2020/09/16 by Byung Chul Yeo, Yeo, Byung Chul, Hyunji Nam +15 · 2 citations
Materials Science · Chemical Engineering · #Machine Learning in Materials Science #Catalytic Processes in Materials Science #Catalysis and Oxidation Reactions
paper · pdf · doi:10.48550/arxiv.2009.08048
For decades of catalysis research, the d-band center theory that correlates\nthe d-band center and the adsorbate binding energy has successfully enabled the\naccelerated discovery of novel catalyst materials. Recent studies indicate\nthat, on top of the d-band center value, the full consideration of the d-band\nshapes describing higher moments of the d-band as well as sp-band properties\ncan help better capturing surface reactivity. However, the density-of-states\n(DOS) patterns themselves have never been used as a descriptor in combined\ncomputational-experimental studies. Here, we propose the full DOS patterns as a\nkey descriptor in high-throughput screening protocols, and prove its\neffectiveness. For the hydrogen peroxide (H2O2) synthesis as our demo catalytic\nreaction, the present study focuses on discovering bimetallic catalysts that\ncan replace the prototypic palladium (Pd) one. Through a series of screening\nprocesses based on DOS pattern similarities (evaluated using first-principles\ncalculations) and synthetic feasibility, 9 candidates are finally proposed out\nof 4,350 bimetallic alloy, which then are expected to have a catalytic\nperformance comparable to that of Pd. The subsequent experimental tests\ndemonstrate that 4 bimetallic catalysts (Ni61Pt39, Au51Pd49, Pt52Pd48,\nPd52Ni48) indeed exhibit the catalytic properties comparable to those of Pd.\nMoreover, we discovered a novel bimetallic (Ni-Pt) catalyst, which has not yet\nbeen reported for H2O2 direct synthesis. In particular, Ni61Pt39 outperforms\nthe prototypical Pd catalyst for the chemical reaction and exhibits a 9.5-fold\nenhancement in cost-normalized productivity. This protocol provides a new\nopportunity for the catalyst discovery for the replacement or reduction in use\nof the platinum-group metals.\n