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Inert Mg Incorporation to Break the Activity/Stability Relationship in High-Entropy Layered Hydroxides for the Electrocatalytic Oxygen Evolution Reaction
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-05-24 , DOI: 10.1021/acscatal.3c00786 Da Liu 1 , Xiaoxiao Yan 1 , Peifang Guo 1 , Yaxiong Yang 2 , Yufei He 3 , Jing Liu 3 , Jian Chen 2 , Hongge Pan 2, 3 , Renbing Wu 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-05-24 , DOI: 10.1021/acscatal.3c00786 Da Liu 1 , Xiaoxiao Yan 1 , Peifang Guo 1 , Yaxiong Yang 2 , Yufei He 3 , Jing Liu 3 , Jian Chen 2 , Hongge Pan 2, 3 , Renbing Wu 1
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Ni-based layered double hydroxides (LDHs) have been demonstrated as the most active catalyst for the oxygen evolution reaction in alkaline media but suffer from poor stability. Herein, we report the rational breaking of the activity/stability trade-off by a strategy of inert Mg-involved high-entropy coordination. The as-developed high-entropy FeCoNiMg-LDH nanosheets exhibit not only high catalytic activity (302 mV at 100 mA cm–2) but also an unprecedented stability with almost no performance decline at a large current density of 300 mA cm–2. The combined structural investigations and theoretical calculations reveal that the synergistic electronic coupling provides active Ni in desired electronic states, leading to an optimized adsorption energy of intermediates, while the construction of high configuration entropy as well as the formation of the Mg–O interfacial bond can effectively mitigate phase segregation and transformation and thus improve the stability. The current insights into unveiling the composition–activity–stability of high-entropy coordination may provide valuable guidance for the design of catalysts for various electrochemical reactions.
中文翻译：
惰性镁掺入打破高熵层状氢氧化物电催化析氧反应的活性/稳定性关系
镍基层状双氢氧化物（LDHs）已被证明是碱性介质中析氧反应最活跃的催化剂，但稳定性较差。在此，我们报告了通过惰性 Mg 参与的高熵配位策略合理打破活性/稳定性权衡。所开发的高熵 FeCoNiMg-LDH 纳米片不仅具有高催化活性（在 100 mA cm –2时为 302 mV ），而且具有前所未有的稳定性，在 300 mA cm –2的大电流密度下几乎没有性能下降. 结合结构研究和理论计算表明，协同电子耦合提供了所需电子态的活性 Ni，从而优化了中间体的吸附能，同时高构型熵的构建以及 Mg-O 界面键的形成可以有效地缓解了相分离和相变，从而提高了稳定性。目前对揭示高熵配位的组成-活性-稳定性的见解可能为各种电化学反应的催化剂设计提供有价值的指导。
更新日期：2023-05-24
中文翻译：
惰性镁掺入打破高熵层状氢氧化物电催化析氧反应的活性/稳定性关系
镍基层状双氢氧化物（LDHs）已被证明是碱性介质中析氧反应最活跃的催化剂，但稳定性较差。在此，我们报告了通过惰性 Mg 参与的高熵配位策略合理打破活性/稳定性权衡。所开发的高熵 FeCoNiMg-LDH 纳米片不仅具有高催化活性（在 100 mA cm –2时为 302 mV ），而且具有前所未有的稳定性，在 300 mA cm –2的大电流密度下几乎没有性能下降. 结合结构研究和理论计算表明，协同电子耦合提供了所需电子态的活性 Ni，从而优化了中间体的吸附能，同时高构型熵的构建以及 Mg-O 界面键的形成可以有效地缓解了相分离和相变，从而提高了稳定性。目前对揭示高熵配位的组成-活性-稳定性的见解可能为各种电化学反应的催化剂设计提供有价值的指导。
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