In this study, the novel tin-based catalysts (Sn(II)/PN@AC) were prepared using the phosphorus and nitrogen dual-modified activated carbon as support and SnCl as active compounds, as well as then evaluated in acetylene hydrochlorination. Under the reaction temperature of 180 °C and an acetylene gas hourly space velocity (GHSV-CH) of 30 h, the 15%Sn(II)/PN@AC-550 showed the initial acetylene conversion of 100% and vinyl chloride selectivity over 98.5%. Additionally, the deactivation rate of 15%Sn(II)/PN@AC-550 reached 0.47% h, which was lower than that of 15%Sn(II)/AC-550 (1.02% h), suggesting that PN@AC-550 as novel support can retarded the deactivation of Sn(II)/AC-550 catalysts during acetylene hydrochlorination. Based on the catalytic tests and characterization results (XRD, Raman, BET surface area, TEM, CH-TPD, H-TPR, XPS, FT-IR, TGA, and ICP), it demonstrated that PN@AC-550 as support could effectively improve the dispersion of tin species, retard the formation of coke deposition, lessen the oxidation of SnCl during the preparation process, as well as relatively inhibit the leach of tin species during the reaction. By combing the FTIR results and Rideal-Eley mechanism, we proposed that that HSnCl was transition state of SnCl in catalysis acetylene hydrochlorination and then adsorbed the acetylene to produce the vinyl chloride.
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http://dx.doi.org/10.3906/kim-2103-9 | DOI Listing |
ACS Catal
September 2024
Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, Zürich 8093, Switzerland.
Platinum single atoms anchored onto activated carbon enable highly stable Hg-free synthesis of vinyl chloride (VCM) via acetylene hydrochlorination. Compared to gold-based alternatives, platinum catalysts are in initial phases of development. Most synthetic approaches rely on chloroplatinic acid, presenting opportunities to explore other precursors and their impact on catalyst structure, reactivity, and toxicity aspects.
View Article and Find Full Text PDFJ Am Chem Soc
October 2024
State Key Laboratory of Solidification Processing and School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an 710072, P. R. China.
ACS Nano
July 2024
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
Nat Commun
July 2024
School of Environmental Science and Engineering, Shanghai Jiao Tong University, 200240, Shanghai, China.
Ru single-atom catalysts have great potential to replace toxic mercuric chloride in acetylene hydrochlorination. However, long-term catalytic stability remains a grand challenge due to the aggregation of Ru atoms caused by over-chlorination. Herein, we synthesize an asymmetric Ru-In atomic pair with vinyl chloride monomer yield (>99.
View Article and Find Full Text PDFOrg Biomol Chem
May 2024
College of Chemistry, Zhengzhou University, Zhengzhou, Henan, China.
Markovnikov hydrobromination and hydrochlorination of alkynes were achieved using TMSX (X = Br, Cl) instead of corrosive HX (X = Br, Cl) as the bromination and chlorination reagents. Mn(OAc)·4HO was used as the hydrobromination catalyst for electron-neutral/rich alkynes. For the hydrobromination of electron-deficient alkynes and hydrochlorination of alkynes, Zn(OAc)·2HO was employed as the catalyst.
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