College of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, China.
Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300071, China.
Sci Rep. 2017 Jan 4;7:39789. doi: 10.1038/srep39789.
Acetylene hydrochlorination is a major industrial technology for manufacturing vinyl chloride monomer in regions with abundant coal resources; however, it is plagued by the use of mercury(II) chloride catalyst. The development of a nonmercury catalyst has been extensively explored. Herein, we report a N-doped carbon catalyst derived from ZIF-8 with both high activity and quite good stability. The acetylene conversion reached 92% and decreased slightly during a 200 h test at 220 °C and atmospheric pressure. Experimental studies and theoretical calculations indicate that C atoms adjacent to the pyridinic N are the active sites, and coke deposition covering pyridinic N is the main reason for catalyst deactivation. The performance of those N-doped carbons makes it possible for practical applications with further effort. Furthermore, the result also provides guidance for designing metal-free catalysts for similar reactions.
乙炔氯化是在煤炭资源丰富的地区生产氯乙烯单体的主要工业技术,但它受到汞(II) 氯化物催化剂的困扰。因此,人们广泛探索开发非汞催化剂。本文报道了一种由 ZIF-8 衍生的具有高活性和良好稳定性的 N 掺杂碳催化剂。在 220°C 和常压下进行 200 小时测试时,乙炔转化率达到 92%,且略有下降。实验研究和理论计算表明,吡啶氮相邻的 C 原子是活性位,覆盖吡啶氮的积碳是催化剂失活的主要原因。通过进一步的努力,这些 N 掺杂碳的性能使其有可能应用于实际应用。此外,该结果还为设计类似反应的无金属催化剂提供了指导。