Catalytic mechanism and design principles for heteroatom-doped graphene catalysts in dye-sensitized solar cells
Catalytic mechanism and design principles for heteroatom-doped graphene catalysts in dye-sensitized solar cells
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DOI：
10.1016/j.nanoen.2018.04.053
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发表时间：
2018-07
期刊：
影响因子：
17.6
通讯作者：
Zhenghang Zhao;Chun-Yu Lin;Jinlong Tang;Z. Xia
中科院分区：
文献类型：
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作者：
Zhenghang Zhao;Chun-Yu Lin;Jinlong Tang;Z. Xia
掺杂碳纳米材料是取代昂贵的Pt对电极用于催化染料敏化太阳能电池（DSSC）中的三碘还原反应（IRR）的有希望的候选者，但是已经使用试错法来开发更好的催化剂。在这里，通过密度泛函理论（DFT）计算，开发了p-嵌段杂原子掺杂石墨烯作为高效IRR催化剂的设计原理。基于掺杂剂元素的固有性质的描述符被识别以建立将掺杂结构与催化活性相关联的定量关系。此外，还建立了催化性能和外在因素之间的定量关系，如暴露的活性中心的数量为特定的质量负载。据预测，大多数p-区元素掺杂的石墨烯催化剂具有比Pt更好的性能，并且在石墨烯边缘处掺杂增强催化活性。这些预测与实验结果是一致的。所提出的设计原则使我们能够合理地设计和寻找高活性的催化剂的基础上，地球丰富的，成本效益的材料。
Doped carbon nanomaterials are promising candidates to replace expensive Pt counter electrode for catalyzing triiodide reduction reaction (IRR) in dye-sensitized solar cells (DSSCs), but trial-and-error approaches have been used to develop better catalysts. Here, design principles are developed for p-block heteroatom-doped graphene as efficient IRR catalysts through density functional theory (DFT) calculations. The descriptors based on the intrinsic properties of dopant elements are identified to establish a quantitative relationship that correlates the doped structures to catalytic activities. Moreover, a quantitative relationship is also established between the catalytic performance and the extrinsic factors such as the number of exposed active sites for a particular mass loading. It is predicted that most p-block element doped graphene catalysts have better performance than Pt, and that doping at graphene edges enhances catalytic activities. These predictions are consistent with experimental results. The proposed design principles enable us to rationally design and search for highly active catalysts based on earth-abundant, cost-effective materials.