Historical Experimental Data and Theoretical Volcano Map Accelerated Cross-Scale Design of Highly Active and Durable Ternary Alloy Electrocatalyst for Formic Acid Oxidation

Abstract

Traditional trial in comprehensive multicomponent spaces driven by redundant chemical experiment may cause ignoring important features. Herein, we introduce historical experimental data and theoretical volcano map, coupled with the thermodynamic stability to provide insights by features ranking based on a robust formic acid oxidation reaction (FOR) database. The results indicate that the PdCuNi alloy catalyst screened by density functional theory (DFT) calculations and machine learning (ML) is a promising candidate for FOR. Electron-deficient surface Ni atoms promote the reduction of the thermodynamic energy barrier of FOR. PdCuNi medium entropy alloy aerogel (PdCuNi AA) was successfully synthesis through a simple one-pot NaBH4-reduction synthesis strategy. Obtained catalyst exhibits mass activity of 2.7 A/mg, surpassing PdCu, PdNi and commercial Pd/C by approximately 2.1, 2.7 and 6.9 folds. Moreover, the PdCuNi AA achieve an impressive power density around 153 mW/cm2 with 0.5 mg/cm2 loading in anode of direct formic acid fuel cells. Combining cutting-edge methods to drive innovative catalysts design will play a key role in advancing the development of fuel cells field.