JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2018
·Vol. 93
·期 10
·3028-3034
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IF 2.587
Wei Chen,Yong Sun,Juan Du,Zhihao Si,Xing Tang,Xianhai Zeng,Lu Lin,Shijie Liu,Tingzhou Lei
BACKGROUND 5-(Aminomethyl)-2-furanmethanol (AMF), used widely in medicinal chemistry, is usually synthesized by the reductive amination of furfural or 5-hydroxymethylfurfural (HMF) with ammonia. However, a challenging task when synthesizing this furyl primary amine is to enhance the selectivity of the product due to its high nucleophilicity. Conventional measures have used excessive liquid ammonia and precious metal catalysts. Usually, the molar ratio of ammonia to substrate is up to 30:1. This study employed aqueous ammonia to synthesize AMF by the direct reductive amination of HMF using the non-noble metal Ni/SBA-15 catalyst. RESULTS The Ni/SBA-15 catalyst displayed higher catalytic selectivity in the reductive amination of HMF to AMF compared to other precious metal catalysts, such as Ru/C, Pd/C and Pt/C. The AMF yield of 89.8% was obtained at the relatively mild reaction temperature of 100 °C for 4 h. After the fifth cycle, an acceptable decrease in catalytic activity with 74.2% yield of AMF was observed. CONCLUSION An improved process was developed for preparing AMF by the reductive amination of HMF with aqueous ammonia using the non-noble Ni/SBA-15 catalyst. The high selectivity of nickel catalyst is attributed mainly to the moderate catalytic activity. Moreover, a small amount of water enhanced the yield of AMF by promoting the formation of ammonium ions to prevent the further side reaction of AMF with HMF. Results of recycling experiments and analyses showed that agglomeration, loss and oxidization of nickel species together with carbon deposition were responsible for the slight deactivation of the catalyst. © 2018 Society of Chemical Industry
研究领域:
有机化学
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催化
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药物化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yingjie Niu,Shiying Zou,Haonan Liu,Minyue Hu,Jinjun Cai,Chao'en Li,Kathryn A. Mumford,Masood S. Alivand,Francesco Barzagli,Rui Zhang
Improving the energy efficiency of CO 2 desorption remains a key challenge in post-combustion carbon capture using amine solvents. In this work, a series of solid acid catalysts based on sulfonated mesoporous SBA-15 and functionalized with phosphotungstic acid (HPW) were synthesized via post-synthetic modification and applied to the catalytic regeneration of monoethanolamine (MEA). The catalysts, featuring both Brønsted and Lewis acid sites, were thoroughly characterized and tested in desorption experiments using CO 2 -loaded MEA solutions. Among the synthesized materials, HPW-SBA-15-SO 3 H-1 exhibited the best performance, achieving significantly higher CO 2 desorption rate and cyclic capacity compared to the uncatalyzed system, while reducing the relative heat duty by up to 37.7 %. This catalyst also demonstrated good stability over 20 absorption–desorption cycles, maintaining its structural integrity. In addition, machine learning was employed to correlate the catalysts' physicochemical features with their desorption performance, highlighting the role of acidity and porosity and supporting the proposed mechanism by which acidic sites promote carbamate decomposition and MEAH + deprotonation. These findings underscore the potential of functionalized mesoporous silica as efficient solid catalysts for lowering the regeneration energy penalty in MEA-based carbon capture systems.
研究领域:
化学工程
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材料科学
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环境科学
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催化
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机器学习
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产品关联
DOI
高影响因子
EUROPEAN POLYMER JOURNAL
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2020
·
IF 3.862
Xiang Xu,Junjie He,Yanning Zeng,Caili Yu,Faai Zhang
The surface-initiated metal-free atom transfer radical polymerization (ATRP) solution polymerization of methyl methacrylate was carried out for the first time on the basis of the reductive quenching mechanism. In this study, the 2-bromoisobutyryl bromide (BiBB) was anchored on the surface of self-synthesized rod-like mesoporous material SBA-15 as the initiator, with the commercially available organic dye fluorescein (FL) as photocatalyst and triethylamine (TEA) as electron donor under the irradiation of blue lamp. The obtained composites and polymers were characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, N 2 adsorption/desorption measurements, scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and gel permeation chromatography. The results demonstrated that the ordered mesoporous structure of SBA-15 was not disrupted after the polymerization. With an increase in illumination time, the grafting amount and the number average molecular weight of poly(methyl methacrylate) (PMMA) on the surface of SBA-15 linearly increased, and the molecular weight distribution ( Đ ) widened. PMMA with a relatively narrow Đ value was obtained after polymerization for 10 h (1.47). The increase in the grafting amount and molecular weight after chain extension confirmed the chain end functionality of PMMA grafted on SBA-15.
研究领域:
高分子化学
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材料科学
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纳米技术
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表面工程
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光化学
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DOI
高影响因子
Journal of Macromolecular Science Part B-Physics
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2024
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IF 1.2
Yangyang Zhao,Longshan Cheng,Liwei Wu,Shuang Cheng,Zhixiong Huang,Yanbing Wang
In this work, a mesoporous silica (SBA-15) was synthesized using a hydrothermal method and the surface of the SBA-15 was further modified by utilizing the organosilane compound γ- aminopropyltriethoxysilane(APTES); FT-IR testing confirmed the successful grafting of these organic groups onto the surface of the SBA-15, the result being the AP-S. Composite films were subsequently prepared through a casting method, with SBA-15 and AP-S serving as the inorganic filler particles, and PVA acting as the matrix material. These films were characterized by tensile texts, dynamic mechanical analysis, scanning electron microscopy, and dielectric measurements. The results showed that the tensile modulus, loss modulus and dielectric properties of the modified AP-S/PVA composite films were improved compared with those of SBA-15/PVA, with the tensile strength being the largest at 145.25 MPa when the AP-S content was 2%. This result combined with the SEM analysis, shows that the incorporation of SBA-15 modified by APTES into PVA films can effectively improve the dispersion of SBA-15 in the PVA films, which can also explain the performance enhancement.
研究领域:
材料科学
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高分子科学
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纳米技术
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化学工程
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复合材料
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2024
·
IF 7.1
Li Cui,Ren Gao,Qiaowei Zhang,Kun Jiang,Hongyan He,Wei-Lu Ding,Fangqin Cheng
Crown ethers (CEs) are promising materials for lithium isotope (6Li and 7Li) separation for their unique cavity structure and size effect, but the low partitioning of Li+ makes the practical implementation not applicable. The loss of CE molecules is also a critical problem. In this work, benzo-15-crown-5 functionalized imidazolium ionic liquids with different alkyl chain lengths ([Cn(B15C5)mim][NTf2], n = 6, 8, 10) are synthesized. The association constants of [Cn(B15C5)mim][NTf2] and Li+, Li+ partition, and the separation factor of 6Li and 7Li using [Cn(B15C5)mim][NTf2] were investigated. Compared with the B15C5 monomer, the covalent bonding of B15C5 onto the cation of imidazolium ILs contributes to the dramatic increase of binding ability toward Li+. The association constants of [Cn(B15C5)mim][NTf2] with Li+ increase with the elevation of the alkyl chain length due to the flexibility changes. However, [C8(B15C5)mim][NTf2] delivers the most outstanding partition coefficient of Li+ up to 7.59 with a separation factor of 1.033 (273 K), exceeding those reported for CE-based materials. The increased hydrophobicity of [Cn(B15C5)mim][NTf2] enables sustainable and robust use in the separation process. Both molecular dynamics simulations and interfacial tension experiments confirm that [C8(B15C5)mim][NTf2] exhibits the best affinity to the interfaces of dichloroethane/water. The coordination environment of Li+ can be tuned by regulating the length of the alkyl chains, resulting in different isotopic effects. This study offers a promising system for the effective and sustainable separation of 6Li and 7Li.
研究领域:
材料科学
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化学工程
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分析化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2025
·
IF 0
Maqinana Siphosethu,Kowenje Chrispin B. O.,Ojwach Stephen O.
Reactions of N 1 ,N 3 -bis(2-mercaptoethyl)isophthalamide with (3-aminopropyl)triethoxysilane (3-APTES) afforded the the corresponding Schiff base chelating ligand, (1Z,3Z)-N 1 ,N 3 -bis(2-mercaptoethyl)-N' 1 ,N' 3 bis(3(triethoxysilyl)propyl) isophthalimidamide ( L1 ) in high yields. Subsequent immobilization of L1 on mesoporous silica supports (SBA-15 and MCM-41) following a divergent method produced the respective fabricated L1@SBA-15 and L1@MCM-41 materials. Characterization of the fabricated chelating agents was accomplished using SEM, TEM, EDX, BET, PXRD, FT-IR, and TGA-DTA/DSC techniques. The fabricated materials were used as adsorbents for the removal of Cd(II), Pb(II) and Cr(VI) metal ions from water. Both the L1@SBA-15 and L1@MCM-41 materials demonstrated high extraction efficiencies for Cd(II) and Pb(II) cations, achieving over 98% and 97% removal, respectively, across a broad pH range (3–9). For Cr(VI) anions, relatively lower optimal extraction efficiencies of 67% and 77% were recorded between pH 3–12, for L1@SBA-15 and L1@MCM-41 , adsorbents, respectively. Faster extraction kinetics were observed for Cd(II) and Pb(II) cations, with over 94% removal achieved within 30 min, even at low initial metal concentrations (5 ppm) and adsorbent dosages (10 mg). Kinetic modelling showed that the adsorption process followed a pseudo -second-order kinetics, with high correlation coefficients (R 2 ) for Cd(II), Pb(II), and Cr(VI) of 0.97573, 0.97348, and 0.91017 using L1@MCM-41 , and 0.9754, 0.97089, and 0.89411 using L1@SBA-15 , respectively. Equilibrium data best fitted the Freundlich isotherm model, with R 2 values of 0.97952, 0.99892, and 0.97374 for L1@SBA-15 and 0.99879, 0.99999, and 0.90923 for L1@MCM-41 , corresponding to Cd(II), Pb(II), and Cr(VI), respectively. In competitive metal ion systems, the extraction selectivity followed the order Cd(II) > Pb(II) > Cr(VI), with L1@SBA-15 exhibiting superior overall performance compared to L1@MCM-41 . The extraction mechanism was postulated to occur through the coordination of the metal ions to the nitrogen/sulfur donor atoms in the chelating agents, consistent with the hard and soft acid and base (HSAB) principle. Furthermore, L1@MCM-41 demonstrated notable regeneration potential, retaining Cr(VI) extraction efficiencies over four successive cycles. Graphical
研究领域:
环境化学
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材料科学
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无机化学
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水处理技术
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吸附科学
✓ 已验证
产品关联
DOI
PubMed
Desalination and Water Treatment
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2024
·
IF 1
Qinglong Luo,Lei Liu,Ruiqiang Dong,Zhongfu Cheng,Mingzhe Dong,Zhijian Wu,Jun Li,Xueli Huang
ABSTRACT The removal of boron from aqueous solution and the enrichment of boron from salt lake have attracted more attention. In this work, organo-inorganic hybrid mesoporous boron adsorbents were synthesized by tris(hydroxymethyl)methyl aminomethane (TRIS) grafted onto the meso-porous SBA-15, SBA-16 and MCM-41, respectively. And the structures are characterized by infrared, scanning electron microscopy, energy-dispersive X-ray, mapping, X-ray diffraction, point of zero charge, and Marvin laser particle size analyzer. The results showed that TRIS was successfully grafted onto SBA-15, SBA-16, and MCM-41. The adsorption isotherm and adsorption kinetics were best fitted with Langmuir model and pseudo-second-order rate equation, respectively. The adsorption capacity of the three adsorbents was 15.28, 15.70 and 14.17 mg/g, respectively. And the same functional group has little influence on the boron adsorption capacity of different carrier adsorbents of the same type (organosilicon material). These adsorbents have highly selective adsorption of boron, and maintain good lifetime after adsorption–desorption for 5 times, and the dissolution loss rate of SBA-16-TRIS after ten cycles was 0.93%.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
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2024
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IF 10.5
Xiaoxuan Wang,Fangxuan Li,Jialu Zhang,Lu Guo,Mengmeng Shang,Xiao Sun,Shan Xiao,Dandan Shi,Dong Meng,Yading Zhao,Chao Jiang,Jie Li
PD-1/PD-L1-based immune checkpoint blockade therapy has shown limited benefits in tumor patients, partially attributed to the inadequate infiltration of immune effector cells within tumors. Here, we established a nanoplatform named DPPA/IL-15 NPs to target PD-L1 for the tumor delivery of IL-15 messenger RNA (mRNA). DPPA/IL-15 NPs were endowed with ultrasound responsiveness and contrast-enhanced ultrasound (CEUS) imaging performance. They effectively protected IL-15 mRNA from degradation and specifically transfected it into tumor cells through the utilization of ultrasound-targeted microbubble destruction (UTMD). This resulted in the activation of IL-15-related immune effector cells while blocking the PD-1/PD-L1 pathway. In addition, UTMD could generate reactive oxygen species (ROS) that induce endoplasmic reticulum (ER) stress-driven immunogenic cell death (ICD), initiating anti-tumor immunity. In vitro and in vivo studies revealed that this combination therapy could induce a robust systemic immune response and enhance anti-tumor efficacy. Thus, this combination therapy has the potential for clinical translation through enhanced immunotherapy and provides real-time ultrasound imaging guidance.
研究领域:
肿瘤学
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免疫学
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纳米技术
·
超声成像
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2015
·
IF 1.964
Huimin Liu,Yuming Li,Hao Wu,Jiaxiong Liu,Dehua He
Organic compounds containing multiple hydroxyl groups, namely α-cyclodextrin and γ-cyclodextrin, were used as additives for promoting Ni dispersion on supported Ni/SBA-15 catalysts. Catalysts prepared using modified and unmodified impregnation methods were characterized using N 2 adsorption-desorption isotherms, X-ray diffraction, transmission electron microscopy, temperature-programmed reduction, and thermogravimetric analysis, and their catalytic performance in the CO 2 reforming of methane (CRM) to syngas was evaluated. The results show that compared with Ni/SBA-15 prepared using a conventional impregnation method, the cyclodextrin-modified catalysts had smaller NiO particles. They also exhibited higher catalytic activity and had stronger ability to resist carbon deposition in the CRM. Mechanistic studies showed that for the unmodified catalysts, Ni 2+ could migrate into the channels of SBA-15 as a result of concentration differences, and the Ni species were sintered during the following thermal treatment processes, and could not be well dispersed. In contrast, various types of complex were formed between Ni(NO 3 ) 2 and the cyclodextrins, and this would be favorable for Ni 2+ being taken into the channels of the SBA-15. The presence of cyclodextrins was beneficial to the mutual isolation of Ni species, and finally resulted in better dispersion of Ni species.
研究领域:
催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
Environmental Science-Water Research & Technology
·
2022
·Vol. 8
·期 8
·1763-1776
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IF 5.819
Di Li,Mingyang Long,Qianqian Zhao,Hongmiao Li,Qi Wen,Fang Song
Nanosized CoTiO3, NiTiO3 and Fe2TiO5 photocatalysts were synthesized by a simple sol–gel method successfully. However, they showed lower photocatalytic activity for the degradation of oxytetracycline hydrochloride under visible light irradiation. After the CoTiO3, NiTiO3 and Fe2TiO5 nanoparticles were loaded in the SBA-15 channels, the photocatalytic activity was enhanced obviously. In order to further enhance the removal efficiency of CoTiO3/SBA-15, NiTiO3/SBA-15 and Fe2TiO5/SBA-15, they were used to activate peroxymonosulfate under visible light irradiation. In particular, CoTiO3/SBA-15 could completely photodegrade oxytetracycline hydrochloride with the assistance of peroxymonosulfate in an hour. The influencing factors on activating peroxymonosulfate to degrade oxytetracycline hydrochloride were investigated in detail. In addition, the electron transfer and peroxymonosulfate activation mechanism for the efficient improvement in the photocatalytic performance were also proposed and proved by radical quenching experiments, electron spin resonance analysis, X-ray photoelectron spectroscopy, transient photocurrent responses and cyclic voltammetry. It was found that the combined activation effects of photogenerated electrons and transition metals on peroxymonosulfate to produce sulfate radicals could enhance the degradation efficiency obviously. This study could provide a new way for the synergetic effect of photocatalysis and peroxymonosulfate activation by transition metal to be used for efficient photocatalytic degradation in the field of antibiotic removal.
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高影响因子
Catalysts
·
2021
·Vol. 11
·期 6
·710
·
IF 4.146
Linmeng Huo,Tian Wang,Keng Xuan,Lei Li,Yanfeng Pu,Chenxin Li,Congzhen Qiao,Hao Yang,Yan Bai
The adsorption and activation of both CO2and methanol are mainly affected by the distance of the Lewis acid site, Zr4+, and Lewis base, Zr4+/O2−, of the Zr-based catalysts. In this paper, Zr-incorporated SBA-15 (Zr-SBA-15) and Zr-grafted SBA-15 (Zr/SBA-15) catalysts were prepared with different Zr environments, and were analyzed with N2adsorption–desorption isotherms, X-ray diffraction, UV-vis spectra, and XPS. It was proposed that Zr-SBA-15 catalyst with Si-O-Zr-OH and Zr-O-Si-OH structure exhibited non-adjacent sites between Zr4+and Zr4+/O2−, while Zr/SBA-15 catalyst with Zr-O-Zr-OH structure showed neighboring sites between Zr4+and Zr4+/O2−. Furthermore, the Zr/SBA-15 catalyst exhibited good catalytic activity, while no DMC was detected over the Zr-SBA-15 catalyst at the same reaction conditions. For combined in situ infrared and catalytic performance, it was indicated that the methanol and CO2could be activated to form DMC, only when the Zr4+and Zr4+/O2−sites existed and were adjacent to each other in the Zr-O-Zr-OH of Zr/SBA-15 catalyst.Keywords:dimethyl carbonate;in situ FTIR spectra;ZrO2-grafted SBA-15;Zr-incorporated SBA-15;carbon dioxide
研究领域:
催化化学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Lin Dai,Jiaxin Xu,Jinbin Lin,Lingbin Wu,Huahua Cai,Jing Zou,Jun Ma
In this study, iodometric spectrophotometry , the most-used method for detecting peroxydisulfate (PDS), was modified by increasing the concentration of potassium iodide (KI) for realizing the immediate PDS determination and avoiding the interference of hydroxylamine. Kinetic studies showed that the reaction between PDS and I − to generate the yellow-colored I 3 − followed the kinetic equation as - d P D S d t = d I 3 - d t = 1 . 995 × 10 - 2 M - 2 · s - 1 · P D S 1 · I - 2 . Detection time of the iodometric spectrophotometry was shortened from 15 min to 15 s when KI concentration was increased from 0.6 M to 4.8 M. Different with the previous iodometric spectrophotometry, the modified method using 4.8 M KI as the indicator was well tolerable to the interference of hydroxylamine at acidic pH conditions. The calibration curve of the modified method showed a well linear relationship (R 2 = 0.999) between the absorbance of I 3 − at 352 nm and PDS concentration in the range of 0–80 μM. The modified method was highly sensitive with the absorptivity of 2.5 × 10 4 M −1 cm −1 and the limit of detection of 0.11 μM. Moreover, the modified method was successfully applied for monitoring the change of PDS concentration during the degradation of diclofenac with four different PDS-based AOPs , the calculated reaction stoichiometric efficiency ( R S E ( % ) = D i c l o f e n a c d e g r a d e d P D S c o n s u m e d × 100 % ) followed the order as heat/PDS system > hydroxylamine/Fe 2+ /PDS system > hydroxylamine/Cu 2+ /PDS system > Fe 2+ /PDS system.
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产品关联
DOI
PubMed
高影响因子
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