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Synthesis of C4 Olefins from Acetylene over Supported Copper Catalysts
ChemCatChem ( IF 3.8 ) Pub Date : 2020-04-15 , DOI: 10.1002/cctc.202000396 Qingyuan Li 1 , Yuxin Wang 1 , Jianli Hu 1
ChemCatChem ( IF 3.8 ) Pub Date : 2020-04-15 , DOI: 10.1002/cctc.202000396 Qingyuan Li 1 , Yuxin Wang 1 , Jianli Hu 1
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Conversion of acetylene to C4 olefins enables on‐purpose synthesis of C4 olefins using abundant natural gas resource due to acetylene can be synthesized from methane or ethane. In this study, Cu‐based catalysts supported on SiO2, ZSM‐5 and mordenite (MOR) were tested for acetylene hydrodimerization. Effect of promoters including Ru, Ga, Ag and Pd on the acetylene conversion and C4 olefins selectivity are investigated. The structures of these catalysts were characterized by TEM, XRD, BET, H2‐TPR, NH3‐TPD and XPS measurements. Results showed that temperature, pressure and hydrogen partial pressure had positive effect on acetylene conversion. In the presence of Ru promotor, 100 % acetylene conversion and 87 % selectivity to C4 olefins were achieved over Cu/MOR catalyst under conditions of 0.1 MPa and 200 °C. The mechanistic aspect of acetylene hydrodimerization was elucidated where the C4 intermediate was formed by the reaction between [Cu]−C2H2 π‐complex and [Cu]−C2H2 σ‐complex which were transformed to 1,3‐butadiene and butene.
中文翻译：
负载型铜催化剂上由乙炔合成C4烯烃
乙炔可转化为C 4烯烃，可利用丰富的天然气资源按需合成C 4烯烃，因为乙炔可从甲烷或乙烷中合成。在这项研究中，对负载在SiO 2，ZSM-5和丝光沸石（MOR）上的Cu基催化剂进行了乙炔加氢二聚化测试。研究了Ru，Ga，Ag和Pd等促进剂对乙炔转化率和C 4烯烃选择性的影响。通过TEM，XRD，BET，H 2 -TPR，NH 3表征了这些催化剂的结构。TPD和XPS测量。结果表明，温度，压力和氢分压对乙炔转化率有积极影响。在Ru促进剂的存在下，在0.1MPa和200℃的条件下，在Cu / MOR催化剂上实现了100％的乙炔转化率和87％的对C 4烯烃的选择性。乙炔hydrodimerization的机械方面是阐明当C 4中间体通过之间的反应形成[铜] -C 2 ħ 2 π络合物和物[Cu] -C 2 ħ 2 σ络合物，其被转化为1,3-丁二烯和丁烯。
更新日期：2020-06-18
中文翻译：
负载型铜催化剂上由乙炔合成C4烯烃
乙炔可转化为C 4烯烃，可利用丰富的天然气资源按需合成C 4烯烃，因为乙炔可从甲烷或乙烷中合成。在这项研究中，对负载在SiO 2，ZSM-5和丝光沸石（MOR）上的Cu基催化剂进行了乙炔加氢二聚化测试。研究了Ru，Ga，Ag和Pd等促进剂对乙炔转化率和C 4烯烃选择性的影响。通过TEM，XRD，BET，H 2 -TPR，NH 3表征了这些催化剂的结构。TPD和XPS测量。结果表明，温度，压力和氢分压对乙炔转化率有积极影响。在Ru促进剂的存在下，在0.1MPa和200℃的条件下，在Cu / MOR催化剂上实现了100％的乙炔转化率和87％的对C 4烯烃的选择性。乙炔hydrodimerization的机械方面是阐明当C 4中间体通过之间的反应形成[铜] -C 2 ħ 2 π络合物和物[Cu] -C 2 ħ 2 σ络合物，其被转化为1,3-丁二烯和丁烯。
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