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Catalysts · 2023 ·Vol. 13 ·期 5 ·857 · IF 3.9

The Construction of p/n-Cu2O Heterojunction Catalysts for Efficient CO2 Photoelectric Reduction

Qianqian Zhou,Yanxin Chen,Haoyan Shi,Rui Chen,Minghao Ji,Kexian Li,Hailong Wang,Xia Jiang,Canzhong Lu

Cu2O is a p-type direct bandgap semiconductor with a band gap of 2~2.2 eV, which has excellent visible light absorption and utilization. However, slow charge transfer and poor stability hinder its practical application. In this paper, a facile electrodeposition approach successfully synthesized the heterostructure of p-Cu2O and n-Cu2O. The protective layer of n-Cu2O on the surface of p-Cu2O nanoparticles forms a p/n heterojunction. Due to the p/n heterojunction, the PEC performance of p/n-Cu2O is enhanced significantly. The charge separation efficiency of photogenerated electron/hole pairs in p/n-Cu2O is greatly improved. Therefore, p/n-Cu2O shows superior photoelectrochemical (PEC) CO2reduction reaction (CO2RR) efficiency when used as a photocathode.Keywords:Cu2O;electrodeposition;p/n heterojunction;carbon dioxide reduction reaction

研究领域: 材料科学 · 环境科学
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

SnOx-Decorated Pt Catalysts for the Reductive N-Methylation of Quinoline with Methanol

Kun Li,Chengjie Duan,Weitao Mao,Dongliang Wang,Yumeng Liang,Wenbo Ye,Guangke He,Xiang Liu

A direct and efficient synthesis of N-methyl-1,2,3,4-tetrahydroquinolines (MTHQs) is achieved through the one-pot reductive N-methylation of quinolines. The SnOx-decorated Pt/Al2O3 (Pt-SnOx/Al2O3) catalyst proves to be highly effective in the transformation from quinolines to MTHQs, using methanol as the exclusive source for hydrogen (H) and methyl (CH3), without the addition of additional bases or additives. Mechanistic and kinetic studies reveal a tandem reaction pathway: (1) the dehydrogenation of methanol, (2) reduction of quinolines to 1,2,3,4-tetrahydroquinolines (THQs), and (3) N-methylation of THQs to MTHQs, with the dehydrogenation of methanol identified as the rate-determining step. Characterization and catalytic performance results demonstrate that SnOx modifies the morphology and electronic properties of Pt-based metal active sites, which dramatically facilitates the cleavage of O–H and less reactive C–H bonds in methanol, and maintains a delicate balance between methanol dehydrogenation and reductive N-methylation of quinolines, thus obtaining a high reactivity for the total transformation.

研究领域: 催化化学 · 有机合成
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2024 · IF 2

Measurement and Correlation of Liquid–Liquid Equilibrium Data for Separating Butyl Acetate from n-Octane Using Various Extractants

Chong Yang,Shimin Xu,Yuyao Xie,Pai Lu,Hui Wang,Lihua Cheng

In this study, a comprehensive investigation was conducted to gather fundamental data for the solvent extraction and separation of n-octane and butyl acetate. Various extractants, including furfural, dimethyl sulfoxide, N,N-dimethylformamide, N-formylmorpholine, ethylene glycol, and N-methylpyrrolidone, were employed to examine the extraction and separation of their mixtures. Measurements were conducted at constant pressure and temperature of 101.3 kPa and 298.2 K, respectively. The distribution constant, separation factor, and performance index were calculated from the obtained liquid–liquid equilibrium data, offering a quantitative assessment of the effectiveness of the extractants in extracting and separating n-octane and butyl acetate. The consistency of the LLE data was validated by using the Hand and Othmer–Tobias equations. Furthermore, the experimental data were successfully correlated using the NRTL and UNIQUAC thermodynamic models. The root-mean-square deviation was used to assess the difference between the calculated results and the experimental data. In addition, the obtained binary interaction parameters were validated using GMcal_TieLinesLL software developed by Marcilla and his collaborators. Our results demonstrate the accuracy and reliability of the experimental data and correlative models, offering valuable insights that will facilitate the future development of solvent extraction separation processes involving n-octane and butyl acetate.

研究领域: 化学工程 · 热力学 · 溶剂萃取 · 过程开发
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Nanoscale Research Letters · 2014 ·Vol. 9 ·期 1 ·1-7 · IF 2.481

Functionalized silicon quantum dots by N-vinylcarbazole: synthesis and spectroscopic properties

Ji Jianwei,Wang Guan,You Xiaozeng,Xu Xiangxing

Silicon quantum dots (Si QDs) attract increasing interest nowadays due to their excellent optical and electronic properties. However, only a few optoelectronic organic molecules were reported as ligands of colloidal Si QDs. In this report, N -vinylcarbazole - a material widely used in the optoelectronics industry - was used for the modification of Si QDs as ligands. This hybrid nanomaterial exhibits different spectroscopic properties from either free ligands or Si QDs alone. Possible mechanisms were discussed. This type of new functional Si QDs may find application potentials in bioimaging, photovoltaic, or optoelectronic devices.

CAS / MDL: 1484-13-5 108-67-8
研究领域: 材料科学 · 光学 · 生物医学工程
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Catalysts · 2023 ·Vol. 13 ·期 7 ·1060 · IF 3.9

Copper-Catalyzed N-Arylation of Pyranoquinolinones with Boronic Acids at Room Temperature without Ligand

Wei Gao,Fang Gao,Haikuan Yang,Zongde Wang,Yaru Huang

Pyranoquinolinones synthesized from citral were used for Cu-catalyzedN-arylation with a wide range of arylboric acids. The reaction proceeded well with a broad substrate scope, providing a direct way to access highly functional pyranoquinolinone core structure derivatives in yields of up to 80%. Compared to citral, the compounds we obtained have a much better inhibitory effect on HeLa cervical cancer cells, and compound3phas an IC50value of 4.6 μM, lower than cisplatin’s 5.9 μM.Keywords:citral;pyranoquinolinone;N-arylation

研究领域: 有机化学 · 药物化学 · 癌症研究
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Advanced Healthcare Materials · 2024 · IF 10

Magnesium-Impregnated Membrane Promotes Bone Regeneration in Rat Skull Defect by N-Linked Glycosylation of SPARC via MagT1

Weisin Chen,Hongwei Lu,Wenhao Yu,Lei Huang,Mengxuan Bian,Ning Wang,Xingdong Xiang,Guokang Mo,Cheng Zhang,Yulin Li,Libo Jiang,Jian Zhang

Autograft has long been the gold standard for various bone surgeries. Nevertheless, the increasing usage of synthetic implants is taking over the operation rooms due to biosafety and standardized protocols. To fulfill such tremendous needs, a magnesium-impregnated membrane is devised that steadily releases magnesium ions to stimulate osteogenesis. The compatibility of Magnesium oxide (MgO) particles is enhanced through hydration and grafting, characterized by scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). With detailed degradation profiles, an in-depth investigation of Magnesium transporter 1 (MagT1) for magnesium intake is carried out and engaging in the N-linked glycosylation by using RNAi and inhibitors. The glycosylation of secreted protein acidic and rich in cysteine (SPARC) affected extracellular secretion and mineral deposition, demonstrated by immunostaining and density-dependent color-SEM (DDC-SEM). Skull defects are treated by implanting magnesium-impregnated membranes in rats and evaluated them by micro-CT and histological exams. This study revealed the compatible integration of grafted magnesium hydroxide (g-MH) particles is the key to functional performance and critical to applicability in vivo; meanwhile, it opens the door to a biological rationale for designing biomimetic materials.

CAS / MDL: 301-10-0 67-66-3
研究领域: 生物医学工程 · 分子生物学 · 材料科学
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ADVANCED MATERIALS · 2024 · IF 27.4

Substrate Induced p–n Transition for Inverted Perovskite Solar Cells

Zhengbo Cui,Wen Li,Bo Feng,Yunfei Li,Xuemin Guo,Haobo Yuan,Qiang Weng,Tengyi You,Wenxiao Zhang,Xiaodong Li,Junfeng Fang

The p- or n-type property of semiconductor materials directly determine the final performance of photoelectronic devices. Generally, perovskite deposited on p-type substrate tends to be p-type, while perovskite deposited on n-type substrate tends to be n-type. Motived by this, a substrate-induced re-growth strategy is reported to induce p- to n-transition of perovskite surface in inverted perovskite solar cells (PSCs). p-type perovskite film is obtained and crystallized on p-type substrate first. Then an n-type ITO/SnO 2 substrate with saturated perovskite solution is pressed onto the perovskite film and annealed to induce the secondary re-growth of perovskite surface region. As a result, p- to n-type transition happens and induces an extra junction at perovskite surface region, thus enhancing the built-in potential and promoting carrier extraction in PSCs. Resulting inverted PSCs exhibit high efficiency of over 25% with good operational stability, retaining 90% of initial efficiency after maximum power point (MPP) tracking for 800 h at 65 °C with ISOS-L-2 protocol.

CAS / MDL: 109-86-4
研究领域: 材料科学 · 光伏技术 · 半导体物理
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Nature Protocols · 2024 · IF 13.1

Open-vessel polymerization of N-carboxyanhydride (NCA) for polypeptide synthesis

Wu Yueming,Chen Kang,Wang Jiangzhou,Dai Wenhui,Yu Haowen,Xie Xinyi,Chen Minzhang,Liu Runhui

Synthetic polypeptides, also known as poly(α-amino acids), have the same polyamide backbone structures as natural proteins and peptides. As an important class of biomaterials, polypeptides have been widely used because of their biocompatibility, bioactivity and biodegradability. Ring-opening polymerization of N -carboxyanhydride (NCA) is a classical and widely used method for the synthesis of polypeptides. The dominantly used primary amine–initiated NCA polymerization can yield well-defined polymers and complex macromolecular architectures, but the reaction is slow and sensitive to moisture, making it necessary to use anhydrous solvents and a glovebox. One solution is to use lithium hexamethyldisilazide (LiHMDS) as the initiator, as described in this protocol. LiHMDS-initiated NCA polymerization is less sensitive to moisture and can be carried out in an open vessel outside the glovebox. It is also very fast; the reaction can be complete within 5 min to produce 30-mer polypeptides. In this protocol, poly(γ-benzyl- l -glutamate) is prepared as an example, but the protocol can easily be adapted to the synthesis of other polypeptides by generating NCAs from different amino acids, making it particularly suitable for the efficient parallel synthesis of polypeptide libraries. We provide detailed procedures for NCA synthesis and purification, the method of polymer end-group modification and measurement of polymerization kinetics and reactivity ratio. The procedure for synthesis of monomers and polymerization to form polypeptides requires <1 d. The superfast and open-vessel NCA polymerization method described here will probably enable a wide range of applications in the synthesis and functional study of polypeptide biomaterials.

CAS / MDL: 7440-23-5
研究领域: 生物化学 · 高分子化学 · 材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

Transforming g-C3N4 from amphoteric to n-type semiconductor: The important role of p/n type on photoelectrochemical cathodic protection

Jiangping Jing,Zhuoyuan Chen,Chang Feng,Mengmeng Sun,Jian Hou

Photoelectrochemical cathodic protection is emerging as a green and environmental method to protect metals against corrosion. Graphitic carbon nitride (g-C 3 N 4 ) shows great application potential in this area because of its high efficiency, high stability and low cost. However, the pristine g-C 3 N 4 shows amphoteric properties, resulting in its failure in providing photoelectrochemical cathodic protection for the coupled metal in NaCl solution. In this work, a K&I co-doping technique was performed to modulate the band structure of g-C 3 N 4 , and an n-type g-C 3 N 4 (n-C 3 N 4 ) was obtained. The changes in the molecular structure were studied by SEM, HRTEM , XRD , EDS, XPS and FT-IR technologies. The n-type semiconductor characteristics were verified by the photoinduced i-V curves, SKP potential distributions and pH drift techniques. The n-C 3 N 4 can generate positive photocurrent in the whole investigated potential range, making it able to provide photoelectrochemical cathodic protection for the coupled 316L stainless steel in NaCl solution. This work is very helpful for promoting the application of g-C 3 N 4 in the fields of the photoelectric conversion and the photoelectrochemical cathodic protection.

研究领域: 材料科学 · 腐蚀与防护 · 电化学
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Molecular Catalysis · 2024 · IF 3.9

Photocatalytic N-formylation of amines with CO2 over Pt-Bi bimetallic decorated CeO2−x

Yi He,Peng Bai,Shibo Yuan,Jiafa Chen,Yicheng Zhao,Yongdan Li

N -formylation of amines with CO 2 is a promising approach to high-efficient utilization of CO 2 as C1 feedstock, while conventional thermocatalytic processes suffer from harsh reaction condition and intense energy consumption. In this work, photocatalytic N -formylation of amines with CO 2 is achieved at room temperature over Pt-Bi/CeO 2− x composite catalyst. The Pt-Bi bimetallic sites increase the concentration of surface oxygen vacancies. Furthermore, the synergistic effects of Pt and Bi improve the light absorption capacity, reduce the band gap energy of the photocatalyst and promote the separation of photoinduced charge carriers. Using PhSiH 3 as the reducing agent, the conversion of N -methylaniline reaches 100 % after 3 h irradiation in N, N -dimethylformamide solvent with a N- methylformanilide selectivity of 90.8 %. The composite photocatalyst shows promising cycling stability and universality.

研究领域: 化学 · 催化 · 材料科学 · 环境科学
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CHEMICAL ENGINEERING SCIENCE · 2024 · IF 4.1

Moderating acidity of ZSM-50 by Fe-substitution for n-Heptane isomerization

Bangjian Liu,Hong Yang,Huiqing Xu,Quanjie Liu,Shuandi Hou,Anfeng Zhang,Xinwen Guo

Effective regulation of acid sites is essential to strengthen the reaction performance and to modulate product distribution of an isomerization reaction. In this study, ZSM-50 (Al-EUO) and Fe-substituted ZSM-50 zeolites, namely FeAl-EUO-n (n = 0.25, 0.50 and 0.75) and Fe-EUO, are synthesized by a seed-assisted hydrothermal method. The study has shown that Fe has effectively entered the Al-EUO framework as a tetrahedrally-coordinated species. More importantly, the Fe-substitution has resulted in a significant increase in the amount of surface weak- and medium-strength Brönsted acids and a reduction in the strength of strong acids of FeAl-EUO-n. This study also evaluates the catalytic performance of Pt/FeAl-EUO-n catalysts in n-heptane hydroisomerization. It shows that the introduction of Fe in ZSM-50 greatly enhances the isomer yield, achieving a maximum yield of 66.1 % at 320 °C over Pt/FeAl-EUO-0.50 compared to 16.4 % at 300°C over Pt/Al-EUO. At the same time, the fraction of multi-branched iso -heptane also increases noticeably in the reaction product.

研究领域: 化学工程 · 材料科学
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AUSTRALIAN JOURNAL OF CHEMISTRY · 2013 ·Vol. 66 ·期 11 ·1361-1369 · IF 1.869

Stimuli-Responsive Films Based on N-Substituted Polyurethane with Different Alkyl Length

Yanyan Wang,Libin Liu,Congde Qiao,Tianduo Li

N-Alkyl-substituted polyurethanes with different alkyl chain lengths were prepared from the corresponding bromoalkane (1-bromooctane, 1-bromotetradecane, and 1-bromooctadecane) and polyurethane consisting of poly(propylene glycol) (PPG), 4,4′-diphenylmethane diisocyanate, and 1,4-butanediol. The synthesised materials were characterised by 1H NMR and FTIR spectroscopy and the degrees of substitution were discussed by changing the reaction conditions. Differential scanning calorimetry and X-ray diffraction were used to characterise the thermal properties and crystalline state. Microphase-separated nanostructures, with hard segments (nanofibre-like) embedded into amorphous PPG soft segments, are observed by atomic force microscopy and scanning electron microscopy. A reversible behaviour of the films was revealed by contact angle measurement. Stimuli-responsive films were realised by solvent vapour annealing and heat treatment, and exhibited a reversible switching in surface wettability with a remarkable change in the water contact angle of 21°.

研究领域: 高分子化学 · 材料科学 · 表面工程
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