Syngas production at a near-unity H 2 /CO ratio from photo-thermo-chemical dry reforming of methane on a Pt decorated Al 2 O 3 –CeO 2 catalyst
Syngas production at a near-unity H 2 /CO ratio from photo-thermo-chemical dry reforming of methane on a Pt decorated Al 2 O 3 –CeO 2 catalyst
复制标题
在 Pt 修饰的 Al 2 O 3 →CeO 2 催化剂上通过光热化学干重整甲烷以接近一致的 H 2 /CO 比例生产合成气
DOI：
10.1039/d1ta10088b
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发表时间：
2022
影响因子：
11.9
通讯作者：
Li, Ying
中科院分区：
文献类型：
--
作者：
Feng, Xuhui;Du, Zichen;Sarnello, Erik;Deng, Wei;Petru, Cullen R.;Fang, Lingzhe;Li, Tao;Li, Ying
制备了等摩尔Al_2O_3-CeO_2二元氧化物负载Pt催化剂（Pt-Al-Ce），并将其应用于聚光太阳辐射驱动的甲烷光热化学干重整反应（DRM）。结果表明，与Pt/CeO 2（Pt-Ce）和Pt/Al 2 O3（Pt-Al）催化剂相比，Pt-Al-Ce催化剂在DRM反应中表现出良好的稳定性，并显著提高了H2和CO的产率。在700 °C的反应温度下，在30太阳当量的太阳照射下，Pt-Al-Ce催化剂表现出稳定的DRM催化性能，H2产生速率为657 mmol g−1 h−1，CO产生速率为666 mmol g−1 h −1，H2/CO比几乎等于1。这些生产率和H2/CO比显着高于在黑暗中在相同的温度下获得的。光照射可诱导Pt-Al-Ce的光催化活性，降低反应活化能。采用原位漫反射红外光谱（in situ DRIFTS）技术对光热化学DRM过程中的活性中间体进行了表征，包括双齿/单齿碳酸盐、吸附在Pt上的CO和甲酸盐.二元Al 2 O3-CeO 2基质的益处可归因于Al 2 O3促进甲烷解离，而CeO 2稳定并消除可能的焦炭形成，从而导致高催化DRM活性和稳定性。
In this work, a Pt catalyst supported on an equimolar Al2O3–CeO2 binary oxide (Pt–Al–Ce) was prepared and applied in photo-thermo-chemical dry reforming of methane (DRM) driven by concentrated solar irradiation. It was found that the Pt–Al–Ce catalyst showed good stability in DRM reactions and significant enhancements in H2 and CO production rates compared with Pt/CeO2 (Pt–Ce) and Pt/Al2O3 (Pt–Al) catalysts. At a reaction temperature of 700 °C under 30-sun equivalent solar irradiation, the Pt–Al–Ce catalyst exhibits a stable DRM catalytic performance at a H2 production rate of 657 mmol g−1 h−1 and a CO production rate of 666 mmol g−1 h−1, with the H2/CO ratio almost equal to unity. These production rates and the H2/CO ratio were significantly higher than those obtained in the dark at the same temperature. The light irradiation was found to induce photocatalytic activities on Pt–Al–Ce and reduce the reaction activation energy. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) was applied to identify the active intermediates in the photo-thermo-chemical DRM process, which were bidentate/monodentate carbonate, absorbed CO on Pt, and formate. The benefits of the binary Al2O3–CeO2 substrate could be ascribed to Al2O3 promoting methane dissociation while CeO2 stabilized and eliminated possible coke formation, leading to high catalytic DRM activity and stability.