Efficient Discovery of Active, Selective, and Stable Catalysts for Electrochemical H2O2 Synthesis through Active Motif Screening
- 주제(키워드) density functional theory calculations , high-throughput screening , hydrogen peroxide , intermetallic alloys , active motif screening , ensemble effect , ligand effect
- 주제(기타) Chemistry, Physical
- 설명문(일반) [Na, Jonggeol] Ewha Womans Univ, BK21 Plus Program, Syst Hlth & Engn Major Grad Sch, Div Chem Engn & Mat Sci, Seoul 03760, South Korea; [Back, Seoin] Sogang Univ, Inst Emergent Mat, Dept Chem & Biomol Engn, Seoul 04107, South Korea; [Ulissi, Zachary W.] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA
- 관리정보기술 faculty
- 등재 SCIE, SCOPUS
- 발행기관 AMER CHEMICAL SOC
- 발행년도 2021
- URI http://www.dcollection.net/handler/ewha/000000181490
- 본문언어 영어
- Published As http://dx.doi.org/10.1021/acscatal.0c05494
초록/요약
Electrochemical reduction of O-2 provides a clean and decentralized pathway to produce H2O2 compared to the current energy-intensive anthraquinone process. As the electrochemical reduction of O-2 proceeds via either a two-electron or a four-electron pathway, it is thus essential to control the selectivity as well as to maximize the catalytic activity. Siahrostami et al. [Nat. Mater. 2013, 12, 1137] demonstrated a novel approach to control the reaction pathway by optimizing an adsorption ensemble to tune adsorption sites of reaction intermediates, identified Pt-Hg catalysts from density functional theory (DFT) calculations, and experimentally validated this catalyst. Inspired by this concept, in this work, we apply a state-of-the-art high-throughput screening to develop an O-2 reduction catalyst for selective H2O2 production. Starting from the 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 performs DFT calculations only for promising materials, which significantly reduces the number of the required calculations. Finally, we discuss a strategy for efficient future high-throughput screening using a machine learning pipeline consisting of a nonlinear dimension reduction and a density-based clustering.
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