Bai Yuqing, Wei Le, Lian Yuebin, Wei Zhihe, Song Daqi, Su Yanhui, Zhu Xiong, Huo Wenxuan, Cheng Jian, Peng Yang, Deng Zhao
Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Suzhou 215006, P. R. China.
ACS Appl Mater Interfaces. 2023 Sep 6;15(35):41457-41465. doi: 10.1021/acsami.3c05778. Epub 2023 Aug 24.
Li-CO batteries that integrate energy storage with greenhouse gas fixation have received a great deal of attention in the pursuit of carbon neutrality. However, cyclic accumulation of the insulative and insoluble LiCO on the cathode surface severely restrains the battery cyclability, especially under a high depth of discharge/charge. Herein, we design and fabricate a microreactor-type catalyst by embedding Ru nanoparticles into the shells of mesoporous hollow carbon spheres. We show that both the hollow cavity and mesoporous shell are indispensable for concertedly furnishing a high activity to catalyze reversible LiCO formation/decomposition. This unique structure ensures that the Ru sites masked by exterior LiCO deposits during charging can resume the redox process of discharge by working with the prestored electrolyte to establish an inner reaction path. The thus fabricated Li-CO batteries demonstrate remarkable cyclability of 1085 cycles under 0.5 Ah g and 326 cycles under 2 Ah g at 1 A g, outshining most of the literature reports. This study highlights a smart catalyst design to boost the reversibility and cyclability of Li-CO batteries through an "in & out" strategy.
将储能与温室气体固定相结合的锂-二氧化碳电池在追求碳中和的过程中受到了广泛关注。然而，绝缘且不溶性的碳酸锂在阴极表面的循环积累严重限制了电池的循环性能，尤其是在高充放电深度下。在此，我们通过将钌纳米颗粒嵌入介孔空心碳球壳中来设计和制造一种微反应器型催化剂。我们表明，空心腔和介孔壳对于协同提供高活性以催化可逆碳酸锂的形成/分解都是必不可少的。这种独特的结构确保了在充电过程中被外部碳酸锂沉积物掩盖的钌位点能够通过与预先储存的电解质协同作用来恢复放电的氧化还原过程，从而建立一条内部反应路径。由此制造的锂-二氧化碳电池在1 A g下，在0.5 Ah g时表现出1085次循环的卓越循环性能，在2 Ah g时表现出326次循环，优于大多数文献报道。这项研究强调了一种智能催化剂设计，通过“内外”策略提高锂-二氧化碳电池的可逆性和循环性能。
