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CO2 hydrogenation to methanol over Cu/ZnO nanocatalysts prepared via a chitosan-assisted co-precipitation method

机译:壳聚糖辅助共沉淀法制备的Cu / ZnO纳米催化剂上CO2加氢制甲醇

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摘要

In this study, CuO-ZnO nanocomposites were prepared by chitosan-assisted co-precipitation method and performed as catalyst for CO2 hydrogenation to methanol. Effects of chitosan concentration on the physico-chemical properties of the nanocomposites as well as the catalytic activity have been investigated. The obtained catalysts were characterized by means of scanning electron microscopy, X-ray diffraction, N2 adsorption-desorption, N2O chemisorption and temperature-programmed reduction. Chitosan was found to act not only as a coordination compound to produce a homogeneous combination of CuO-ZnO nanocomposite, but also as a soft template for the formation of hollow nanospheres. The CuO and ZnO crystallite sizes of the hollow nanospheres were found to be 11.5 and 18.8 nm, respectively, which were smaller than those of other catalysts. The increase of chitosan concentration caused a change in catalyst morphology and a reduction in BET surface area as well as metallic copper surface area, but still higher than those of the unmodified catalyst. The catalysts prepared by using chitosan as precipitating agent exhibited a higher space time yield of methanol than the unmodified catalyst, which was attributed to a synergetic effect of the CuO nanoparticle incorporated in the CuO-ZnO nanocatalyst. However, when the reaction temperature was increased up to 533 K, a decline in the space time yield of methanol was observed for the catalysts prepared at high chitosan concentration.
机译:本研究采用壳聚糖辅助共沉淀法制备了CuO-ZnO纳米复合材料,并作为CO2加氢制甲醇的催化剂。研究了壳聚糖浓度对纳米复合材料的理化性质以及催化活性的影响。通过扫描电子显微镜,X射线衍射,N2吸附-解吸,N2O化学吸附和程序升温还原对所得催化剂进行表征。发现壳聚糖不仅充当配位化合物以产生均一的CuO-ZnO纳米复合材料组合,而且还充当形成空心纳米球的软模板。发现中空纳米球的CuO和ZnO微晶尺寸分别为11.5和18.8nm,小于其他催化剂的尺寸。壳聚糖浓度的增加引起催化剂形态的改变和BET表面积以及金属铜表面积的减少,但仍高于未改性催化剂的表面积。用壳聚糖作为沉淀剂制备的催化剂比未改性的催化剂表现出更高的甲醇时空产率,这归因于CuO-ZnO纳米催化剂中掺入的CuO纳米颗粒的协同作用。然而,当反应温度升高至533K时,对于在高壳聚糖浓度下制备的催化剂,观察到甲醇的时空产率下降。

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