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Keywords = acetylene acetoxylation

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11 pages, 2764 KiB  
Article
Preparation of High-Performance Zn-Based Catalysts Using Printing and Dyeing Wastewater and Petroleum Coke as a Carrier in Acetylene Acetoxylation
by Yuhao Chen, Mengli Li, Zhuang Xu, Guowang Shen, Xugeng Wang and Bin Dai
Catalysts 2023, 13(3), 539; https://doi.org/10.3390/catal13030539 - 8 Mar 2023
Cited by 1 | Viewed by 1747
Abstract
In this study, novel Zn catalysts were prepared by the wet impregnation method using printing and dyeing wastewater (PDW)-modified petroleum coke (petcoke) as a carrier, and they were applied to the acetylene acetoxylation. The pretreated petroleum coke has a high specific surface area [...] Read more.
In this study, novel Zn catalysts were prepared by the wet impregnation method using printing and dyeing wastewater (PDW)-modified petroleum coke (petcoke) as a carrier, and they were applied to the acetylene acetoxylation. The pretreated petroleum coke has a high specific surface area which provides sufficient space for the loading of Zn. Calcination further increases catalyst activity, but when calcination temperatures exceed 1000 °C, a significant loss of Zn occurs, resulting in a dramatic decrease in catalyst activity. This enables the conversion of acetic acid up to 85%. X-ray photoelectron spectroscopy confirmed that a large amount of N is introduced into PC from PDW, which changes the electron transfer around Zn. Temperature-programmed desorption (TPD) analysis revealed that the nitrogen-doped Zn(OAc)2 catalyst enhanced the catalytic activity by modulating the intensity of the catalyzed adsorption of acetic acid and acetylene. This study provides a new way to reuse petroleum coke and printing and dyeing wastewater to support the sustainable development of the vinyl acetate industry. Full article
(This article belongs to the Section Catalytic Materials)
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17 pages, 5702 KiB  
Article
Effect of Pyrolysis Conditions on the MOFs-Derived Zinc-Based Catalysts in Acetylene Acetoxylation
by Guowang Shen, Mengli Li, Yuhao Chen, Zhuang Xu, Xugen Wang and Bin Dai
Catalysts 2023, 13(3), 532; https://doi.org/10.3390/catal13030532 - 6 Mar 2023
Cited by 2 | Viewed by 2067
Abstract
The preparation method and calcination temperature of metal-organic framework (MOFs)-derived materials are critical factors affecting catalytic performance. In this work, the preparation conditions of MOFS precursors were optimized, and zinc-based catalysts with different activities (MOF5-700, MOF5-750, and MOF5-800) were obtained by pyrolysis of [...] Read more.
The preparation method and calcination temperature of metal-organic framework (MOFs)-derived materials are critical factors affecting catalytic performance. In this work, the preparation conditions of MOFS precursors were optimized, and zinc-based catalysts with different activities (MOF5-700, MOF5-750, and MOF5-800) were obtained by pyrolysis of MOFS precursors under nitrogen, which were then applied to an acetylene acetoxylation reaction system. According to the results, the conversion rate of acetic acid under catalysis was significantly different. (MOF5-700 (48%), MOF5-750 (62%), and MOF5-800 (22%)). Comparing the activity of the catalyst with the industrial catalyst Zn(OAc)2/AC (20%), MOF5-750 showed higher activity, and the acetic acid conversion rate remained around 60% after 50 h of stability testing. By characterization analysis, MOFs-derived materials were obtained after proper temperature pyrolysis. They have high mesoporous content, defects, and oxygen-containing functional groups and can maintain a good crystal structure, greatly reducing the loss of active components. This is the main reason for the good performance of the MOF5-750 catalyst in acetylene acetoxylation. Thus, the preparation conditions and favorable pyrolysis temperature of MOF derivative catalysts play a key role in the catalytic performance of acetylene acetoxylation. Full article
(This article belongs to the Section Catalytic Materials)
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11 pages, 2697 KiB  
Article
MOFs-Derived Zn-Based Catalysts in Acetylene Acetoxylation
by Mengli Li, Zhuang Xu, Yuhao Chen, Guowang Shen, Xugen Wang and Bin Dai
Nanomaterials 2022, 12(1), 98; https://doi.org/10.3390/nano12010098 - 29 Dec 2021
Cited by 17 | Viewed by 2852
Abstract
Metal–organic frameworks (MOFs)-derived materials with a large specific surface area and rich pore structures are favorable for catalytic performance. In this work, MOFs are successfully prepared. Through pyrolysis of MOFs under nitrogen gas, zinc-based catalysts with different active sites for acetylene acetoxylation are [...] Read more.
Metal–organic frameworks (MOFs)-derived materials with a large specific surface area and rich pore structures are favorable for catalytic performance. In this work, MOFs are successfully prepared. Through pyrolysis of MOFs under nitrogen gas, zinc-based catalysts with different active sites for acetylene acetoxylation are obtained. The influence of the oxygen atom, nitrogen atom, and coexistence of oxygen and nitrogen atoms on the structure and catalytic performance of MOFs-derived catalysts was investigated. According to the results, the catalysts with different catalytic activity are Zn-O-C (33%), Zn-O/N-C (27%), and Zn-N-C (12%). From the measurements of X-ray photoelectron spectroscopy (XPS), it can be confirmed that the formation of different active sites affects the electron cloud density of zinc. The electron cloud density of zinc affects the ability to attract CH3COOH, which makes catalysts different in terms of catalytic activity. Full article
(This article belongs to the Topic Synthesis and Applications of Nanostructured Metals and Metal Oxides)
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13 pages, 2544 KiB  
Article
Effect of Oxygen-Containing Group on the Catalytic Performance of Zn/C Catalyst for Acetylene Acetoxylation
by Fulong Zhu, Junqing Li, Mingyuan Zhu and Lihua Kang
Nanomaterials 2021, 11(5), 1174; https://doi.org/10.3390/nano11051174 - 29 Apr 2021
Cited by 12 | Viewed by 2349
Abstract
In this study, a series of activated carbon-based supports with different oxygen-containing groups (OCGs) proportions were obtained via thermal treatment in an ozone flow. Semiquantitative analyses indicated that the performance of the catalyst attained a maximum after 30 min of treatment with ozone [...] Read more.
In this study, a series of activated carbon-based supports with different oxygen-containing groups (OCGs) proportions were obtained via thermal treatment in an ozone flow. Semiquantitative analyses indicated that the performance of the catalyst attained a maximum after 30 min of treatment with ozone flow, and had a positive correlation with the content ratios of carboxyl and hydroxyl groups. Further, temperature-programmed desorption analysis demonstrated that the high performance (63% acetic acid conversion) of the prepared catalyst for the acetoxylation of acetylene could be ascribed to the reduced strength of increased capacity of acetylene adsorption. Density functional theory proved that the additional –COOH in the dicarboxylic catalytic system could be employed as a support for the active sites, and enhancing C2H2 adsorption strength in the rate-limiting step in the actual experimental process effectively accelerated the reaction rate. Thus, the OCGs on the surface of activated carbon play a crucial role in the catalytic performance of the acetylene acetoxylation catalyst. Full article
(This article belongs to the Special Issue Green Chemistry for Nanoparticle Synthesis)
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10 pages, 2305 KiB  
Article
A Novel High-Activity Zn-Co Catalyst for Acetylene Acetoxylation
by Peijie He, Liuhua Huang, Xueyi Wu, Zhuang Xu, Mingyuan Zhu, Xugen Wang and Bin Dai
Catalysts 2018, 8(6), 239; https://doi.org/10.3390/catal8060239 - 6 Jun 2018
Cited by 17 | Viewed by 4756
Abstract
In this paper, Zn(OAc)2/AC and Zn-Co/AC catalysts were prepared and applied in an acetylene acetoxylation reaction. Compared with monometallic Zn(OAc)2/AC catalyst, which is widely applied in industry, the Zn-Co catalysts exhibited excellent catalytic performance. Transmission electron microscopy results displayed [...] Read more.
In this paper, Zn(OAc)2/AC and Zn-Co/AC catalysts were prepared and applied in an acetylene acetoxylation reaction. Compared with monometallic Zn(OAc)2/AC catalyst, which is widely applied in industry, the Zn-Co catalysts exhibited excellent catalytic performance. Transmission electron microscopy results displayed that the addition of cobalt improved the dispersity of zinc acetate particles and inhibited catalyst sintering on the catalyst surface. X-ray photoelectron spectra suggested that the Co additive changed the electron density of zinc acetate probably because of the interaction between Zn and Co species. Temperature programmed desorption analysis demonstrated Co additive strengthened the adsorption of acetic acid and weakened the adsorption of acetylene. Full article
(This article belongs to the Special Issue Heterogeneous Acid Catalyst)
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