High-performance Ni-foam-structured Nb2O5-NiO nanocomposite catalyst for oxidative dehydrogenation of shale gas ethane to ethylene: Effects of Nb2O5 loading and calcination temperature
High-performance Ni-foam-structured Nb2O5-NiO nanocomposite catalyst for oxidative dehydrogenation of shale gas ethane to ethylene: Effects of Nb2O5 loading and calcination temperature
复制标题
高性能泡沫镍结构Nb2O5-NiO纳米复合催化剂用于页岩气乙烷氧化脱氢制乙烯：Nb2O5负载量和焙烧温度的影响
DOI：
10.1016/j.micromeso.2019.109609
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发表时间：
2019
影响因子：
5.2
通讯作者：
Lu Yong
中科院分区：
文献类型：
--
作者：
Zhang Zhiqiang;Zhao Guofeng;Liu Ye;Lu Yong
页岩气的大规模开采极大地丰富了乙烷资源，使得乙烷氧化脱氢制乙烯的工艺颇具吸引力，但合适的催化剂是一个巨大的挑战。研制了一系列泡沫镍结构的MOx-NiO （M = Li, Mg, Ga, Ce, Zr, Mo， W, Nb）复合氧化物催化剂（MOx-NiO/Ni-foam），用于乙烷氧化脱氢制乙烯（ODE）。采用水热法将nic2o4生长在泡沫镍（110 PPI）上，然后用含m盐水溶液浸渍和煅烧处理得到催化剂。其中Nb2O5-NiO /Ni-foam表现出较好的ODE催化性能。nb2o5的负载和煅烧温度对催化性能有显著影响。适量的nb2o5改性可显著消除非选择性氧，从而显著提高乙烯选择性。Nb2O5-NiO /Ni-foam催化剂的活性和选择性对煅烧温度也很敏感，煅烧温度可以在很大程度上调节其晶格氧的解吸性能。最有前途的Nb2O5-NiO /Ni-foam催化剂是用5 wt% nb2o5改性，450 °C煅烧，在410 °C， C2H6/O2/N2= 1/1/8 ，GHSV为9000 cm3g−1h−1（对应于0.423 gC2H4gcat−1h−1的高乙烯产率）下，能以68%的乙烯选择性转化60%的乙烷。
Large-scale shale gas exploitation greatly enriches ethane resources, making the oxidative dehydrogenation of ethane (ODE) to ethylene quite fascinating, but the qualified catalyst presents a grand challenge. A series of Ni-foam-structured MOx-NiO (M = Li, Mg, Ga, Ce, Zr, Mo, W, Nb) composite oxide catalysts (denoted as MOx-NiO/Ni-foam) have been developed for the oxidative dehydrogenation of ethane to ethylene (ODE). The catalysts were obtained by hydrothermal growth of NiC2O4onto a Ni-foam (110 PPI) and subsequent impregnation with an M-containing salt aqueous solution and calcination treatment. Among them, the Nb2O5–NiO/Ni-foam showed superior catalytic ODE performance over the others. Both Nb2O5loading and calcination temperature showed remarkable impact on the catalytic performance. The modification with suitable amount of Nb2O5was responsible for the significant elimination of non-selective oxygen species thereby leading to remarkable improvement of the ethylene selectivity. The activity and selectivity of the Nb2O5–NiO/Ni-foam catalysts are also sensitive to the calcination temperature that can modulate the desorption properties of their lattice oxygen species to a great extent. The most promising Nb2O5–NiO/Ni-foam catalyst is the one modified with 5 wt% Nb2O5and calcined at 450 °C, being capable of converting 60% ethane with a 68% ethylene selectivity for a feed of C2H6/O2/N2= 1/1/8 at 410 °C and GHSV of 9000 cm3g−1h−1(corresponding to a high ethylene productivity of 0.423 gC2H4gcat−1h−1).