CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Yu-Shuai Xu,Hong-Hui Wang,Qi-Yuan Li,Shi-Nan Zhang,Si-Yuan Xia,Dong Xu,Wei-Wei Lei,Jie-Sheng Chen,Xin-Hao Li
The development of two-dimensional heterogeneous catalysts with highly exposed active site areas for heterogeneous catalytic systems is highly promising for achieving the green transformation of small molecules. 2D transition metal carbides (TMCs) show great promise for catalysis and carbon capture but suffer from heavy aggregation and autooxidation. Mass transfer barrier is also a standard problem of lamellar TMCs caused by slight aggregation of layers. Here, we successfully developed a method to prepare “ladder-like” heterojunctions of Mo 2 C layers confined inside nitrogen-rich carbon sheaths (2D-Mo 2 C@NC) via an effective oxygen-diffusion etching strategy, acting as efficient catalysts for CO 2 fixation. The enhanced electron enrichment of the as-integrated 2D-Mo 2 C subunits induced by the Schottky barrier could further keep the exposed Mo 2 C surface from possible autooxidation and aggregation confronted by conventional 2D TMCs. The experimental results and density functional theory (DFT) calculation further demonstrate that electron-rich Mo 2 C could boost the adsorption and activation of CO 2 for universal carbonylation of various diamines, providing a turnover frequency value (TOF) of 10.2 h −1 to produce benzimidazolone, which is 5.2 times of that of the state-of-the-art catalyst in the literature under even critical conditions.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2017
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IF 4.421
Yuanfeng Wu,Xianghai Song,Shuai Li,Jiahui Zhang,Xinghui Yang,Pengxin Shen,Lijing Gao,Ruiping Wei,Jin Zhang,Guomin Xiao
[(CH 3 ) 2 NH 2 ][M 3 (BTC)(HCOO) 4 (H 2 O)] . H 2 O (M–BTC, M = Mn, Ni, Co) were prepared under hydrothermal conditions and used as highly efficient catalysts for cycloaddition of CO 2 with epichlorohydrin (ECH). The microstructure and physicochemical properties of the compounds were determined by PXRD, FT-IR, XPS, N 2 -adsorption, TG–DSC, NH 3 –TPD and CO 2 –TPD. 98.01% conversion of ECH and 96.05% selectivity to chloropropene carbonate was obtained over the Mn–BTC under the optimized reaction conditions (105 °C, 3.0 MPa, 9 h, 1.5 wt.% of ECH). Besides, the recyclability result exhibited the Mn–BTC compound can be utilized as least three times with a slight reduction in its catalytic ability. In addition, cycloaddition of CO 2 with other epoxides and DFT calculation were also performed. The result exhibited the yield followed the order: ECH > 1, 2-epoxybutane > propene oxide > Allyl glycidyl ether, which was mainly determined by the energy of reaction.
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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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2022
·Vol. 153
·期 11
·3383-3391
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IF 2.936
Zhang Luping,Tu Xuewei,Han Weihang,Chen Liangchen,Chen Yutong,Zheng Hui
As the main resource of greenhouse gas, CO 2 needs to be fixed into different chemicals to relieve the environmental problem. Fe-based catalyst and g-C 3 N 4 have received extensive attention due to their easy preparation, low cost, and environmental friendliness. Herein, a heterogeneous catalyst system consisting of rich-electron g-C 3 N 4 and strong electron-withdrawing groups Fe-complex [Fe(bpy)(CO) 2 (Cl) 2 ] was developed, which could promote electron transfer and enhance the electronic interaction for fixing CO 2 . o -phenylenediamine substrates with different electron-donating/withdrawing groups were employed to fix CO 2 into high-valued heterocycle benzimidazoles. The optimum reaction conditions were examined by orthogonal experiments. A series of benzimidazole derivatives were synthesized with yield up to 98%, which indicated the catalyst had the ability of fixing CO 2 . This catalyst provides a new pathway for fixing CO 2 into valuable benzimidazole derivatives. Graphical Abstract
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Dandan Ma,Zhonghan Cheng,Ye Yuan,Somboon Chaemchuen
The heterometal functionalization on zeolitic-imidazole frameworks (ZIFs) is a strategy to modify properties over the homometal ZIFs. A green strategy for simultaneously functionalized iron atoms during the crystal formation of ZIF-67 (Fe@ZIF-67) through the solid-solid thermal (SST) method is newly developed. The single-step process and absent solvent conditions are beneficial advantages of this SST method over the early reported synthetic methods. The results show that the iron is well-dispersed and homogeneously coordinated in the structure of Fe@ZIF-67. Moreover, the optimal iron-functionalized ZIF-67 (20Fe@ZIF-67) significantly enhances the catalytic performance of CO 2 cycloaddition epoxide by 2.3 times compared to pristine ZIF-67 under mild reaction conditions. The DFT calculation reveals that the iron atom induces the unsaturated sites or defect structure on the Fe@ZIF-67 catalyst, providing more reactive sites for the catalytic activity of the reaction.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
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2023
·Vol. 13
·期 5
·689-698
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IF 2.2
Xuewei Tu,Luping Zhang,Yutong Chen,Shouxin Zhu,Can Sun,Jiali Jin,Min Liu,Hui Zheng
The conversion of CO 2 into valuable chemicals to reduce greenhouse gas emissions has received extensive attention. Converting CO 2 into pharmaceutical intermediates via graphitic carbon nitride (CN) at atmospheric pressure is a challenge. In this work, a series of novel graphitic carbon nitrides (K-CN) catalysts with different doping ratios of K were synthesized by post-treatment of CN with KOH as a dopant under magnetic stirring. Herein, substrates of o -phenylenediamine with different electron-donating/withdrawing groups were employed to convert CO 2 into high-value heterocyclic benzimidazoles. The optimal reaction conditions were determined by a single factor optimization approach. A series of benzimidazole derivatives were synthesized with a yield of up to 96% under atmospheric pressure, indicating that the catalyst can efficiently fix CO 2 . This work not only designs a simple and low-cost K-CN catalyst but also provides a new pathway for converting CO 2 into valuable benzimidazole derivatives at atmospheric pressure. © 2023 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
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2021
·Vol. 23
·期 21
·8571-8580
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IF 10.182
Yuting He,Huimin Lu,Xue Li,Jun Wu,Tiancheng Pu,Wei Du,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
The multi-step reaction of CO2 over basic catalysts significantly improves the diversity of products, vividly embodying the ability of green chemistry to turn waste into treasure. However, under a Lewis acidic CO2 atmosphere, the activity maintenance of the multi-step reaction puts forward higher requirements for the reversible regeneration ability of the basic catalysts. Novel Lewis–Brønsted binary basic poly(ionic liquid)s (LB-PILs) were successfully developed through a radical copolymerization followed by ion-exchange strategy, and were applied to the two-step synthesis of dimethyl carbonate (DMC) by coupling CO2 cycloaddition and CH3OH transesterification without any cocatalyst. Relying on the activation of CO2 by Lewis basic tertiary N and the thermal recovery of nucleophilic HCO3− to stronger Brønsted basic OH− with the help of temperature control in CH3OH transesterification, the LB-PILs presented high activity, stable repeatability and linear carbonate universality. In situ IR analysis and Knoevenagel condensation, combined with theoretical calculations, provided reliable support for the ingenious incorporation of reversible regeneration of basic catalysts in a Lewis acidic CO2 atmosphere and multi-step coupling reaction process of CO2.
研究领域:
化学工程
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绿色化学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xuewei Tu,Yutong Chen,Can Sun,Yang Hu,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Shijie Zhang,Hui Zheng
The utilization of CO 2 as an economical C1 feedstock for the production of valuable fine chemicals is widely recognized as a green and environmentally friendly approach. In this work, iron/cobalt oxide nanowires (FCO@NWs) composites were synthesized by a simple, convenient and cost-effective hydrothermal process. The FCO@NWs catalyst demonstrated efficient CO 2 fixation with o -phenylenediamine to produce benzimidazole at atmospheric pressure and 150 ℃. After 12 h reaction, the conversion rate of o -phenylenediamine reached an impressive 98%, indicating the catalyst's high efficiency in CO 2 fixation process. Through orthogonal experiments, the optimal reaction condition was confirmed and the application of the FCO@NWs catalyst for various o -phenylenediamine derivatives by substrate expansion was screened. Notably, this catalyst exhibited easy recoverability and reusability without significant loss in catalytic activity even after five cycles of experimentation. This study presents a promising approach for fixing CO 2 into valuable benzimidazole derivatives and contributes some experience to sustainable chemistry.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
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2024
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IF 3.9
Na Wei,Lin Liu,Jia-Qi Chu,Ting Fang,Zheng-Bo Han,Zhen Zhao
Metal-organic frameworks (MOFs) are widely studied for cycloaddition of CO 2 as a heterogeneous catalyst, because of their potential Lewis acidic sites and adjustable porous structure. However, most of them exhibit good catalytic performance need the assistance of nucleophilic co-catalysts. Herein, a novel MOFs and porous organic polymers (POPs) hybrid catalyst, core-shell ZIF-67@PDB-Br, is constructed by a convenient synthetic strategy, which possesses abundant Lewis acidic sites, imidazole cations and nucleophilic centers and shows robust chemical and thermal stability. This material demonstrates high-efficient catalytic activities and recyclability in the cycloaddition of CO 2 and propylene oxide without co-catalysts, the conversion and selectivity can reach 94.1 % and 99.0 %, respectively (100 °C, 1.0 MPa CO 2 pressure). Furthermore, the effects of the temperature, pressure, amount of catalyst and thickness of POPs shell on the catalytic activity were investigated. This study provides a viable direction for the development of synergistic heterogeneous catalysts for fixation of CO 2 without co-catalysts.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Polymer Chemistry
·
2011
·Vol. 2
·期 10
·2306-2315
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IF 0
Yubing Xiong,Yujiao Wang,Hong Wang,Rongmin Wang
Highly cross-linked polymeric nanoparticles (CLPNs) were prepared via a facile one-step synthesis, and these nanoparticles are effective catalysts for CO2 cycloaddition with epoxides. In this study, CLPNs were synthesized by radical copolymerization of 4-vinylbenzyl-tributylphosphorous chloride (PIL) and ethylene glycol dimethacrylate (EGDMA) in selective solvent, such as C1∼C5 alcohols. The results revealed that spherical nanoparticles with the mean diameter range of 10–100 nm could be prepared in these alcohols, and the size of the CLPNs could be facilely tuned by the feed ratio of EGDMA to PIL. The CLPNs were characterized using dynamic light scattering, scanning electron microscopy, transmission electron microscopy, atomic force microscopy, thermogravimetric analysis, atom absorbance spectrometry, and Fourier transform infrared spectroscopy techniques. In addition, CLPNs can be exploited as highly active and selective catalyst for the cycloaddition of CO2 to epoxides. The effects of parameters, such as reaction temperature, pressure, reaction time, and catalyst amount, on the cycloaddition reaction were investigated. As a result, excellent yield (100%) and selectivity (100%) of cyclic carbonates could be achieved under mild conditions (0.1 g CLPNs, 3.0 MPa CO2, 140 °C and 3 h) without the addition of any solvents or co-catalysts. Unexpectedly, the CLPNs could be dispersed in the products homogeneously, which resulted in the extremely high activity and selectivity. At the same time, the CLPNs could be easily separated by filtration after pouring the reaction mixture into toluene. CLPNs could be recycled six times with less than 1.5% loss of catalytic activity.
研究领域:
化学工程
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
JOURNAL OF POROUS MATERIALS
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2022
·Vol. 30
·期 3
·889-897
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IF 2.523
Hu Lihua,Chen Li,Mo Xiaohong,Peng Xiong,Xu Wei,Liu Feng,Yan Zongcheng
For the effective utilization of carbon resources, a facile and recyclable heterogeneous catalyst system with high reactivity and stability is urgently needed for chemical fixation of CO 2 . Herein, a micro/nanostructured ZIF-8/CeO 2 composite was designed by direct surface-nucleated ZIF-8 nanoparticles on spindle-like CeO 2 . The ZIF-8 nanoparticles content of the ZIF-8/CeO 2 composite could be tuned by the changing of reaction parameters, such as the molar ratio of reactants and the reaction time. The ZIF-8/CeO 2 composite exhibits remarkably enhanced catalytic activity and superior reusability for cycloaddition reaction of CO 2 and epoxide than its pure substance. The enhanced performance of ZIF-8/CeO 2 composite should be attributed to its high specific surface area and abundant porosity, outstanding thermal stability, and the appearance of a new moderate acid/base site in composite material. Considering the convenient preparation, enhanced catalytic activity and excellent reusability of ZIF-8/CeO 2 composite, this work offers a new strategy to replace ZIFs-based porous catalysts for chemical fixation of CO 2 .
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
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2021
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IF 4.527
Jie Min,Wei Song,Tianding Hu,Yunfei Zhi,Zhenhao Xia,Tiecheng Zhang,Shaoyun Shan,Hongying Su
Magnetic nanoparticle-supported heterogeneous catalysts have been widely researched in green catalysis, due to their convenient magnetic separation and nanometer effects. Herein, a magnetic Co(III)-Salen heterogeneous catalyst with uniform spherical core-shell structure was synthesized for the chemical fixation of CO 2 into cyclic carbonate based on the sustainable protocol development and green chemistry principles. Fe 3 O 4 @SiO 2 nanoparticles with uniform spherical core-shell structure were prepared by the reverse microemulsion method, and Co(III)-Salen complexes were subsequently immobilized on the resulted Fe 3 O 4 @SiO 2 nanoparticles via covalent bonding, leading to Fe 3 O 4 @SiO 2 @Co(III)-Salen nanocomposites with particle size of 29 nm and saturation magnetization value of 27.2 emu/g. The catalytic performance study indicated that the catalyst exhibited high yield of 99% with selectivity of 100% for the ring-opening addition reaction of CO 2 and epoxide under solvent-free reaction condition. A plausible reaction mechanism was proposed that the Lewis acidic sites of Co(III)-Salen and nucleophilic bromine ion components played synergetic roles in promoting cycloaddition reactions. A stable geometry of the Co(III)-Salen complex and a detailed evidence for the reaction mechanism were provided by the density functional theory (DFT) calculations. Based on their excellent magnetic properties , the Co(III)-Salen nanocomposites could be easily recovered by using an external magnet and reused for 5 times without significant leaching of metal center and loss of catalytic activity.
研究领域:
材料科学
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绿色化学
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催化反应
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 16
·6406-6416
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IF 5.287
Mengshuai Liu,Kunqi Gao,Lin Liang,Jianmin Sun,Li Sheng,Masahiko Arai
The combination of a metal-modified SBA-15 catalyst with potassium iodide was developed as heterogeneous dual catalysts for chemical fixation of CO2 to cyclic carbonates. It was observed that the binary Zn-SBA-15/KI catalysts were the most efficient among various metal-modified SBA-15/KI catalysts and showed an excellent synergetic effect in promoting the reaction under mild conditions. Moreover, the effects of reaction parameters on cycloaddition of CO2 with propylene oxide (PO) to propylene carbonate (PC) were optimized. Under the optimal conditions determined, the Zn-SBA-15/KI catalytic system was also versatile in CO2 cycloaddition with other epoxides. Additionally, the mechanistic details for the fixation of CO2 into a cyclic carbonate catalyzed by SBA-15/KI and Zn-SBA-15/KI were also contrastively elucidated using the density functional theory (DFT) method. The DFT results suggested that the zinc-modified and unmodified catalysts showed different coupling modes of CO2, and the ring-opening reaction was the rate-determining step in the SBA-15/KI catalyzed cycloaddition reaction, but the zinc-modified SBA-15/KI catalysts could enhance the CO2 cycloaddition, as the formation of a stable complex was beneficial to CO2 trapping. As a result, the ring-closing reaction became the rate-determining step in the Zn-SBA-15/KI catalyzed cycloaddition reaction, which was a promising result to guide the catalyst design for CO2 conversion.
研究领域:
催化化学
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环境科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）