Autobifunctional Mechanism of Jagged Pt Nanowires for Hydrogen Evolution Kinetics via End-to-End Simulation
Autor: | Heting Pu, Juhyung Lim, Juhwan Kim, Xiangfeng Duan, Juhwan Noh, Changhyeok Choi, Chengzhang Wan, Tao Cheng, Yousung Jung, Sungwon Kim, Geun Ho Gu, William A. Goddard |
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Rok vydání: | 2021 |
Předmět: |
Chemistry
Kinetics Nanowire General Chemistry 010402 general chemistry Electrochemistry 01 natural sciences Biochemistry Catalysis 0104 chemical sciences Gibbs free energy chemistry.chemical_compound symbols.namesake Colloid and Surface Chemistry Adsorption Chemical physics symbols Bifunctional Nanoscopic scale |
Zdroj: | Journal of the American Chemical Society. 143(14) |
ISSN: | 1520-5126 |
Popis: | The extraordinary mass activity of jagged Pt nanowires can substantially improve the economics of the hydrogen evolution reaction (HER). However, it is a great challenge to fully unveil the HER kinetics driven by the jagged Pt nanowires with their multiscale morphology. Herein we present an end-to-end framework that combines experiment, machine learning, and multiscale advances of the past decade to elucidate the HER kinetics catalyzed by jagged Pt nanowires under alkaline conditions. The bifunctional catalysis conventionally refers to the synergistic increase in activity by the combination of two different catalysts. We report that monometals, such as jagged Pt nanowires, can exhibit bifunctional characteristics owing to its complex surface morphology, where one site prefers electrochemical proton adsorption and another is responsible for activation, resulting in a 4-fold increase in the activity. We find that the conventional design guideline that the sites with a 0 eV Gibbs free energy of adsorption are optimal for HER does not hold under alkaline conditions, and rather, an energy between -0.2 and 0.0 eV is shown to be optimal. At the reaction temperatures, the high activity arises from low-coordination-number (≤7) Pt atoms exposed by the jagged surface. Our current demonstration raises an emerging prospect to understand highly complex kinetic phenomena on the nanoscale in full by implementing end-to-end multiscale strategies. |
Databáze: | OpenAIRE |
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