Single Metal Site and Versatile Transfer Channel Merged into Covalent Organic Frameworks Facilitate High-Performance Li-CO2 Batteries,ACS Central Science

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Single Metal Site and Versatile Transfer Channel Merged into Covalent Organic Frameworks Facilitate High-Performance Li-CO2 Batteries
ACS Central Science ( IF 12.7 ) Pub Date : 2020-12-29 , DOI: 10.1021/acscentsci.0c01390
Yu Zhang ₁ , Rong-Lin Zhong ₂ , Meng Lu ₁ , Jian-Hui Wang ₁ , Cheng Jiang ₁ , Guang-Kuo Gao ₁ , Long-Zhang Dong ₁ , Yifa Chen ₁ , Shun-Li Li ₁ , Ya-Qian Lan _{1,

3}

Affiliation

The sluggish kinetics and unclear mechanism have significantly hindered the development of Li-CO₂ batteries. Here, a Li-CO₂ battery cathode catalyst based on a porphyrin-based covalent organic framework (TTCOF-Mn) with single metal sites is reported to reveal intrinsic catalytic sites of aprotic CO₂ conversion from the molecular level. The battery with TTCOF-Mn exhibits a low overpotential of 1.07 V at 100 mA/g as well as excellent stability at 300 mA/g, which is one of the best Li-CO₂ battery cathode catalysts to date. The unique features of TTCOF-Mn including uniform single-Mn(II)-sites, fast Li⁺ transfer pathways, and high electron transfer efficiency contribute to effective CO₂ reduction and Li₂CO₃ decomposition in the Li-CO₂ system. Density functional theory calculations reveal that different metalloporphyrin sites lead to different reaction pathways. The single-Mn(II) sites in TTCOF-Mn can activate CO₂ and achieve an efficient four-electron CO₂ conversion pathway. It is the first example to reveal the catalytic active sites and clear reaction pathways in aprotic Li-CO₂ batteries.

中文翻译：

单一金属位点和多功能传输通道合并为共价有机框架，可促进高性能Li-CO ₂电池的使用

缓慢的动力学和不清楚的机理已经严重阻碍了Li-CO ₂电池的发展。在此，据报道，基于具有单个金属位点的基于卟啉的共价有机骨架（TTCOF-Mn）的Li-CO ₂电池阴极催化剂从分子水平揭示了质子惰性CO ₂转化的内在催化位点。具有TTCOF-Mn的电池在100 mA / g时表现出1.07 V的低过电势，在300 mA / g时表现出出色的稳定性，这是迄今为止最好的Li-CO ₂电池阴极催化剂之一。TTCOF-Mn的独特特征包括均匀的单Mn（II）位，快速的Li ⁺转移途径和高的电子转移效率，有助于产生有效的CO ₂Li-CO ₂系统中的还原和Li ₂ CO ₃分解。密度泛函理论计算表明，不同的金属卟啉位点导致不同的反应途径。TTCOF-Mn中的单Mn（II）位点可以激活CO ₂并实现有效的四电子CO ₂转化途径。这是揭示非质子型Li-CO ₂电池中催化活性位点和清晰反应路径的第一个例子。

更新日期：2021-01-27

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