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Highly dispersed metal doping to ZnZr oxide catalyst for CO2 hydrogenation to methanol: Insight into hydrogen spillover
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-12-08 , DOI: 10.1016/j.jcat.2020.11.039
Di Xu , Xinlin Hong , Guoliang Liu

Metallic oxide based catalysts have received much attention in CO2 hydrogenation to methanol because of their high methanol selectivity and long-term stability. But the relatively weak hydrogenation ability leads to low methanol activity. Here, we introduce a small amount of Cu (molar fraction < 2%) into ZnZrOx to form ternary metal oxide solid solution catalysts (x% CuZnZr) to promote methanol production. The optimized 0.5% CuZnZr catalyst performs CO2 conversion of 9.5% and methanol yield of 7.2%, both of which are about 4 times that of ZnZr catalyst at comparable methanol selectivity (76% versus 80%) at 290 °C. Chemisorption and in situ diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) analyses reveal that the enhanced activity is attributed to the improved hydrogenation capacity and accelerated transformation of HCOO* to CH3O* caused by hydrogen spillover from well dispersed Cu. This can also be applied to trace amount of Pd or Pt doping to ZnZrOx.



中文翻译:

高度分散的金属掺杂到ZnZr氧化物催化剂中,用于CO 2加氢成甲醇:氢气溢出的认识

基于金属氧化物的催化剂由于其高的甲醇选择性和长期稳定性而在CO 2加氢至甲醇中受到了广泛的关注。但是相对较弱的氢化能力导致较低的甲醇活性。在这里,我们将少量的Cu(摩尔分数<2%)引入ZnZrO x中,以形成三元金属氧化物固溶催化剂(x%CuZnZr)来促进甲醇的生产。优化的0.5%CuZnZr催化剂在290°C时具有相当的甲醇选择性(76%对80%),可实现9.5%的CO 2转化率和7.2%的甲醇产率,均为ZnZr催化剂的约4倍。化学吸附和原位漫反射傅里叶变换红外光谱(DRIFTS)分析表明,增强的活性归因于氢化能力的提高以及由氢从分散良好的铜中溢出引起的HCOO *向CH 3 O *的加速转化。这也可以应用于痕量的Pd或Pt掺杂到ZnZrO x中

更新日期:2020-12-23
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