Selvaraj Seenivasan, Miyeon Kim, Jeong Woo Han, Do-Heyoung Kim
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引用次数: 0
摘要
了解氧氧化还原过程对于推动氧进化催化剂的发展至关重要,而氧进化催化剂在可再生燃料合成的电化学装置中至关重要。高熵金属氧化物的热力学不稳定性会通过电化学重构干扰氧氧化还原反应。通过在 KOH 中进行电化学处理,将 WN 预催化剂转化为热力学稳定的 KWO,并掺入极少量的铁,改变了氧进化反应(OER)的途径,使其具有氧氧化还原活性,而电解质的 pH 值对其影响很大。掺杂铁的 KWO 催化剂具有卓越的 OER 性能,在过电位仅为 181 mV(无 iR 补偿)的情况下就能达到 10 mA/cm^2,在 1000 mA/cm 的条件下可维持 1200 小时的使用寿命。电化学方法和 DFT 计算证实,铁掺杂会产生氧空位,增加费米级附近的电子密度,从而增强 OER 途径。这种方法为高熵催化剂适应广泛的电化学能量转换应用提供了一种通用方法,突出了其在可再生能源技术创新方面的潜力。
Minimal doping approach to activate lattice oxygen participation in K2WO4 electrocatalysts for oxygen evolution reaction
Understanding oxygen redox processes is pivotal for advancing oxygen evolution catalysts, critical in electrochemical devices for renewable fuel synthesis. Thermodynamic instability of high entropy metal oxides can interfere with oxygen redox reactions via electrochemical reconstruction. Transforming a WN pre-catalyst into thermodynamically stable KWO through electrochemical treatment in KOH, and incorporating minimal Fe doping, modifies the oxygen evolution reaction (OER) pathway towards oxygen redox activity, significantly influenced by the pH of the electrolyte. The Fe-doped KWO catalyst demonstrates superior OER performance, achieving 10 mA/cm^2 at an overpotential of merely 181 mV (without iR compensation) and sustaining a lifetime of 1200 h at 1000 mA/cm. Electrochemical methods and DFT calculations confirmed Fe doping creates oxygen vacancies and increases electron density near the Fermi level, enhancing the OER pathway. This methodology offers a versatile approach to adapt high entropy catalysts for broad electrochemical energy conversion applications, highlighting its potential for innovation in renewable energy technologies.