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High-Throughput Computational-Experimental Screening Protocol for the Discovery of Bimetallic Catalysts

For decades of catalysis research, the d-band center theory that correlates the d-band center and the adsorbate binding energy has successfully enabled the accelerated discovery of novel catalyst materials. Recent studies indicate that, on top of the d-band center value, the full consideration of the d-band shapes describing higher moments of the d-band as well as sp-band properties can help better capturing surface reactivity. However, the density-of-states (DOS) patterns themselves have never been used as a descriptor in combined computational-experimental studies. Here, we propose the full DOS patterns as a key descriptor in high-throughput screening protocols, and prove its effectiveness. For the hydrogen peroxide (H2O2) synthesis as our demo catalytic reaction, the present study focuses on discovering bimetallic catalysts that can replace the prototypic palladium (Pd) one. Through a series of screening processes based on DOS pattern similarities (evaluated using first-principles calculations) and synthetic feasibility, 9 candidates are finally proposed out of 4,350 bimetallic alloy, which then are expected to have a catalytic performance comparable to that of Pd. The subsequent experimental tests demonstrate that 4 bimetallic catalysts (Ni61Pt39, Au51Pd49, Pt52Pd48, Pd52Ni48) indeed exhibit the catalytic properties comparable to those of Pd. Moreover, we discovered a novel bimetallic (Ni-Pt) catalyst, which has not yet been reported for H2O2 direct synthesis. In particular, Ni61Pt39 outperforms the prototypical Pd catalyst for the chemical reaction and exhibits a 9.5-fold enhancement in cost-normalized productivity. This protocol provides a new opportunity for the catalyst discovery for the replacement or reduction in use of the platinum-group metals.