Bimetallic or Multimetallic materials with atomic-precise structure and composition have shown great promise for catalyzing many chemical and electrochemical reactions1,2. By exploiting the synergy of metallic species alloyed, surface sites with novel physicochemical properties can be realized3,4. However, it is very time-consuming and costly to search for highly optimized alloys by high-throughput experiments and/or quantum-chemical calculations. Herein we tackle this problem by developing a machine-learning-augmented chemisorption model that captures complex, non-linear adsorbate-substrate interactions through artificial neural networks (ANNs) and thus enables large-scale exploration of reactivity descriptors in alloy materials space5. In this work, we use electrochemical reduction of carbon dioxide (CO2) on metal electrodes as an example because of current interest in this process for sustainable production of fuels and value-added chemicals6,7 (1) Calle-Vallejo, F.; Koper, M. T. M.; Bandarenka, A. S. Tailoring the Catalytic Activity of Electrodes with Monolayer Amounts of Foreign Metals. Chem. Soc. Rev. 2013, 42 (12), 5210–5230. (2) Campbell, C. T. Bimetallic Surface Chemistry. Annu. Rev. Phys. Chem. 1990, 41 (1), 775–837. (3) Xin, H.; Holewinski, A.; Linic, S. Predictive Structure–Reactivity Models for Rapid Screening of Pt-Based Multimetallic Electrocatalysts for the Oxygen Reduction Reaction. ACS Catal. 2012, 2 (1), 12–16. (4) Hammer, B.; Nørskov, J. K. Electronic Factors Determining the Reactivity of Metal Surfaces. Surf. Sci. 1995, 343 (3), 211–220. (5) Ma, X.; Li, Z.; Achenie, L. E. K.; Xin, H. Machine-Learning-Augmented Chemisorption Model for CO2 Electroreduction Catalyst Screening. J. Phys. Chem. Lett. 2015, 6 (18), 3528–3533. (6) Whipple, D. T.; Kenis, P. J. A. Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction. J. Phys. Chem. Lett. 2010, 1 (24), 3451–3458. (7) Peterson, A. A.; Abild-Pedersen, F.; Studt, F.; Rossmeisl, J.; Nørskov, J. K. How Copper Catalyzes the Electroreduction of Carbon Dioxide into Hydrocarbon Fuels. Energy Environ. Sci. 2010, 3 (9), 1311–1315.

Machine-learning-augmented chemisorption model for CO2 electroreduction catalyst screening

251st National Meeting (2016)

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