期刊
CHEMSUSCHEM
卷 14, 期 7, 页码 1737-1746出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202002946
关键词
density functional calculations; electrocatalysis; hydroxides; porous materials; relaxation processes
资金
- Ministry of energy and water, Israel
- Israel National Research Center for Electrochemical Propulsion (INREP)
- Grand Technion Energy Program (GTEP)
- Leonard and Diane Sherman Interdisciplinary Graduate School Fellowship
- Technion-Israel Institute of Technology
- UConn-GTEP joint program
Trimetallic double hydroxide NiFeCo-OH was prepared by coprecipitation, and three different catalysts were fabricated by different heat treatments, with the catalyst prepared at a heating and cooling rate of 2 degrees C min(-1) in N-2 atmosphere (designated NiFeCo-N-2-2 degrees C) showing the best catalytic performance. The study also found that hydroxide phase catalysts are less suitable for long-term use compared to oxide phase catalysts, with the higher surface energy of the hydroxide-phase catalyst impairing stability.
Trimetallic double hydroxide NiFeCo-OH is prepared by coprecipitation, from which three different catalysts are fabricated by different heat treatments, all at 350 degrees C maximum temperature. Among the prepared catalysts, the one prepared at a heating and cooling rate of 2 degrees C min(-1) in N-2 atmosphere (designated NiFeCo-N-2-2 degrees C) displays the best catalytic properties after stability testing, exhibiting a high current density (9.06 mA cm(-2) at 320 mV), low Tafel slope (72.9 mV dec(-1)), good stability (over 20 h), high turnover frequency (0.304 s(-1)), and high mass activity (46.52 A g(-1) at 320 mV). Stability tests reveal that the hydroxide phase is less suitable for long-term use than catalysts with an oxide phase. Two causes are identified for the loss of stability in the hydroxide phase: a) Modeling of the distribution function of relaxation times (DFRT) reveals the increase in resistance contributed by various relaxation processes; b) density functional theory (DFT) surface energy calculations reveal that the higher surface energy of the hydroxide-phase catalyst impairs the stability. These findings represent a new strategy to optimize catalysts for water splitting.
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