title: Silicon carbide-derived carbon nanocomposite as a substitute for mercury in the catalytic hydrochlorination of acetylene.
abstract: Acetylene hydrochlorination is an important coal-based technology for the industrial production of vinyl chloride, however it is plagued by the toxicity of the mercury chloride catalyst. Therefore extensive efforts have been made to explore alternative catalysts with various metals. Here we report that a nanocomposite of nitrogen-doped carbon derived from silicon carbide activates acetylene directly for hydrochlorination in the absence of additional metal species. The catalyst delivers stable performance during a 150 hour test with acetylene conversion reaching 80% and vinyl chloride selectivity over 98% at 200 °C. Experimental studies and theoretical simulations reveal that the carbon atoms bonded with pyrrolic nitrogen atoms are the active sites. This proof-of-concept study demonstrates that such a nanocomposite is a potential substitute for mercury while further work is still necessary to bring this to the industrial stage. Furthermore, the finding also provides guidance for design of carbon-based catalysts for activation of other alkynes.
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Xingyun
authors.initials: X
authors.lastname: Li
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Xiulian
authors.initials: X
authors.lastname: Pan
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Liang
authors.initials: L
authors.lastname: Yu
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Pengju
authors.initials: P
authors.lastname: Ren
authors.affiliation: Department of Electronic Science & Engineering, SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, Southeast University, Nanjing 210096, China.
authors.forename: Xing
authors.initials: X
authors.lastname: Wu
authors.affiliation: Department of Electronic Science & Engineering, SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, Southeast University, Nanjing 210096, China.
authors.forename: Litao
authors.initials: L
authors.lastname: Sun
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Feng
authors.initials: F
authors.lastname: Jiao
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China.
authors.forename: Xinhe
authors.initials: X
authors.lastname: Bao