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Artificial Intelligence to Accelerate the Discovery of N2Electroreduction Catalysts
- Source :
- Chemistry of Materials; January 2020, Vol. 32 Issue: 2 p709-720, 12p
- Publication Year :
- 2020
-
Abstract
- The development of catalysts for the electrochemical N2reduction reaction (NRR) with a low limiting potential and high Faradaic efficiency is highly desirable but remains challenging. Here, to achieve acceleration, we develop and report a slab graph convolutional neural network (SGCNN), an accurate and flexible machine learning (ML) model that is suited for probing surface reactions in catalysis. With a self-accumulated database of 3040 surface calculations at the density-functional-theory (DFT) level, SGCNN predicted the binding energies, ranging over 8 eV, of five key adsorbates (H, N2, N2H, NH, NH2) related to NRR performance with a mean absolute error (MAE) of only 0.23 eV. SGCNN only requires the low-level inputs of elemental properties available in the periodic table of elements and connectivity information of constituent atoms; thus, accelerations can be realized. Via a combined process of SGCNN-driven predictions and DFT verifications, four novel catalysts in the L12crystal space, including V3Ir(111), Tc3Hf(111), V3Ni(111), and Tc3Ta(111), are proposed as stable candidates that likely exhibit both a lower limiting potential and higher Faradaic efficiency in the NRR, relative to the reference Mo(110). The ML work combined with a statistical data analysis reveals that catalytic surfaces with an average d-orbital occupation between 4 and 6 could lower the limiting potential and potentially overcome the scaling relation in the NRR.
Details
- Language :
- English
- ISSN :
- 08974756
- Volume :
- 32
- Issue :
- 2
- Database :
- Supplemental Index
- Journal :
- Chemistry of Materials
- Publication Type :
- Periodical
- Accession number :
- ejs51901575
- Full Text :
- https://doi.org/10.1021/acs.chemmater.9b03686