ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mei Ma,Jia-qi Bai,Huangfei Liu,Ben Liu,Zhangkai Qian,Suiqin Li,Jingshuai Chen,Mengdie Cai,Song Sun
The preparation of methyl-substituted amines by direct N-methylation of amines with CO2/H2 is an important reaction for CO2 utilization and organic synthesis. However, the design and construction of effective and stable non-noble-metal catalysts for this reaction remain challenging. Here, a cheap non-noble-Cu-based catalyst was prepared and applied in the direct N-methylation reaction of N-methylaniline with CO2 and H2. 5%Cu-ZnO(3.75%)/TiO2 showed 98.8% yield with an initial TOF of 7.7 h–1 after 24 h under 453 K, 1.5 MPa CO2, and 4.5 MPa H2, which was superior to 5%Cu/TiO2, 5%Cu/ZnO, and reported Cu-based catalysts. Furthermore, 5%Cu-ZnO(3.75%)/TiO2 can be reused at least four times and applied to the direct N-methylation of various amines with excellent selectivity. The various characterizations and experimental results showed that Cu0 was the active site, and 5%Cu-ZnO(3.75%)/TiO2 exhibited the largest surface Cu0 amount, thereby contributing to superior catalytic performance. The reaction mechanism of the direct N-methylation reaction of N-methylaniline with CO2 and H2 was proposed based on spectroscopic studies, kinetic studies, and control experiments. The reaction proceeded with the HCHO and N-methylformanilide intermediates, and the formation of HCHO from H2 and CO2 was the rate-determining step.
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ACS Nano
·
2024
·
IF 15.8
Jixi Zeng,Jing Wang,Jinzhao Wang,Jia Li,Jiwen Chen,Feng Wei,Jing Zhang,Weijie Song,Xi Fan
Flexible tin–lead (Sn–Pb) mixed perovskite solar cells (PSCs) are among the promising flexible photovoltaics, owing to the narrow bandgap (NBG) of Sn–Pb perovskites, flexible and wearable features, and their role as a critical component in all-perovskite tandem photovoltaics. However, the flexible Sn–Pb PSCs suffer from a low power conversion efficiency, no higher than 18.5%, along with limited stability. Herein, we reported an efficient and stable flexible NBG Sn–Pb PSC via an N,N′-carbonyldiimidazole (CDI) passivation strategy. CDI, with strong adsorption energy, preferentially binds to Sn2+ compared with oxygen (O2), thus effectively inhibiting the adsorption of O2 on perovskite surfaces. The transfer of electron density around Sn2+ dramatically decreased, thus suppressing Sn2+ oxidation. The CDI treatments endowed the Sn–Pb mixed films with fewer defects, improved crystallinity, better morphology, and matched energy-level alignment. The flexible Sn–Pb devices exhibited a high PCE of 21.02%. Besides, the devices showed enhanced stability and promoted flexibility. This work provides a pathway to visibly increase the efficiency and stability of the flexible Sn–Pb mixed photovoltaic cells.
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高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Xin Wang,Yubing Xu,Yuzhu Pan,Shunjie Chai,Jie Wu,Jingda Zhao,Yuwei Li,Zhiwei Zhao,Qing Li,Jun Wu,Jing Chen,Byung Seong Bae,Jianming Zhou,Ying Zhu,Wei Lei,Xiaobao Xu
Solution-processed lead halide perovskite single crystals (LHPSCs) are believed to have great potential in gamma-ray spectroscopy. However, obtaining low-defect LHPSCs from a solution at low temperatures is difficult compared to obtaining Bridgman single crystals such as CdTe and Si. Herein, noise from the intrinsic defects of LHPSCs is considered as the main problem hindering their gamma-ray detection performance. By isolating the defect-induced holes in LHPSCs via energy barriers, we show that NIN photodiodes based on three types of LHPSCs, i.e., MAPbBr3 (MA = CH3NH3), MAPbBr2.5Cl0.5, and cascade LHPSCs, have demonstrated good energy resolution in the range of 6.7–10.3% for 662 keV 137Cs gamma-ray photons. The noise for >10 mm3 devices is low, in the order of 340–860 electrons, and the electron collection efficiency reaches 23–43%. These results pave the way for obtaining low-cost, large, high energy-resolution gamma-ray detectors at room temperature (300 K).
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7208-7218
·
IF 6.177
Wenjing Song,Yujie Wan,Yuefeng Li,Xin Luo,Weiping Fang,Quanxing Zheng,Pengfei Ma,Jianping Zhang,Weikun Lai
Low cost and high efficiency catalysts for the reductive amination of carbonyl compounds are critical to the utilization of renewable biomass. In this paper, a highly efficient N-doped porous carbon supported Ni catalyst was prepared by a template-assisted pyrolysis and impregnation method. In the presence of NH3 and H2, the as-prepared catalyst could effectively catalyze the reductive amination of various carbonyl compounds into corresponding primary amines with high yield and excellent stability. Comprehensive characterization demonstrated that the reductive amination of furfural towards furfuryl amine was linked to the formation of Ni–Nx sites and the electronic interaction of N and Ni species on the N-doped carbon surface, which promoted the reductive amination of CO bonds and significantly reduced the activation energy in reductive ammonolysis of trimers and Schiff base intermediates. This work provided a new insight into rational design of reductive amination catalysts for primary amine production.
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
He Yingchun,Ma Dong-Dong,Ma Ke,Li Xiaofang,Han Lili,Wu Xin-Tao,Zhu Qi-Long
Electrochemically constructing C–N and N–C–N bonds provides an economical and sustainable alternative to conventional chemosynthesis. Herein, a hierarchically ordered open superstructure of N-doped carbon isolated with accessible three-coordinated Zn single-atom sites is explored for efficient electrocatalytic N–C–N coupling. Benefiting from the distinctive structural merits, this catalyst enables electrocatalytic preparation of N–C–N bonded compounds from methanol and amines. Notably, the Faradaic efficiency and selectivity of N,N,N’,N’ -tetramethyldiaminomethane reach up to 77% and 96% at 0.8 V, respectively. Further integrating the aminoalkylation reaction, an electro-thermo cascade synthesis is explored with the electrochemically obtained N,N,N’,N’ -tetramethyldiaminomethane serving as a unique reagent, leading to a specific set of organonitrogen compounds with (dimethylamino)methyl substituent, including topotecan hydrochloride, an anti-tumor drug, with a high yield of 95%. Furthermore, the in situ spectroscopic characterization and calculations unveil that the under-coordinated Zn-N 3 sites play a pivotal role in stabilizing the key *CH 2 O intermediate, thereby facilitating subsequent nucleophilic addition with amines.
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JOURNAL OF MEMBRANE SCIENCE
·
2011
·
IF 3.673
Xiao-Lin Li,Li-Ping Zhu,You-Yi Xu,Zhuan Yi,Bao-Ku Zhu
A novel method for the preparation of hydrophilic and positively charged nanofiltration (NF) membranes was developed. An active top-layer with NF characteristic was composited onto polysulfone (PSf) ultrafiltration substrate by UV-induced graft polymerization of N , N -dimethylaminoethyl methacrylate (DMAEMA) followed by quaternization cross-linking with p -xylylene dichloride (XDC). Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and atomic force microscopy were employed to monitor membrane surface chemical and morphological changes after poly(DMAEMA) grafting and quaternization cross-linking. The influences of UV irradiation time, monomer DMAEMA concentration, the cross-linker XDC concentration on the separation and permeation properties of membrane were investigated. The surface hydrophilicity of the composite membranes was evaluated by contact angle measurement. It was found that membrane hydrophilicity was obviously enhanced after UV-induced grafting and quaternization cross-linking. As the UV irradiation time and DMAEMA monomer concentration were increased, salts rejection of the composite membranes increased while water permeability decreased. Under the optimized preparing conditions, water flux and MgCl 2 rejection (1.0 g/L) of the composite membranes reached 60.3 L/(m 2 h MPa) and 93.2%, respectively. The membrane surface charge property was measured via a streaming potential method. It was found that, at pH from 4.5 to 9, the composite membranes showed positive zeta potentials. The rejections of the composite membranes to different salts followed the order Na 2 SO 4 < NaCl < MgSO 4 < MgCl 2 < CaCl 2 . Moreover, the composite NF membranes showed a good stability in water-phase filtration process.
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高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 21
·5663-5672
·
IF 7.779
Qixuan Qin,Asu Li,Yizhuo Fan,Xindong Zhang
In this work, Au nanoparticle-loaded ZnO/ZnFe2O4 (Au-ZnO/ZnFe2O4) microspheres were prepared using a combination of a two-step hydrothermal process and a co-precipitation method. The SEM and TEM analyses showed that the synthesized Au-ZnO/ZnFe2O4 samples were microspheres with a yolk–shell structure assembled from nanosheets. Gas-sensitive performance tests indicated that Au-ZnO/ZnFe2O4 showed the highest response to 100 ppm acetone (18.18), higher than those of ZnFe2O4 (8.4) and ZnO/ZnFe2O4 (11.6). In addition, the optimum operating temperature of Au-ZnO/ZnFe2O4 decreased from 279 to 206 °C compared to ZnFe2O4 and ZnO/ZnFe2O4. In addition, Au-ZnO/ZnFe2O4 yolk–shell microspheres exhibited fast response and recovery times (4 and 23 s, respectively). The sensor has a lower limit of acetone detection (0.7 ppm) at 85% RH and is able to effectively differentiate diabetic patients from healthy subjects by detecting acetone in their exhaled breath. The enhanced response of Au-ZnO/ZnFe2O4-based sensor is attributed not only to its high specific surface area but also to the synergistic effect of the n–n heterojunction structure of ZnO-ZnFe2O4 and the catalysis of Au nanoparticles.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·
IF 2.8
Boyun Gao,Huijiang Huang,Mooeez Ur Rehman,Bin Ren,Yuruo Liu,Weipeng Fan,Pengfei Li,Lizhi Zhang,Yan Xu,Yujun Zhao
BACKGROUND The synthesis of fatty amines via fatty alcohol amination offers a promising avenue for environmentally friendly production, particularly when compared with the methods employing hydrocyanic acid which often involve significant emissions. RESULT This study explores the synthesis of n-hexylamine through one-step amination of n-hexanol utilizing a series of Ru-doped Ni catalysts supported over γ-Al 2 O 3 , achieving 61% n-hexanol yield, 35% dihylamine yield and 3.5% trihylamine yield at the n-hexanol conversion of 99%. CONCLUSION The characterization results of the catalysts revealed a significant interaction between ruthenium and nickel in the bimetallic catalysts, leading to the enhanced reducibility of Ni species and improved metal dispersion. Moreover, ruthenium species were found to play an important role in the dissociation of NH 3 into NH x (x = 1, 2), thereby significantly improving the dehydrogenation process of n-hexanol at Ni sites. The synergistic effect between the two kinds of metal sites emerges as crucial factor for the boosted alcohols amination process. © 2024 Society of Chemical Industry (SCI).
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Industrial Chemistry & Materials
·
2022
·Vol. 1
·期 2
·240-246
·
IF 0
Hui Cao,Mengyu Dou,Zexiang Lyu,Yingxiong Wang,Christian Marcus Pedersen,Yan Qiao
Carbazole and anthracene, two aromatic hydrocarbon components contained in coal tar, are used as essential organic intermediates to synthesize various carbazole derivatives and anthraquinones. N,N-Dimethylformamide (DMF) is a commonly used solvent to extract carbazole from crude mixtures of carbazole and anthracene. However, the interaction between carbazole/anthracene and DMF in the extraction process is still to be fully understood at the molecular level. In this work, the intermolecular interaction of carbazole/anthracene with DMF was investigated using various NMR techniques, including 1H NMR titration, variable temperature NMR spectroscopy (VT-NMR), Nuclear Overhauser Effect Spectroscopy (NOESY), and diffusion-ordered spectroscopy (DOSY). The observed 1H chemical shift changes of carbazole indicated strong intermolecular hydrogen bonds between carbazole and DMF, which was further supported by the decrease in the molecular self-diffusion coefficients (D) of both carbazole and DMF according to DOSY measurements. Moreover, NOESY experiments revealed that the distance between the aldehydic hydrogen of DMF and the N–H of carbazole was smaller than 5 Å. Accordingly, an intermolecular hydrogen bond between carbazole and DMF in the form of CO⋯H–N was proposed. This research increases our knowledge about the separation process of carbazole and anthracene and hence helps improve the methods.
Keywords: NMR; Carbazole; Separation; Intermolecular hydrogen bonds.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Sarula Li,Zheyan Hu,Tianqi Wang,Fang Song,Hong Shao,Feng Li,Xiangting Dong
Triethylamine (TEA) gas is a kind of toxic gas that can lead to health problems. In this work, a novel Janus structure nanofibers (NFs) have been synthesized via a parallel electrospinning method. SnO 2 and In 2 O 3 are selected as the components of the Janus structure and different ratios of SnO 2 and In 2 O 3 in Janus structure are regulated. To investigate its TEA sensing application, gas sensors have been fabricated and the concentration of TEA gas is set at 20 ppm. The gas sensing results indicate that the optimum ratio of SnO 2 to In 2 O 3 is 1:1 and the gas sensors exhibit good sensing performances including a good response (8.45), short response time (4 s), high signal-to-noise ratio (4.45) and stable reproducibility. The improved gas sensing performances can be attributed to the n-n type Janus heterostructure interface. This research may make contributions to the development of semiconductor heterostructure sensing materials and gas sensors.
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KEY ENGINEERING MATERIALS
·
2012
·
IF 0
Xuan Min Zhu,Xiu Jian Zhao,Zhi Yong Ning,Xiao Tao Sui
Nanosized silver (Ag) was synthesized by reducing high concentration AgNO3 in N, N-dimethylformamide (DMF), in the presence of stabilizer polyvinyl pyrrolidone (PVP). PVP of two different molecular weights (MW=40000, 1300000) at the reaction temperature of 80°C and 100°C were tested for the effect on the formation of diverse silver nanoparticles. Our results indicated that the PVP with different molecular weights plays different role in the controlling of the Ag nanostructure owing to the PVP molecular selective adsorption on different crystal facets, thus affecting the growth rate of different facets of Ag nanoparticles. When all the other conditions kept the same and the temperature of 100°C, if PVP (Mw=40,000) was used, only a small amount of Ag decahedra were found. However, when the PVP with larger molecular weight such as PVP K88 (Mw=1300, 000), a large quantity of the triangular nanoprisms existed in the final solution in spite of the minority of quasi-sphere. The growth process and causation of different silver morphology with two distinct PVP have been briefly discussed.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·125570
·
IF 7.5
Yan Zhang,Guannan Ren,Hongfen Zuo,Mingjia Liao,Ningrui Zhang,Zhou Xu,Genghao Gong
An interlayer regulates organosilica deposition on porous polymer supports. • A 150 nm organosilica layer was obtained after two spray cycles. • The membrane achieved a flux of about 1.0 kg m⁻² h⁻¹ for DMF dehydration. • The membrane maintained relatively stable performance over 50 h. Pervaporation dehydration of N,N-dimethylformamide (DMF) is challenging because low-viscosity organosilica sols can penetrate porous polymer supports during selective-layer deposition. In this work, a polyarylate (PAR) interlayer was introduced onto a porous poly(ether ether ketone) (PEEK) support by interfacial polymerization to regulate the deposition of a bis(triethoxysilyl)ethane (BTESE)-derived organosilica layer by ultrasonic spray coating. Cross-sectional SEM observations showed that the PAR interlayer reduced BTESE-sol penetration into the porous PEEK support and facilitated the formation of a relatively thin BTESE-derived layer. The selected membrane prepared with two spray-coating cycles exhibited a BTESE-layer thickness of approximately 150 nm. For a 90 wt% DMF/water feed at 50°C, the membrane achieved a total permeation flux of approximately 1.0 kg m⁻² h⁻¹ with a separation factor of 3–4. During 50 h of continuous operation, the permeation flux decreased initially and subsequently remained relatively stable, while the separation performance showed no pronounced deterioration under the tested conditions. Additional pervaporation experiments with NMP/water and DMAc/water mixtures showed different permeation and separation behaviors. Overall, the results indicate that the PAR interlayer can regulate BTESE-sol deposition on the porous PEEK support and facilitate the fabrication of a thin organosilica composite membrane for pervaporation dehydration under the investigated conditions. Download: Download high-res image (287KB) Download: Download full-size image
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