Decarboxylation-Induced Defects in MOF-Derived Single Cobalt Atom@Carbon Electrocatalysts for Efficient Oxygen Reduction,Angewandte Chemie International Edition

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Decarboxylation-Induced Defects in MOF-Derived Single Cobalt Atom@Carbon Electrocatalysts for Efficient Oxygen Reduction
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-07-31 , DOI: 10.1002/anie.202107053
Shuai Yuan ₁ , Jinwei Zhang ₁ , Linyu Hu ₁ , Jiani Li ₁ , Siwu Li ₁ , Yanan Gao ₂ , Qinghua Zhang ₃ , Lin Gu ₃ , Wenxiu Yang ₁ , Xiao Feng ₁ , Bo Wang ₄

Affiliation

Developing transition metal single-atom catalysts (SACs) for oxygen reduction reaction (ORR) is of great importance. Zeolitic imidazolate frameworks (ZIFs) as a subgroup of metal-organic frameworks (MOFs) are distinguished as SAC precursors, due to their large porosity and N content. However, the activity of the formed metal sites is limited. Herein, we report a decarboxylation-induced defects strategy to improve their intrinsic activity via increasing the defect density. Carboxylate/amide mixed-linker MOF (DMOF) was chosen to produce defective Co SACs (Co@DMOF) by gas-transport of Co species to DMOF upon heating. Comparing with ZIF-8 derived SAC (Co@ZIF-8-900), Co@DMOF-900 with more defects yet one fifth Co content and similar specific double-layer capacitance show better ORR activity and eight times higher turnover frequency (2.015 e s⁻¹ site⁻¹). Quantum calculation confirms the defects can weaken the adsorption free energy of OOH on Co sites and further boost the ORR process.

中文翻译：

MOF衍生的单钴原子@碳电催化剂中脱羧引起的缺陷，用于高效氧还原

开发用于氧还原反应 (ORR) 的过渡金属单原子催化剂 (SAC) 非常重要。沸石咪唑骨架 (ZIF) 作为金属有机骨架 (MOF) 的一个亚组，由于其大孔隙率和 N 含量而被区分为 SAC 前体。然而，形成的金属位点的活性是有限的。在此，我们报告了一种脱羧诱导的缺陷策略，通过增加缺陷密度来提高其内在活性。选择羧酸盐/酰胺混合接头 MOF（DMOF）通过加热时将 Co 物质气体传输到 DMOF 来生产有缺陷的 Co SAC（Co@DMOF）。与 ZIF-8 衍生的 SAC（Co@ZIF-8-900）相比，Co@DMOF-900 具有更多的缺陷，但具有五分之一的 Co 含量和相似的特定双层电容显示出更好的 ORR 活性和八倍的周转频率（2.015 e s^-1 位点^-1 )。量子计算证实，这些缺陷会削弱 OOH 在 Co 位点上的吸附自由能，并进一步促进 ORR 过程。

更新日期：2021-09-20

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