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Ni/SBA-15 catalysts for CO methanation: effects of V, Ce, and Zr promoters

机译:用于甲烷化甲烷的Ni / SBA-15催化剂:V,Ce和Zr助催化剂的作用

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摘要

Ni/SBA-15 catalysts with various promoters (V, Ce, and Zr) were prepared by an ultrasonic coimpregnation method and used in CO methanation. The addition of promoters played a significant role in improving the catalytic activity of the Ni/SBA-15 catalyst. This improvement could be explained by changes in the valences of the V and Ce promoter species through an oxidation-reduction shift cycle process (Mx+ <-> My+, M = V, Ce), which could trigger electron transfer. This transfer enhanced the electron density of active Ni species and promoted CO dissociation. The Zr promoter could produce oxygen vacancies during calcination and reduction, thereby increasing the ability of CO to adsorb and dissociate. In addition, the formation of a Si-O-M bond (M = Zr, Ce, V) increased the interaction between the active species and support, which facilitated CO methanation. Under 1.0 MPa and a WHSV of 15 000 mL g(-1) h(-1), 10Ni-5V/SBA-15 exhibited the best catalytic performance (99.9% CO conversion; 95.5% CH4 selectivity).
机译:通过超声共浸渍法制备了具有多种促进剂(V,Ce和Zr)的Ni / SBA-15催化剂,并将其用于CO甲烷化。助催化剂的添加在改善Ni / SBA-15催化剂的催化活性中起着重要作用。可以通过氧化还原移位循环过程(Mx +-My +,M = V,Ce)改变V和Ce启动子的化合价来解释这种改善,这可以触发电子转移。这种转移提高了活性镍物质的电子密度并促进了CO的离解。 Zr促进剂可在煅烧和还原过程中产生氧空位,从而增加CO吸附和离解的能力。此外,Si-O-M键(M = Zr,Ce,V)的形成增加了活性物质与载体之间的相互作用,从而促进了CO甲烷化。在1.0 MPa和15,000 mL g(-1)h(-1)的WHSV下,10Ni-5V / SBA-15表现出最佳的催化性能(99.9%的CO转化率; 95.5%的CH4选择性)。

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