Lv Chunmei, Liu Jing, Lu Borong, Ye Ke, Wang Guiling, Zhu Kai, Cao Dianxue, Xie Ying
Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.
Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.
J Colloid Interface Sci. 2024 Jun;663:674-684. doi: 10.1016/j.jcis.2024.02.193. Epub 2024 Feb 29.
Reasonable design of cost-effective counter electrode (CE) catalysts for triiodide (I) reduction reaction (IRR) by simultaneously combining heteroatom doping and facet engineering is highly desired in iodine-based dye-sensitized solar cells (DSSCs), but really challenging. Herein, the density function theory (DFT) calculations were first conducted to demonstrate that the Fe-doped NiSe (111) showed an appropriate adsorption energy for I, increased number of metal active sites, reinforced charge-transfer ability, and strong interaction between 3d states of metal sites and 5p state of I atoms in I, compared to NiSe (111). Based on this finding, the well-defined Fe-NiSe octahedron with exposed (111) plane (marked as Fe-NiSe (111)) and NiSe octahedron with the same exposed plane (named as NiSe (111)) are controllably synthesized. When the as-prepared Fe-NiSe (111) and NiSe (111) worked as CE catalysts, Fe-NiSe (111) exhibits improved electrochemical performance with higher power conversion efficiency (PCE) than NiSe (111), providing new opportunity to replace precious Pt for DSSCs.
在基于碘的染料敏化太阳能电池（DSSC）中，通过同时结合杂原子掺杂和面工程来合理设计用于三碘化物（I）还原反应（IRR）的具有成本效益的对电极（CE）催化剂是非常必要的，但极具挑战性。在此，首先进行密度泛函理论（DFT）计算以证明，与NiSe（111）相比，Fe掺杂的NiSe（111）对I表现出合适的吸附能、增加的金属活性位点数量、增强的电荷转移能力以及金属位点的3d态与I原子的5p态之间在I中的强相互作用。基于这一发现，可控合成了具有暴露（111）面的明确的Fe-NiSe八面体（标记为Fe-NiSe（111））和具有相同暴露面的NiSe八面体（命名为NiSe（111））。当所制备的Fe-NiSe（111）和NiSe（111）用作CE催化剂时，Fe-NiSe（111）表现出比NiSe（111）更高的功率转换效率（PCE），从而展现出改善的电化学性能，为DSSC替代昂贵的Pt提供了新机会。
