhihong Liu,Yujiao Tan,Xiaosong Chen,Ping Huang,Libo Ma,Xu Xiong,Weibin Gao,Yu Tao,Hongxia Lu,Zheng Dai
Nitrogen atoms has been widely adopted in preparation of porous organic polymers (POPs). In our study, flexible nitrogen porous organic polymers (FNPOPs) with high nitrogen content are synthesized by using acetic acid both as solvent and catalyst. The materials show moderate Brunauer–Emmett–Teller (BET) surface area and outstanding thermal stabilities ( T d : 330°C). FNPOP-2 is prepared into phase change material (PCM) composites by self-adsorption method. From differential scanning calorimetry (DSC) analysis, the PCM composites show high encapsulation ratio (55.2 wt%) and latent heat (135.7 J g −1 ) due to flexible structure and high nitrogen atomic content. Furthermore, the thermal energy storage properties of all PCM composites remained after several thermal cycles. In general, FNPOPs have potential applications in phase change materials adsorption and thermal energy storage.
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FUEL
·
2022
·
IF 8.035
Hu Liu,Jingwen Xue,Pengfei Yu,Yankang Zhang,Jinhua Wang,Defu Che
Hydrogen is a clean secondary energy as well as an efficient energy carrier, but the low density and small molecular hydrogen result in high economic and energetic efforts to store and transport hydrogen. In addition, the hydrogen produced by the current industry is usually impure and requires gas separation, which consequently increases the cost of hydrogen. A promising hydrogen storage technology using liquid organic hydrogen carrier (LOHC) can permit the safe storage of hydrogen for long time through the reversible chemical reaction in the presence of catalyst. The selective hydrogenation reaction of N -ethylcarbazole (NEC), an attractive LOHC compound due to the low dehydrogenation temperature of perhydro- N -ethylcarbazole (12H-NEC), with hydrogen was conducted in this study to achieve both separation and hydrogen storage for hydrogen-rich raw gas from natural gas steam reforming. First, hydrogenation experiments of molten NEC under a pure hydrogen atmosphere were carried out to determine the suitable hydrogenation conditions and reaction pathways. Then, the effect of methane addition on NEC hydrogenation was analyzed. Results indicate that there are multiple parallel pathways in the hydrogenation of NEC. The reaction rate from 8H-NEC to 12H-NEC step is extremely slow and this step is unstable at 453 K. The optimal hydrogenation temperature of NEC is 443 K and the apparent activation energy is 67.6 kJ·mol −1 . The addition of methane reduces the initial reaction rate from 0.877 g H2 ·(g Ru ·min) −1 to 0.640 g H2 ·(g Ru ·min) −1 but increases the maximum degree of hydrogenation ( DoH ) from 0.870 to 0.909.
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