Abstract
The Ru-based catalysts, including Ru/AC (activated carbon), TPAP (tetrapropylammonium perruthenate)/AC, TPAP/AC-HNO3, and TPAP/AC-HCl, were prepared and assessed for the direct synthesis of vinyl chloride monomer. The results indicate that the TPAP/AC-HCl catalyst exhibits the best performance with the conversion falling from 97% to 91% in 48 hours’ reaction under the conditions of 180 °C, a GHSV(C2H2) of 180 h−1, and the feed ratio VHCl/VC2H2 of 1.15. The substitution of RuCl3 precursor with high valent TPAP species leads to more ruthenium oxides active species in the catalysts; the acidification treatment of carrier in TPAP/AC catalyst can produce an enhanced interaction between the active species and the modified functional groups on the carrier, and it is beneficial to inhibit the carbon deposition and sintering of ruthenium species in the reaction process, greatly increase the adsorption ability of reactants, and further increase the amount of dominating active species in the catalysts, thus improving the catalytic performance. This also provides a promising strategy to explore high efficient and economic mercury-free catalysts for the hydrochlorination of acetylene.
Highlights
The addition reaction of acetylene with hydrogen chloride is an essential route for the direct synthesis of vinyl chloride monomer (VCM), the catalyst ever used in traditional industry is carbon-supported HgCl2, which posseses a serious environmental pollution and personnel hazard for its high toxicity and effumability
The results show that the pretreatment of activated carbon, especially the hydrochloric acid, may produce an interaction between the actives species and the carrier, which acidification modification by catalytic hydrochloric acid, mayof produce an interaction between actives speciesof significantly promotes the performance the prepared catalysts for thethe direct synthesis and the carrier, which significantly promotes the catalytic performance of the prepared catalysts for the direct synthesis of VCM
After the catalyst bed was heated to the reaction temperature under the atmospheric pressure, acetylene and hydrogen chloride were fed through the heated reactor, and the flow rates of the reactants were controlled via mass flow controllers to maintain a V HCl /V C2H2 of 1.15 and a gas hourly space velocity (GHSV)(C2 H2 ) of
Summary
The addition reaction of acetylene with hydrogen chloride is an essential route for the direct synthesis of vinyl chloride monomer (VCM), the catalyst ever used in traditional industry is carbon-supported HgCl2 , which posseses a serious environmental pollution and personnel hazard for its high toxicity and effumability. Whereafter, extensive researches on the Ru-based catalysts have been carried out, for example, Li et al came to a conclusion that Ru catalysts deposited inside carbon nanotubes exhibits better catalytic performance, with a 95.0% conversion and a 99.9% selectivity to VCM at 170 ◦ C, the feed ratio V HCl /V C2H2 of 1.10, and a C2 H2 gas hourly space velocity (GHSV) of 90 h−1 [10]. We prepared the Ru-based catalysts with the tetrapropylammonium perruthenate (TPAP) supported on AC, which was treated by a certain concentration of hydrochloric acid or nitric acid in this paper, and evaluated the catalytic performannce for the hydrochlorination of acetylene, intending to find out an prepared, higher activated, more stable and economic mercury-free catalyst. The effect of the supported ruthenium complexes catalysts on the catalytic behavior was explored in detail
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