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Nickel phyllosilicate derived Ni/SiO2 catalysts for CO2 methanation: Identifying effect of silanol group concentration
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-05-28 , DOI: 10.1016/j.jcou.2021.101587
Yang Zhang , Qing Liu

For the conventional Ni/SiO2 catalyst, the weak metal-support interaction usually resulted in serious Ni sintering at high temperature. To address this problem, a group of Ni-phyllosilicate-derived Ni/SiO2 catalysts were synthesized via the hydrothermal reaction of nickel nitrate and mesostructured silica nanoparticles (MSN) with three different sizes of 99 (MS), 184 (MM), and 725 (ML) nm. The Ni contents of three nickel phyllosilicate catalysts varied from 5.9 to 19.7 wt%, which exhibited a reverse order of the particle size. It was found that the concentration of silanol group (triple bondSiOsingle bondH) of MSN significantly affected the construction of Ni-phyllosilicate material. The surface silanol group concentration increased with the decrease of particle size of MSN, resulting in the improved formation of nickel phyllosilicate and enhanced catalytic activity for CO2 methanation. Among all catalysts, MS/H-24 showed the highest CO2 conversion of 76.5 % at 450 °C due to the highest Ni dispersion and largest CO2 and H2 uptakes. In addition, the optimal catalyst exhibited higher anti-sintering property, long-term stability and hydrothermal stability than an impregnated catalyst (Ms/Im) with the similar Ni content in a lifetime test (450 °C, 100 h) and steam treatment test (600 °C, 6 h), owing to its strong metal-support interaction derived from nickel phyllosilicate.



中文翻译:

用于CO 2甲烷化的页硅酸镍衍生的Ni/SiO 2催化剂:识别硅烷醇基团浓度的影响

对于传统的Ni/SiO 2催化剂,弱金属-载体相互作用通常会导致Ni在高温下严重烧结。为了解决这个问题,通过硝酸镍和介孔结构二氧化硅纳米粒子(MSN)的水热反应合成了一组Ni-页硅酸盐衍生的Ni/SiO 2催化剂,具有三种不同尺寸的99(M S),184(M M) ,和725(M大号)纳米。三种层状硅酸镍催化剂的 Ni 含量从 5.9 到 19.7 wt% 不等,表现出相反的粒度顺序。发现硅烷醇基团(SiO三键单键H) MSN显着影响Ni-页硅酸盐材料的构建。表面硅烷醇基团浓度随着MSN粒径的减小而增加,导致页硅酸镍形成的改善和对CO 2甲烷化的催化活性增强。在所有催化剂中,M S /H-24在 450 °C 时表现出最高的 CO 2转化率,达到 76.5 %,这是因为 Ni 分散度最高,CO 2和 H 2最大吸收。此外,在寿命试验(450℃,100h)和蒸汽处理试验中,最佳催化剂比具有相似Ni含量的浸渍催化剂(Ms/Im)表现出更高的抗烧结性能、长期稳定性和水热稳定性(600 °C, 6 h),由于其来自页硅酸镍的强金属-载体相互作用。

更新日期:2021-05-28
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