An Efficient Discovery of Active, Selective and Stable Catalysts for Electrochemical H2O2 Synthesis Through Active Motif Screening

Abstract

<div> <div> <div> <p>Electrochemical reduction of O2 provides a clean and decentralized pathway to produce H2O2 compared to the current energy-intensive anthraquinone process. As the electrochemical reduction of O2 proceeds via either two-electron or four-electron path- way, it is thus essential to control the selectivity as well as to maximize the catalytic activity. Siahrostami et al. demonstrated a novel approach to control the reaction pathway by optimizing an adsorption ensemble to tune adsorption sites of reaction intermediates, and identified Pt-Hg catalysts from density functional theory (DFT) calculations and experimentally validated this catalyst (Nat. Mater. 2013, 12, 1137). Inspired by this concept, in this work, we apply a state-of-the-art high-throughput screening to develop O2 reduction catalyst for selective H2O2 production. Starting from Materials Project database, we evaluate activity, selectivity and electrochemical stability. To efficiently perform the screening, we introduce an active motif based approach which pre-screens unpromising materials and only performs DFT calculations for promising materials, which significantly reduce the number of the required calculations. We not only provide a list of promising candidates identified by DFT calculations, but also suggest element species to achieve high catalytic activity or H2O2 selectivity for future experimental attempts. Finally, we discuss a strategy for efficient future high-throughput screening using a machine learning pipeline consisting of a non-linear dimension reduction and a density-based clustering. </p> </div> </div> </div>

Atomic Structure-free Representation of Active Motifs for Expedited Catalyst Discovery

“…7,8 In this sense, binding energies are considered as descriptors for predicting catalytic activity and selectivity, which can be utilized to discover new catalysts by performing high-throughput screening for diverse classes and compositions of materials. [9][10][11][12][13][14][15] A procedure of the conventional high-throughput screening is summarized as follows 16,17 : (1) bulk structures are collected from inorganic materials database such as The Materials Project 18 or The Open Quantum Materials Database (OQMD) 19 , (2) lattice parameters and a shape of the bulk unit cell are optimized using density functional theory (DFT) calculations, (3) surface atomic structures (e.g., (111) or (211) facets) are modelled and (4) binding energies at all unique sites are calculated. As the number of candidate materials increases, the number of required DFT calculations would significantly increase.…”

Atomic Structure-free Representation of Active Motifs for Expedited Catalyst Discovery

“…7,8 In this sense, binding energies are considered as descriptors for predicting catalytic activity and selectivity, which can be utilized to discover new catalysts by performing high-throughput screening for diverse classes and compositions of materials. [9][10][11][12][13][14][15] A procedure of the conventional high-throughput screening is summarized as follows 16,17 : (1) bulk structures are collected from inorganic materials database such as The Materials Project 18 or The Open Quantum Materials Database (OQMD) 19 , (2) lattice parameters and a shape of the bulk unit cell are optimized using density functional theory (DFT) calculations, (3) surface atomic structures (e.g., (111) or (211) facets) are modelled and (4) binding energies at all unique sites are calculated. As the number of candidate materials increases, the number of required DFT calculations would significantly increase.…”