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FeO–CeO 2 nanocomposites: an efficient and highly selective catalyst system for photothermal CO 2 reduction to CO
NPG Asia Materials ( IF 9.7 ) Pub Date : 2020-01-24 , DOI: 10.1038/s41427-019-0171-5
Jiaqing Zhao , Qi Yang , Run Shi , Geoffrey I. N. Waterhouse , Xin Zhang , Li-Zhu Wu , Chen-Ho Tung , Tierui Zhang

Solar-driven catalysis is a promising strategy for transforming CO2 into fuels and valuable chemical feedstocks, with current research focusing primarily on increasing CO2 conversion efficiency and product selectivity. Herein, a series of FeO–CeO2 nanocomposite catalysts were successfully prepared by H2 reduction of Fe(OH)3-Ce(OH)3 precursors at temperatures (x) ranging from 200 to 600 °C (the obtained catalysts are denoted as FeCe-x). An FeCe-300 catalyst with an Fe:Ce molar ratio of 2:1 demonstrated outstanding performance for photothermal CO2 conversion to CO in the presence of H2 under Xe lamp irradiation (CO2 conversion, 43.63%; CO selectivity, 99.87%; CO production rate, 19.61 mmol h−1 gcat−1; stable operation over 50 h). Characterization studies using powder X-ray diffraction and high-resolution transmission electron microscopy determined that the active catalyst comprises FeO and CeO2 nanoparticles. The selectivity to CO of the FeCe-x catalysts decreased as the reduction temperature (x) increased in the range of 300–500 °C due to the appearance of metallic Fe0, which introduced an additional reaction pathway for the production of CH4. In situ diffuse reflectance infrared Fourier transform spectroscopy identified formate, bicarbonate and methanol as important reaction intermediates during light-driven CO2 hydrogenation over the FeCe-x catalysts, providing key mechanistic information needed to explain the product distributions of CO2 hydrogenation on the different catalysts.



中文翻译:

FeO–CeO 2纳米复合材料:用于将光热CO 2还原为CO的高效且高度选择性的催化剂体系

太阳能驱动的催化是将CO 2转化为燃料和有价值的化学原料的一种有前途的策略,目前的研究主要集中在提高CO 2转化效率和产品选择性方面。本文中,通过在200至600°C的温度(x)下H 2还原Fe(OH)3 -Ce(OH)3前体,成功制备了一系列FeO-CeO 2纳米复合催化剂。FeCe- x)。Fe:Ce摩尔比为2:1的FeCe-300催化剂显示出在H 2存在下将光热CO 2转化为CO的出色性能在Xe灯照射下(CO 2转化率为43.63%; CO选择性为99.87%; CO产率为19.61 mmol h -1  g cat -1;在50 h内稳定运行)。使用粉末X射线衍射和高分辨率透射电子显微镜进行的表征研究确定,活性催化剂包含FeO和CeO 2纳米颗粒。FeCe- x催化剂对CO的选择性随着还原温度(x)在300–500°C范围内的升高而降低,这归因于金属Fe 0的出现,这为生产CH 4引入了额外的反应途径。原位漫反射红外傅里叶变换光谱法将甲酸,碳酸氢盐和甲醇确定为FeCe- x催化剂上光驱动CO 2加氢过程中的重要反应中间体,提供了解释不同催化剂上CO 2加氢产物分布所需的关键机理信息。。

更新日期:2020-01-24
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