钙钛矿氧化物中CO$_2$转化活性的电子结构描述符
Electronic Structure Descriptors for CO$_2$ Conversion Activity in Perovskite Oxides
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- Kyungpook National University（庆北大学）
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中文总结 AI 辅助
本研究通过电子结构描述符揭示钙钛矿氧化物中CO₂转化活性与未占据TM 3d带中心、电荷转移能及带宽比W₃d/W₂p的负相关，并利用BFS方法得到仅依赖W₃d/W₂p的拟合方程，成功筛选出La₂CoGaO₆等有前景的候选材料。
中文摘要 AI 辅助
电子结构描述符已被广泛用于合理化催化活性，但其在钙钛矿氧化物中CO$_2$-to-CH$_4$转化中的应用仍然相对有限。在此，我们研究了与带中心和带宽相关的六个电子结构描述符。我们发现，未占据的过渡金属（TM）$3d$带中心、电荷转移能以及未占据的TM $3d$与占据的O $2p$带宽之比$W_{3d}/W_{2p}$与CH$_4$活性呈负相关。这些定性趋势通过参数化暴力搜索（BFS）方法进一步量化，以获得显式拟合方程。值得注意的是，所选方程仅依赖于$W_{3d}/W_{2p}$，为双钙钛矿中增强的活性提供了电子结构视角。我们将所选方程应用于筛选24种La基双钙钛矿。该筛选表明，La$_2$CoGaO$_6$、La$_2$CoAlO$_6$和含Ti的组合物是有前景的候选材料。本方法有助于识别描述符-活性关系，并指导钙钛矿氧化物的材料筛选。
英文摘要
Electronic structure descriptors have been widely used to rationalize catalytic activity, but their application to CO$_2$-to-CH$_4$ conversion in perovskite oxides remains relatively limited. Here, we investigate six electronic structure descriptors related to band centers and bandwidths. We find that the unoccupied transition-metal (TM) $3d$-band center, charge-transfer energy, and the ratio of the unoccupied TM $3d$ to occupied O $2p$ bandwidths, $W_{3d}/W_{2p}$, exhibit negative correlations with CH$_4$ activity. These qualitative trends are further quantified using a parametric brute-force searching (BFS) approach to obtain explicit fitting equations. Notably, the selected equations depend only on $W_{3d}/W_{2p}$, providing an electronic structure perspective on the enhanced activity in double perovskites. We apply the selected equation to screen 24 La-based double perovskites. This screening suggests that La$_2$CoGaO$_6$, La$_2$CoAlO$_6$, and Ti-containing compositions are promising candidates. The present approach can help identify descriptor-activity relationships and guide materials screening in perovskite oxides.
