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Highly Active AuCu-Based Catalysts for Acetylene Hydrochlorination Prepared Using Organic Aqua Regia.

ABSTRACT: Development of a sustainable process for designing and synthesising an active and stable catalyst for hydrochlorination of acetylene is challenging, yet crucial, for industrial vinyl chloride monomer (VCM) production. Herein, direct synthesis of bimetallic AuCu catalysts using organic aqua regia (OAR) preparation methods was investigated. In comparison with conventional aqua regia (AR), bimetallic AuCu catalysts synthesised from OAR exhibit enhanced activity and stability. After careful characterisation of the catalyst samples using X-ray diffraction patterns (XRD), Scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy (XPS), and Temperature-programmed desorption (TPD), this observation was justified for the following reasons: 1) the existence of sulphur and nitrogen atoms stabilised the cationic Au active sites, and 2) OAR helped to sustain the function of the Cu promotor by stabilising it. Advanced understanding on the importance of promoter stability has unveiled new perspectives for this research area.

SUBMITTER: He H

PROVIDER: S-EPMC6515409 | biostudies-literature | 2019 Apr

REPOSITORIES: biostudies-literature

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Highly Active AuCu-Based Catalysts for Acetylene Hydrochlorination Prepared Using Organic Aqua Regia.

He Haihua H Zhao Jia J Wang Bolin B Yue Yuxue Y Sheng Gangfeng G Wang Qingtao Q Yu Lu L Hu Zhong-Ting ZT Li Xiaonian X

Materials (Basel, Switzerland) 20190422 8

Development of a sustainable process for designing and synthesising an active and stable catalyst for hydrochlorination of acetylene is challenging, yet crucial, for industrial vinyl chloride monomer (VCM) production. Herein, direct synthesis of bimetallic AuCu catalysts using organic aqua regia (OAR) preparation methods was investigated. In comparison with conventional aqua regia (AR), bimetallic AuCu catalysts synthesised from OAR exhibit enhanced activity and stability. After careful characte ...[more]

PMID: 31013614

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Project description:In this paper, the ultrasonic-assisted desilication technique was reported as an attractive and efficient way for the preparation of hierarchical zeolites with MFI structure type. The prepared materials were used as active catalysts for the dehydration of ethanol into diethyl ether and ethylene. For all catalysts, the selectivity to diethyl ether was ca 95% or higher up to 210 °C, with catalytic activity in the range of 40-68%. In case of desilicated zeolites, at 270-290 °C, the conversion of ethanol was full with selectivity to ethylene ca 80%. MFI-type commercial zeolite was treated with a sodium and/or tetrabutylammonium hydroxide aqueous solutions (NaOH or NaOH/TBAOH) for 30 min. In the case of the application of ultrasounds, a QSonica Q700 sonicator (60 W and 20 kHz) equipped with a "1" diameter horn was used. In all cases, desilication was performed in an ice bath in order to keep the procedure conditions at low temperature. It was indicated that the use of ultrasounds during desilication procedure caused higher extraction of silicon and aluminum, which was connected with an elevated mesoporosity in relation to the samples modified in the absence of ultrasounds. Ultrasonic-assisted treatment of MFI-type zeolite caused also an apparent formation of numerous holes inside zeolite grains, resembling the look of "swiss cheese". Furthermore, it was indicated that the samples prepared using ultrasonic irradiation exhibited enhanced catalytic properties in the dehydration of ethanol. For instance, MFI-type zeolite treated with NaOH/TBAOH alkaline mixture containing 10 mol% of TBAOH in the presence of ultrasounds (M-10 s) demonstrated higher both conversion of ethanol (59% vs. 47%) and selectivity to diethyl ether (95% vs. 93%) in comparison with zeolite modified conventionally (M-10c). The best catalyst was zeolite ultrasonically desilicated with NaOH/TBAOH solution of 70 mol% of TBAOH (M-70s). Generally, this catalyst indicated the highest conversion of ethanol, very high selectivity to diethyl ether (94-100%) at 150-210 °C and the highest selectivity to ethylene among investigated catalysts (21%, 66% and 84%) at 230 °C, 250 oC and 270 °C.

Dataset Information

Highly Active AuCu-Based Catalysts for Acetylene Hydrochlorination Prepared Using Organic Aqua Regia.

Publications

Highly Active AuCu-Based Catalysts for Acetylene Hydrochlorination Prepared Using Organic Aqua Regia.

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