TpyCo2+‐Based Coordination Polymers by Water‐Induced Gelling Trigged Efficient Oxygen Evolution Reaction,Advanced Functional Materials

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TpyCo2+‐Based Coordination Polymers by Water‐Induced Gelling Trigged Efficient Oxygen Evolution Reaction
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-08-05 , DOI: 10.1002/adfm.202000593
Qianqian Liu ₁ , Qichen Wang ₂ , Jun Wang ₃ , Zhengguang Li ₃ , Jingjing Liu ₃ , Xiaoyi Sun ₃ , Juan Li ₃ , Yongpeng Lei ₂ , Liming Dai ₄ , Pingshan Wang _{1,

3}

Affiliation

Though the use of conventional self‐assembled architectures in functional applications involving advanced energy chemistries is an important research area, it remains largely unexplored. The self‐assembly of the threefold and sixfold‐symmetric terpyridines (tpy) with Co(II) salts results in a novel morphological and structural characteristics, regardless of the nature of the self‐assembled fragments. Herein, such metallopolymers are achieved by one‐pot synthesis in CH₃OH/CHCl₃ (v/v = 5:1) mixture ambient. It is found, for the first time, that Co‐containing polymers can be well dispersed in deionized water to form gel‐like self‐assemblies that consist of a highly interconnected 3D network and exhibit enhanced electrical conductivity and thus are attractive as electrocatalysts. As expected, the optimized Co‐based polymeric structures exhibit a low overpotential of 320 mV at 10 mA cm⁻² and high stability over 2000 cycles toward oxygen evolution reaction (OER), surpassing commercial RuO₂/C, single‐site Co catalysts, polymer, and metal–organic framework‐based OER catalysts reported to date. X‐ray absorption spectroscopy and density functional theory calculations reveal that the tpy‐Co²⁺ (3N‐Co or tpy‐Co²⁺) configurations act as highly active sites. Importantly, this work demonstrates the functional application of the self‐assembled metallopolymers as electrocatalysts for energy conversion.

中文翻译：

水诱导胶凝引发的高效氧析出反应生成的基于TpyCo2 +的配位聚合物

尽管在涉及高级能源化学的功能应用中使用传统的自组装体系结构是一个重要的研究领域，但在很大程度上仍未得到开发。三重和六重对称的吡啶（Co）盐与Co（II）盐的自组装可产生新的形态和结构特征，而与自组装片段的性质无关。本文中，此类金属聚合物是通过在CH ₃ OH / CHCl _3中一锅合成而实现的（v / v = 5：1）混合环境。首次发现含钴聚合物可以很好地分散在去离子水中，形成凝胶状的自组装体，该组装体由高度互连的3D网络组成，并具有增强的电导率，因此作为电催化剂具有吸引力。正如预期的那样，经过优化的钴基聚合物结构在10 mA cm ^{-2的条件下}显示出320 mV的低过电势，并且在经过2000次循环进行放氧反应（OER）时具有很高的稳定性，超过了商用RuO ₂ / C，单中心Co催化剂，迄今已报道了聚合物和金属-有机构架基OER催化剂。X射线吸收光谱法和密度泛函理论计算表明tpy-Co ²⁺（3N-Co或tpy-Co ²⁺）配置充当高度活跃的网站。重要的是，这项工作证明了自组装金属聚合物作为电催化剂进行能量转换的功能性应用。

更新日期：2020-09-18

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