Integrating photocatalysis and thermocatalysis to enable efficient CO2 reforming of methane on Pt supported CeO2 with Zn doping and atomic layer deposited MgO overcoating
Integrating photocatalysis and thermocatalysis to enable efficient CO2 reforming of methane on Pt supported CeO2 with Zn doping and atomic layer deposited MgO overcoating
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DOI：
10.1016/j.apcatb.2019.118189
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发表时间：
2020
影响因子：
22.1
通讯作者：
Fuping Pan;Xianmei Xiang;Zichen Du;Erik Sarnello;Tao Li;Ying Li
中科院分区：
文献类型：
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作者：
Fuping Pan;Xianmei Xiang;Zichen Du;Erik Sarnello;Tao Li;Ying Li
二氧化碳重整或甲烷干重整 (DRM) 生产的合成气具有低碳足迹，但 DRM 的效率和稳定性仍然是一个挑战。在此，我们报告了一种在 Pt 支持的 CeO2 催化剂上的高效光热化学 DRM (PTC-DRM) 工艺，该催化剂具有 Zn 掺杂和表面原子层沉积 (ALD) 启用的 MgO 外涂层，使用集中阳光作为能量输入。在600°C、30个太阳光照射下，H2和CO的合成气产量分别达到356和516 mmol g−1h−1，分别比热驱动DRM中的产量高9倍和3倍以上。此外，光照射稳定了干重整过程而不会失活，这是由于光诱导电子在CeO2上原位产生氧空位，从而实现稳定的CO2热激活。 ALD 涂层还通过钝化表面态减少表面电荷复合，从而增强光催化活性。
CO2reforming or dry reforming of methane (DRM) produces syngas with a low carbon footprint, but the efficiency and stability of DRM remains a challenge. Herein, we report an efficient photo-thermo-chemical DRM (PTC-DRM) process on a Pt supported CeO2catalyst with Zn doping and surface atomic layer deposition (ALD)-enabled MgO overcoating using concentrated sunlight as the energy input. Under 30 suns irradiation at 600 °C, high syngas production rates of 356 and 516 mmol g−1h−1for H2and CO are achieved, which are more than 9 and 3 times larger than those obtained in the thermally driven DRM. Moreover, the light illumination stabilizes the dry reforming process without deactivation, which results from the in situ generation of oxygen vacancy on CeO2by photo-induced electrons that enables stable CO2thermo-activation. The ALD coating also reduces surface charge recombination through passivating surface states, thereby enhancing photocatalytic activity.