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Morphology effect of ZnO support on the performance of Cu toward methanol production from CO2 hydrogenation
Journal of Saudi Chemical Society ( IF 5.8 ) Pub Date : 2019-09-12 , DOI: 10.1016/j.jscs.2019.09.002
Guangyu Shi , Qing Chen , Qiuhong Zhang , Weijie Cai , Zhongcheng Li , Shangru Zhai , Hao Yu , Fengzhi Tan , Yuanhao Wang

Recently, the chemical conversion of the greenhouse gas CO2 into value-added methanol has been of great interest. To address this issue, ZnO nanorods were synthesized by a facile microwave assisted technique and selected as support in Cu/ZnO catalyst. Herein, structure-activity relationship of the as-prepared catalysts in CO2 hydrogenation to methanol were elucidated in detail using different characterization technique including N2 physisorption, XRD, TPR, TEM, XPS and insitu DRIFTS (CO chemisorption) etc. Interestingly, rodlike ZnO hosted the highly dispersed Cu species, stronger Cu-support interaction at the interface in comparison with another reference CuZn-C sample, which was supported on commercial ZnO. In particular, EPR and XPS analysis evidenced the direct electron transfer from ZnO support to Cu species in CuZn-R, thereby facilitating the formation of O vacancies. These positive factors could provide the extremely active sites for CO2 hydrogenation and be correlated to the better catalytic activity. Indeed, the calculated TOFmethanol for CuZn-R was approximately ten times larger than that of CuZn-C sample. The results implied that the morphology structure of ZnO support, which could induce various crystal planes and amounts of defects and/or imperfections, possessed a critical role on the catalytic performance. This finding might shed light on the design of efficient catalysts for catalytic conversion of the undesirable CO2.



中文翻译:

ZnO载体的形貌对Cu对CO 2加氢生产甲醇性能的影响

近来,温室气体CO 2到增值甲醇的化学转化引起了人们的极大兴趣。为了解决这个问题,通过简便的微波辅助技术合成了ZnO纳米棒,并选择其作为Cu / ZnO催化剂的载体。在此,使用包括N 2在内的不同表征技术,详细阐明了在CO 2加氢中制得的催化剂与甲醇的构效关系。有趣的是,棒状ZnO具有高度分散的Cu物种,与另一种支持的参考CuZn-C样品相比,其界面处的Cu-支撑相互作用更强。在商用ZnO上。特别是,EPR和XPS分析证明了电子从ZnO载体直接转移到CuZn-R中的Cu物种,从而促进了O空位的形成。这些积极因素可以为CO 2加氢提供极活泼的位置,并与更好的催化活性相关。实际上,计算出的TOF甲醇CuZn-R的样品比CuZn-C样品的样品大约大十倍。结果表明,ZnO载体的形貌结构可以诱导各种晶面和大量的缺陷和/或缺陷,对催化性能具有至关重要的作用。这一发现可能为有效催化不希望的CO 2转化的催化剂的设计提供了启示。

更新日期:2019-09-12
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