Expediting in-Situ Electrochemical Activation of Two-Dimensional Metal–Organic Frameworks for Enhanced OER Intrinsic Activity by Iron Incorporation,ACS Catalysis

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Expediting in-Situ Electrochemical Activation of Two-Dimensional Metal–Organic Frameworks for Enhanced OER Intrinsic Activity by Iron Incorporation
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-07-08 00:00:00 , DOI: 10.1021/acscatal.9b00072
Zehua Zou , Tongtong Wang , Xiaohua Zhao , Wen-Jie Jiang ₁ , Hairui Pan , Daqiang Gao , Cailing Xu

Affiliation

Electrochemical activation is an effective and simple method to obtain in-situ surface modification of MOF materials away from thermal decomposition. However, the impact of the rate and related phase transformation on OER intrinsic activity during the electrochemical activation process is often overlooked. Herein, we synthesized a kind of Co-MOF with a unique crystal structure in which the center metals were coordinated with the oxygen and nitrogen atoms from two water molecules and organic linkers. The bond strength between the center metals and the coordinated water molecules can be modulated by introducing Fe into Co-MOF, causing the expedited electrochemical activation. First-principles calculations suggest the electronic state of cobalt in CoFe-MOF can be modified to alter the free energy of adsorbed intermediates. Therefore, the obtained electrocatalyst possesses the optimal OER intrinsic activity, showing a low overpotential of 265 mV at 10 mA cm^–2, a small Tafel slope of 44 mV dec^–1, and a long-term electrochemical durability with a period of 40 h. The findings are expected to help understand the fundamental principles of electrochemical activation.

中文翻译：

通过铁结合加速二维金属有机骨架的原位电化学活化，以增强OER的本征活性

电化学活化是一种有效且简单的方法，可以使MOF材料进行原位表面改性，而不会发生热分解。然而，在电化学活化过程中，速率和相关相变对OER固有活性的影响常常被忽略。本文中，我们合成了一种具有独特晶体结构的Co-MOF，其中中心金属与来自两个水分子和有机连接基的氧和氮原子配位。可以通过将Fe引入Co-MOF中来调节中心金属与配位水分子之间的结合强度，从而加快电化学活化。第一性原理计算表明，可以修改CoFe-MOF中钴的电子状态，以改变吸附的中间体的自由能。所以，^–2，Tafel斜率小，dec ^-1为44 mV ，长期电化学耐久性为40 h。预期该发现将有助于理解电化学活化的基本原理。

更新日期：2019-07-08

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