Wang Yanqiu, Wu Dengdeng, Liu Tangkang, Liu Guoliang, Hong Xinlin
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, PR China.
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, PR China.
J Colloid Interface Sci. 2021 Sep;597:260-268. doi: 10.1016/j.jcis.2021.03.135. Epub 2021 Mar 26.
The conversion of CO to methanol is of great significance for providing a means of CO fixation and the development of future fuels. Supported Pd catalysts have been demonstrated to be active for CO hydrogenation to methanol and PdZn alloy plays a key role in this reaction. Therefore, using ZnO-enriched support to increase the amount of nanometric PdZn alloy particles on the surface is an effective strategy to develop ideal catalysts. Herein, we fabricated a PdZn alloy catalyst supported on ZnO-enriched ZnFeO spinel for efficient CO hydrogenation to methanol. The amount of formed PdZn alloy and catalyst structure influenced by ZnO concentration on ZnFeO were explored to obtain the best Pd-ZFO catalyst, which achieves a methanol space-time yield (STY) of 593 gkgh (12 ggh) with CO conversion of 14% under reaction conditions of 290 °C, 4.5 MPa and 21600 mLgh. Furthermore, the amount of exposed PdZn alloy sites were measured by using CO-pulse chemisorption and we find a linearity between methanol production rate and PdZn alloy sites.
将一氧化碳转化为甲醇对于提供一种固定一氧化碳的方法以及未来燃料的开发具有重要意义。负载型钯催化剂已被证明对一氧化碳加氢制甲醇具有活性,钯锌合金在该反应中起关键作用。因此,使用富含氧化锌的载体来增加表面纳米级钯锌合金颗粒的数量是开发理想催化剂的有效策略。在此,我们制备了一种负载在富含氧化锌的锌铁氧体尖晶石上的钯锌合金催化剂,用于高效一氧化碳加氢制甲醇。通过探索锌铁氧体上氧化锌浓度对形成的钯锌合金量和催化剂结构的影响,以获得最佳的钯 - 锌铁氧体催化剂,该催化剂在290℃、4.5MPa和21600mLgh的反应条件下,甲醇时空产率(STY)达到593gkgh(12ggh),一氧化碳转化率为14%。此外,通过一氧化碳脉冲化学吸附测量了暴露的钯锌合金位点的数量,我们发现甲醇产率与钯锌合金位点之间存在线性关系。