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Reverse water-gas shift in a packed bed DBD reactor: Investigation of metal-support interface towards a better understanding of plasma catalysis
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2019-12-31 , DOI: 10.1016/j.apcata.2019.117407
Yuhai Sun , Jingjing Li , Peirong Chen , Bangfen Wang , Junliang Wu , Mingli Fu , Limin Chen , Daiqi Ye

Palladium-loaded ZnO (Pd/ZnO) catalyst was synthesized by co-precipitation method and evaluated for plasma-catalytic reverse water-gas shift (RWGS) reaction. A CO2 conversion of 32.5% was achieved on “Pd/ZnO + Plasma”, and was around two times higher than that of “ZnO + Plasma” (17.3%). Catalyst characterization by X-ray diffraction, high-resolution transmission electron microscopy, temperature-programmed reduction and quasi in situ X-ray photoelectron spectroscopy revealed the possible formation of ZnOx@PdZn (ZnOx decorated PdZn alloy) at the interface of Pd active phase and ZnO support. The role of ZnOx@PdZn in plasma-catalytic CO2 conversion was systematically investigated by plasma-excited CO2 temperature-programmed desorption and in situ Fourier transform infrared spectroscopy. It was found that ZnOx@PdZn at Pd-ZnO interface improved significantly plasma-catalytic CO2 conversion by promoting the production of bidentate carbonate and bidentate formate species. In situ Raman spectroscopy studies proved that the ZnOx@PdZn remained largely intact during the RWGS process. Our in situ spectroscopic findings thus unveil that the ZnOx@PdZn at Pd-ZnO interface favors the activation of CO2, and, consequently, leads to a higher plasma-catalytic performance for CO2 conversion.



中文翻译:

填充床DBD反应器中的水煤气反向转化:研究金属-载体界面以更好地了解等离子体催化

通过共沉淀法合成了负载钯的ZnO(Pd / ZnO)催化剂,并进行了等离子体催化逆水煤气变换(RWGS)反应的评估。“ Pd / ZnO +等离子体”的CO 2转化率为32.5%,是“ ZnO +等离子体”的17.3%的两倍左右。通过X射线衍射,高分辨率透射电子显微镜,程序升温还原和准原位X射线光电子能谱对催化剂进行表征,发现可能在Pd活性物界面上形成ZnO x @PdZn(ZnO x装饰的PdZn合金)。相和ZnO载体。ZnO x @PdZn在等离子体催化CO 2中的作用通过等离子激发CO 2程序升温脱附和原位傅里叶变换红外光谱系统地研究了转化率。结果发现,Pd-ZnO界面处的ZnO x @PdZn通过促进碳酸盐和碳酸盐的生成,显着提高了等离子体催化的CO 2转化率。原位拉曼光谱研究证明,在RWGS过程中ZnO x @PdZn基本上保持完整。因此,我们的原位光谱发现揭示了Pd-ZnO界面处的ZnO x @PdZn有利于CO 2的活化。,因此导致更高的CO 2转化等离子体催化性能。

更新日期:2019-12-31
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