Direct Machine Learning Predictions of C3 Pathways,Advanced Energy Materials

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Direct Machine Learning Predictions of C3 Pathways
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-02-11 , DOI: 10.1002/aenm.202400152
Mingzi Sun ₁ , Bolong Huang _{1,

2}

Affiliation

The C₃ pathways of CO₂ reduction reaction (CO₂RR) lead to the generation of high-value-added chemicals for broad industrial applications, which are still challenging for current electrocatalysis. Only limited electrocatalysts have been reported with the ability to achieve C₃ products while the corresponding reaction mechanisms are highly unclear. To overcome such challenges, the first-principle machine learning (FPML) technique on graphdiyne-based atomic catalysts (GDY-ACs) is introduced to directly predict the reaction trends for the key C─C─C coupling processes and the conversions to different C₃ products for the first time. All the prediction results are obtained only based on the learning dataset constructed by density functional theory (DFT) calculation results for C₁ and C₂ pathways, offering an efficient approach to screen promising electrocatalyst candidates for varied C₃ products. More importantly, the ML predictions not only reveal the significant role of the neighboring effect and the small–large integrated cycle mechanisms but also supply important insights into the C─C─C coupling processes for understanding the competitive reactions among C₁ to C₃ pathways. This work has offered an advanced breakthrough for the complicated CO₂RR processes, accelerating the future design of novel ACs for C₃ products with high efficiency and selectivity.

中文翻译：

C3 通路的直接机器学习预测

CO ₂还原反应（CO ₂ RR）的C ₃途径可产生用于广泛工业应用的高附加值化学品，这对当前的电催化仍然具有挑战性。仅报道了有限的电催化剂能够获得C ₃产物，而相应的反应机制还非常不清楚。为了克服这些挑战，引入石墨炔基原子催化剂（GDY-AC）的第一原理机器学习（FPML）技术来直接预测关键C─C─C偶联过程的反应趋势以及向不同C的转化_3种产品为首次。所有预测结果仅基于C ₁和C _{2路径的密度泛函理论（DFT）计算结果构建的学习数据集获得，为筛选各种C}₃产物的有前景的电催化剂候选物提供了有效的方法。更重要的是，ML预测不仅揭示了邻近效应和小-大整合循环机制的重要作用，而且还为C─C─C耦合过程提供了重要的见解，以了解C ₁到C ₃途径之间的竞争反应。这项工作为复杂的CO ₂ RR过程提供了先进的突破，加速了未来用于C ₃产品的高效和选择性的新型AC的设计。

更新日期：2024-02-11

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