钼配位高熵合金作为析氧反应的高效电催化剂,ACS Catalysis

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钼配位高熵合金作为析氧反应的高效电催化剂
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-08-19 , DOI: 10.1021/acscatal.2c02604
Yunjie Mei ₁ , Yuebin Feng ₁ , Chengxu Zhang _{1,

2} , Yue Zhang ₁ , Qianglong Qi ₁ , Jue Hu _{1,

3}

Affiliation

电化学水解制氢是可再生能源储存和转换最有前景的方法。然而，动力学缓慢析氧反应（OER）限制了阳极水电解的发展。最先进的 OER 催化剂面临着贵金属含量高和 OER 活性低的困境。本文报道了一种通过 Mo 配位实现高效稳定的高熵合金 (HEA) 催化剂的策略。^{地球丰富的 FeCoNiMo HEA 催化剂在碱性介质中的电流密度为 10 mA cm –2}时提供低至 250 mV 的过电势，比最先进的 IrO ₂低 89 mV 。周转频率 0.051 s ^–1在 300 mV 的过电位下，FeCoNiMo HEA 比商业 IrO ₂催化剂高 3 倍，甚至比没有 Mo 配位的 FeCoNi 合金高 11 倍。^{重要的是，FeCoNiMo HEA 在 100 mA cm –2}的高电流密度下表现出高 OER 稳定性. 甲醇分子探针实验和 X 射线光电子能谱分析表明，在 FeCoNiMo HEA 催化剂中，Mo 的电子转移到 Fe、Co 和 Ni，导致 OH* 键减弱，从而提高了 OER 性能。 FeCoNiMo HEA 催化剂。与甲醇分子探针分析一致，实时OER动力学模拟表明，Mo在FeCoNi中的配位可以加快OER的决定速率的OH*去质子化步骤。我们的发现开辟了一种为 OER 设计高效、具有成本效益的电催化剂的常规方法，这可以促进 OER 催化剂的发现。

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High-Entropy Alloy with Mo-Coordination as Efficient Electrocatalyst for Oxygen Evolution Reaction

Electrochemical hydrolytic hydrogen production is the most promising method for renewable energy storage and conversion. However, the kinetic slow oxygen evolution reaction (OER) limits the development of water electrolysis at the anode. The state-of-the-art OER catalysts face a dilemma of high content of noble metals and low OER activities. Herein, a strategy for achieving efficient and stable high-entropy alloy (HEA) catalysts by Mo-coordination is reported. The earth-abundant FeCoNiMo HEA catalyst provides an overpotential as low as 250 mV at the current density of 10 mA cm^–2 in alkaline medium, which is 89 mV lower than that of state-of-the-art IrO₂. The turnover frequency of 0.051 s^–1 at the overpotential of 300 mV of FeCoNiMo HEA is 3 times higher than that of commercial IrO₂ catalyst and even 11 times higher than that of the FeCoNi alloy without Mo-coordination. Importantly, the FeCoNiMo HEA exhibits high OER stability at a high current density of 100 mA cm^–2. Methanol molecular probe experiment and X-ray photoelectron spectroscopy analyses suggest that the electrons of Mo transfer to Fe, Co, and Ni in the FeCoNiMo HEA catalyst, which leads to a weakened OH* bonding and, as a result, enhanced OER performance of the FeCoNiMo HEA catalyst. Consistent with the methanol molecular probe analysis, the real-time OER kinetic simulation reveals that the coordination of Mo within FeCoNi can speed up the rate-determining OH* deprotonation step of OER. Our finding opens up a routine for designing efficient cost-effective electrocatalysts for OER, which could facilitate discoveries in OER catalysts.

更新日期：2022-08-19

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