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Selective hydrogenation of CO2 to CH4 over two-dimensional nickel silicate molecular sieves

机译:在二维镍硅酸盐分子筛上将CO2的选择性氢化为CH4

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Two-dimensional (2D) Ni-containing delaminated MWW layers (Ni-DML) were synthesized by hydrothermal treatment of a borosilicate MWW precursor with a nickel nitrate solution, and their catalytic properties were investigated for the selective hydrogenation of CO2. Increasing the hydrothermal temperature promoted the structural transformation of 3D tectosilicate into 2D phyllosilicate. The isomorphic substitution of the framework boron by nickel was facilitated by increasing the hydrothermal temperature, and the content of Ni on Ni-DML was increased up to 38 wt% at 180 °C with high dispersion. The framework Ni in Ni-DML formed metallic Ni clusters in situ, which were active for the selective hydrogenation of CO2 to CH4. However, a significant reduction in the number of micropores was observed at hydrothermal temperatures above 160 °C because of the transformation of the delaminated MWW layers to 2D nickel phyllosilicates. A volcano-shaped distribution in the CH4 yield was observed with respect to the hydrothermal temperature.
机译:通过用硝酸镍溶液对硼硅酸盐MWW前体进行热液处理,研究了二维(2D)含Ni的分层MWW层(Ni-DML),并研究了其催化性能以进行CO2的选择性氢化。升高水温促进了3D构硅酸盐到2D phyllosilicate的结构转化。通过升高热温度来促进镍硼的同构替代,Ni-DML上的Ni含量在180°C下增加到38 wt%,并具有高分散体。 Ni-DML中的框架Ni原位形成了金属Ni簇,这些金属簇对CO2的选择性氢化为活性。然而,由于分层MWW层转化为2D镍纤维硅酸盐,在高于160°C的热液温度下观察到微孔的数量显着减少。相对于热液温度,观察到CH4产量中的火山形分布。

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