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Enhancement of catalytic activity in CO2 methanation in Ni-based catalysts supported on delaminated ITQ-6 zeolite
Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-06-15 , DOI: 10.1016/j.jcat.2024.115609
R.B. Machado-Silva , J.F. Da Costa-Serra , A. Chica

Ni-based catalysts supported on delaminated ITQ-6 zeolite with different Si/Al ratios, 30 and ∞, were tested in the methanation of CO and CO. ITQ-6 supports exhibited high surface areas (> 590 m/g), and the catalysts based on them presented elevated CO and CO conversion values, turnover frequencies (TOF), and CH selectivity (> 90 %). Comparing the ITQ-6 catalyst and its precursor ferrierite (FER)-based catalyst, H-chemisorption results confirmed higher metallic dispersion for the former, which resulted in improved H uptake and efficient interaction of reaction intermediates via the associative pathway. Combined kinetic studies indicated that their higher available metallic surface contributed to lower apparent activation energies towards CH formation, accounting for the higher selectivity values. A 15 wt% Ni-based catalyst supported on ITQ-6 zeolite (Si/Al = 30) exhibited catalytic results (X = 79 % y S = 98 %) comparable or even superior to some of the best zeolite-based catalysts reported so far.

中文翻译:


分层 ITQ-6 沸石负载镍基催化剂提高 CO2 甲烷化催化活性



在 CO 和 CO 的甲烷化中测试了负载在具有不同 Si/Al 比(30 和 ∞)的分层 ITQ-6 沸石上的镍基催化剂。ITQ-6 载体表现出高表面积(> 590 m/g),并且基于它们的催化剂具有较高的 CO 和 CO 转化值、周转频率 (TOF) 和 CH 选择性 (> 90%)。比较 ITQ-6 催化剂及其前体镁碱沸石 (FER) 基催化剂,H 化学吸附结果证实前者具有更高的金属分散性,从而提高了 H 吸收并通过缔合途径实现反应中间体的有效相互作用。综合动力学研究表明,它们较高的可用金属表面有助于降低 CH 形成的表观活化能,从而导致较高的选择性值。负载在 ITQ-6 沸石 (Si/Al = 30) 上的 15 wt% 镍基催化剂表现出的催化结果 (X = 79% y S = 98%) 与报道的一些最好的沸石基催化剂相当甚至更好远的。
更新日期:2024-06-15
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