Uniform Ni particles on amino-functionalized SBA-16 with excellent activity and stability for syngas methanation

Uniform Ni particles on amino-functionalized SBA-16 with excellent activity and stability for syngas methanation
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氨基官能化 SBA-16 上的均匀镍颗粒具有优异的合成气甲烷化活性和稳定性

DOI:
10.1016/j.molcata.2016.03.028
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发表时间:
2016-06
期刊:
Journal of Molecular Catalysis A: Chemical
影响因子:
--
通讯作者:
Zhong Xin
Zhong Xin
中科院分区:
其他
文献类型:
--
作者:
Zhicheng Bian;Xin Meng;Miao Tao;YuHao Lv;Zhong Xin

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采用硅烷偶联剂对介孔材料SBA-16进行改性,制备了负载镍的新型功能化SBA-16催化剂。在连续流动固定床反应器上系统考察了该催化剂在CO甲烷化反应中的性能。采用N_2吸附-脱附、X-射线衍射仪、透射电子显微镜、FT-IR、~(29)Si-核磁共振、H_2程序升温还原和H_2脉冲化学吸附等手段对催化剂进行了表征。经氨丙基三甲氧基硅烷(APTMS)修饰后,载体SBA-16的内表面硅醇基被氨基取代。氨基取代羟基可防止金属离子在溶液中团聚。此外,由于SBA-16上取代的有机基团可以与金属形成均一的相互作用,因此镍颗粒大小均匀。与未功能化的催化剂相比,Ni/SBA-16-NH_2催化剂在CO甲烷化反应中表现出更高的活性、更好的耐热性能和更好的稳定性。在最佳反应温度下,CO转化率可达100%,CH4选择性可达99.9%。同时,在100小时的寿命试验中,催化剂的活性没有下降。
Via modification of mesoporous material SBA-16 with silane coupling agent, a new functionalized SBA-16 catalyst immobilized Ni has been prepared. The performance of the catalyst for CO methanation then were systemically investigated in a continuous flow fixed-bed reactor. The as-synthesized catalyst was characterized with N2absorption-desorption, X-ray diffraction, Transmission electron microscopy (TEM), FT-IR spectrum,29Si-nuclear magnetic resonance (NMR), H2—Temperature Programmed Reduction (TPR) and H2pulse chemisorption. After modification by aminopropyl-trimethoxysilane (APTMS), the internal surface silanol group of support SBA-16 was replaced by amino-groups. The replacement of hydroxyl groups by amino groups could prevent the agglomeration of metal ion in the solution. Also uniform nickel particle size was observed because the replaced organic groups on SBA-16 could form homogeneous interaction towards the metal. Comparing with the catalyst without functionalized, the catalyst Ni/SBA-16-NH2exhibited higher activity, excellent heat-resistant performance and better stability in CO methanation. The CO conversion and CH4selectivity could be 100% and 99.9% at the optimal temperature. Meanwhile, the catalyst showed no decrease of activity in the 100 h life test.
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