CATALYSIS LETTERS
·
2024
·Vol. 155
·期 1
·1-17
·
IF 2.3
Wei Ruiping,Wang Ziqi,Yao Mingzhu,Xia Rongying,Liu Huijun,Yang Lei,Ma Guanghui,Gao Lijing,Xiao Guomin
The metal-organic frameworks (MOFs) with oxidative and acidic active sites demonstrate promising potential for tandem reactions involving olefin oxidation carboxylation. In this study, M-BTCs were synthesized via a solvothermal method, employing 1,3,5-benzenetricarboxylic acid (H 3 BTC) as a ligand in combination with various metals (Mn, Co, Cu, Ni). The good thermal stability and morphology of M-BTC was verified by various characterization techniques, and its catalytic performance was evaluated for oxidative carboxylation. The catalytic activity of Mn-BTC, with Mn 3+ / Mn 2+ as the primary oxidation site, was found to be superior in both olefin epoxidation and CO 2 cycloaddition. The effects of reaction conditions on both epoxidation of styrene and the cycloaddition reaction were investigated, respectively. Under optimal reaction conditions (epoxidation: 10 wt% Mn-BTC of styrene, 80 ℃ for 12 h; cycloaddition: 100 ℃ for 12 h with a CO 2 flow rate of 15 ml/min and tetrabutylammonium bromide (TBAB) amount of 15 mol%), a 53% yield of styrene carbonate (SC) was obtained in the assisted tandem reactions. Furthermore, cycling experiments as well as XRD and FT-IR spectra of the catalysts after use demonstrated that Mn-BTC maintained its crystal structure and retained a yield of 49% SC after three cycles. Finally, a possible mechanism for assisted tandem catalytic reaction over Mn-BTC was proposed. Graphic
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2017
·
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
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Lu Long,Kaiji Xu,Kok Bing Tan,Dongren Cai,Yucheng Yang,Shu-Feng Zhou,Guowu Zhan
Catalytically agitating paddles are essential to perform liquid-solid heterogeneous catalytic reactions on an industrial scale due to the improved mass transfer and easy catalyst recovery. Herein, bimetallic oxides were formed after the calcination of nanomaterials derived from metal-organic frameworks (MOFs). Particularly, Mn(M)-BTC nanomaterials were synthesized by self-assembly of Mn 2+ ions (mixed with various dopants such as Cu 2+ , Ce 3+ , or Fe 2+ ) and H 3 BTC ligands in a mixed solvent of ethanol and water. It was found that in the powdery form, the Mn-Cu oxide derivate exhibited the highest degradation rate in the catalytic wet peroxide oxidation process (CWPO process), which was significantly higher than that of single metal oxide as well as Mn-Fe and Mn-Ce oxide derivates. The reason was caused by the synergistic effect between Mn-Cu promoted the formation of Mn 3+ and Cu + species to boost the CWPO reaction. Furthermore, the obtained Mn-Cu powdery catalysts were 3D-printed to obtain monolithic agitating paddles with different geometries, which were then mounted on a central shaft in the stirred reactor. An advanced oxidation process was used to investigate the effect of 3D patterns on the degradation efficiency of various organic dyes. It was discovered that the 3D-printed grid with higher cell density (484 cpsi) had better liquid mixing efficiency and thus better catalytic performance, which could be repeatedly used more than seven times. Additionally, the numerical simulation analysis (computational fluid dynamics) revealed a good mixing efficiency and improved mass transfer in the entire reactor equipped with the designed monolithic agitating impellers.
研究领域:
化学工程
·
材料科学
·
环境工程
·
催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）