采用原位生长-模板保护-裂解组装策略,对双金属类沸石咪唑骨架材料(ZIFs)前驱体进行结构调控,成功制备 Co-N_x、N-C活性位点及缺陷共存的二维钴-氮-碳纳米片(Co-N-C NFs)催化剂。Co-N-C NFs耦合了内在的Co-N-C的电子结构和外在的富缺陷的二维片层结构,为锂-二氧化碳电池(LCB)提供了有利的气-液-固三相反应界面;纳米薄片彼此交互,构建出有利于CO₂吸脱附、锂离子和电子迁移输运路径以及便于产物寄宿的空间结构。基于Co-N-C NFs催化剂正极构筑LCB电池,电池表现出优异的电化学性能,放电容量达到2 880 μAh/cm²,在100 μA/cm²的大电流密度下,放-充电平台维持在 2.60 V和4.40 V,且能稳定工作超1 480 h。

Taking in-situ growth-template protection-cracking assembly strategy,the precursor of bimetallic zeolite imidazole framework materials (ZIFs) is regulated on its structure to prepare a two-dimensional cobalt nitrogen carbon nanosheet (Co-N-C NFs) catalyst with coexisting of Co—N_x,and N—C active sites as well as defects.Co—N—C NFs couple the intrinsic electronic structure of Co—N—C with the extrinsic defect rich two-dimensional layered structure,providing a favorable gas-liquid-solid three-phase reaction interface for lithium carbon dioxide batteries (LCB).Nanosheets interact with each other to construct a spatial structure that facilitates the adsorption and desorption of CO₂,the migration transport pathways for lithium ion and electron,and product hosting.LCB battery constructed on the base of Co—N—C NFs catalyst cathode exhibits excellent electrochemical performance with a discharge capacity of 2 880 μAh/cm².At a high current density of 100 μA/cm²,the discharge-charge platform maintains 2.60 V and 4.40 V,and can operate stably for over 1 480 hours.

雷普英(1999-),女,硕士生,研究方向为CO₂的电化学还原与利用,leipuying1169@link.tyut.edu.cn;李雪莲(1990-),女,博士,助理研究员,研究方向为储能材料与器件(金属-气氛电池、金属离子电池、超级电容器)和CO₂电催化还原与氧化,通讯联系人,lixuelian@tyut.edu.cn。