Photothermocatalytic Dry Reforming of Methane for Efficient CO2 Reduction and Solar Energy Storage
Photothermocatalytic Dry Reforming of Methane for Efficient CO2 Reduction and Solar Energy Storage
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DOI：
10.1021/acssuschemeng.1c03692
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发表时间：
2021-09
影响因子：
8.4
通讯作者：
Shaowen Wu;Yuanzhi Li;Q. Hu;Jichun Wu;Qian Zhang
中科院分区：
文献类型：
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作者：
Shaowen Wu;Yuanzhi Li;Q. Hu;Jichun Wu;Qian Zhang
由于温室气体(CO2)的大量排放导致的能源短缺和全球变暖是两大全球战略问题。光催化太阳能燃料生产(例如，二氧化碳还原、水分解等)通过利用取之不尽的太阳能来解决这两个问题是非常有吸引力和前景的。从光催化原理来看，低的光-燃料转换效率(η)和燃料产率(RFuel)是不可逾越的挑战。因此，制定大幅度增加η和燃料的新战略势在必行，也是一个巨大的挑战。最近报道了一种新的甲烷光热催化干法重整反应策略(ΔH298=247kJmol-1)。通过该策略，仅使用基于纳米结构的第VIII族金属催化剂的聚焦照明就可以同时获得很高的η和rFuel值。光热催化DRM遵循光驱动热催化机理。与半导体光催化剂的传统光催化不同，一种新的光活化方法可以显著促进光驱动的热催化。在这一视角下，将讨论光驱动热催化DRM的机理、光到燃料的转化以及光活化。光热催化DRM的主要挑战是催化剂(特别是非贵金属族催化剂)的快速失活，这是由于伴随着DRM的热力学上不可避免的结焦副反应。讨论了通过设计非贵金属第八族金属催化剂来抑制结焦的策略，如通过氧化物团簇对纳米镍进行表面修饰，将纳米镍或钴负载到具有活性氧的氧化物上，形成镍合金纳米颗粒，在纳米镍颗粒周围形成CO2分子屏障等。
Energy shortage and global warming owing to greenhouse gas (CO2) discharge in enormous quantities are two major global strategic issues. Photocatalytic solar fuel production (e.g., CO2reduction, H2O splitting, etc.) by utilizing inexhaustible solar energy is very appealing and promising for addressing the two issues. Low light-to-fuel efficiencies (η) and fuel production rates (rfuel) are the impassable challenges in the view of the photocatalytic principle. Therefore, it is imperative and a great challenge to develop a new strategy of significantly increasing η andrfuel. Recently, a novel strategy of photothermocatalytic dry reforming of methane (DRM, CO2+ CH4= 2CO + 2H2, ΔH298= 247 kJ mol–1) has been reported. By the strategy, very high η andrfuelvalues have been simultaneously achieved merely using focused illumination based on nanostructured group VIII metal catalysts. The photothermocatalytic DRM abides by a mechanism of light-driven thermocatalysis. A novel photoactivation, quite different from conventional photocatalysis on semiconductor photocatalysts, is found to considerably promote light-driven thermocatalysis. In this Perspective, the light-driven thermocatalytic DRM mechanism, light-to-fuel conversion, and the photoactivation will be discussed. The major challenge for the photothermocatalytic DRM is the quick deactivation of the catalysts (especially nonprecious group VIII metal catalysts) due to thermodynamically inevitable side reactions of coke formation accompanying DRM. The strategies of kinetically inhibiting coke formation by designing nonprecious group VIII metal catalysts such as the surface modification of Ni nanoparticles by oxide clusters, loading Ni or Co nanoparticles on oxides with active oxygen, forming NiCo alloy nanoparticles, forming a CO2molecular fence around Ni nanoparticles, and so on, will be discussed.