Lewis Acid Strength of Interfacial Metal Sites Drives CH
<sub>3</sub>
OH Selectivity and Formation Rates on Cu‐Based CO
<sub>2</sub>
Hydrogenation Catalysts
作者:Gina Noh、Erwin Lam、Daniel T. Bregante、Jordan Meyet、Petr Šot、David W. Flaherty、Christophe Copéret
DOI:10.1002/anie.202100672
日期:2021.4.19
formation rates in CO2 hydrogenation on Cu‐based catalysts sensitively depend on the nature of the support and the presence of promoters. In this context, Cu nanoparticles supported on tailored supports (highly dispersed M on SiO2; M=Ti, Zr, Hf, Nb, Ta) were prepared via surface organometallic chemistry, and their catalytic performance was systematically investigated for CO2 hydrogenation to CH3OH. The
铜基催化剂在CO 2加氢中CH 3 OH的生成速率敏感地取决于载体的性质和促进剂的存在。在这种情况下,通过表面有机金属化学方法制备了负载在定制载体上的Cu纳米颗粒(M在SiO 2上高度分散; M = Ti,Zr,Hf,Nb,Ta),并系统地研究了它们的催化性能,用于CO 2加氢成CH。3 OH。路易斯酸位点的存在增强了CH 3OH形成速率,可能是由于Cu纳米颗粒外围的甲酸和甲氧基表面中间体的稳定化所致,这是由路易斯酸强度的度量和表面中间体的检测所证明的。表面中间体的稳定取决于路易斯酸M位点的强度,该位点由吡啶吸附焓和与O配位的OCH 3的13 C化学位移来描述。这些化学位移在这里被证明是路易斯酸强度和CO 2氢化反应性的分子描述。