Chen Yanli, Li Junfeng, Lu Bingyi, Liu Yingqi, Mao Rui, Song Yanze, Li Hongtai, Yu Xinqian, Gao Yongzheng, Peng Qiong, Qi Xiaosi, Zhou Guangmin
Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.
College of Physics, Guizhou University, Guiyang, 550025, China.
Adv Mater. 2024 Oct;36(40):e2406856. doi: 10.1002/adma.202406856. Epub 2024 Aug 23.
Catalytic reactions mainly depend on the adsorption properties of reactants on the catalyst, which provides a perspective for the design of reversible lithium-carbon dioxide (Li-CO) batteries including CO reduction (CORR) and CO evolution (COER) reactions. However, due to the complex reaction process, the relationship between the adsorption configuration and CORR/COER catalytic activity is still unclear in Li─CO batteries. Herein, taking CoS as a model system, nickel (Ni substitution in the tetrahedral site to activate cobalt (Co) atom for forming multiatom catalytic domains in NiCoS is utilized. Benefiting from the special geometric and electronic structures, NiCoS exhibits an optimized adsorption configuration of lithium carbonate (LiCO), promoting its effective activation and decomposition. As a result, the Li-CO batteries with NiCoS cathode exhibit remarkable electrochemical performance in terms of low potential gap of 0.42 V and high energy efficiency of 88.7%. This work provides a unique perspective for the development of highly efficient catalysts in Li-CO batteries.
催化反应主要取决于反应物在催化剂上的吸附特性，这为设计包括CO还原（CORR）和CO析出（COER）反应的可逆锂二氧化碳（Li-CO₂）电池提供了一个视角。然而，由于反应过程复杂，在Li─CO₂电池中，吸附构型与CORR/COER催化活性之间的关系仍不明确。在此，以CoS为模型体系，利用在四面体位置进行镍（Ni）取代来活化钴（Co）原子，从而在NiCoS中形成多原子催化域。受益于特殊的几何和电子结构，NiCoS展现出碳酸锂（Li₂CO₃）优化的吸附构型，促进了其有效活化和分解。结果，具有NiCoS阴极的Li-CO₂电池在0.42 V的低电位差和88.7%的高能量效率方面表现出卓越的电化学性能。这项工作为Li-CO₂电池中高效催化剂的开发提供了独特的视角。
