Xu Changfan, Hong Ping, Dong Yulian, Li Yueliang, Shen Yonglong, Biskupek Johannes, Zhao Huaping, Kaiser Ute, Shao Guosheng, Lei Yong
Fachgebiet Angewandte Nanophysik, Institut für Physik & IMN MacroNano, Technische Universität Ilmenau, 98693, Ilmenau, Germany.
Central Facility for Electron Microscopy, Electron Microscopy Group of Materials Science, Ulm University, 89081, Ulm, Germany.
Adv Mater. 2024 Nov;36(48):e2409533. doi: 10.1002/adma.202409533. Epub 2024 Oct 9.
Despite their favorable high energy density and potential for CO recycling, Na-CO batteries have been held back by limitations in cycling capability, stemming from the sluggish CO reduction/evolution reaction (CORR/COER) kinetics at CO cathode and unmanageable deposition/stripping of metallic Na at the anode upon cycling. Herein, a "two-in-one" electrode with multiscale defective FeCu interfaces (CP@FeCu) is presented, which is capable of improving the CORR/COER kinetics of CO-breathing cathode, while modulating sodium deposition behavior. Experimental and theoretical investigations reveal multiscale defective FeCu interfaces are responsible for the enhancement of sodiophilicity and catalytic properties. The defect and valence oscillation effects originate in multiscale defective FeCu interfaces, effectively facilitating the adsorption of reactants and decomposition of NaCO during CORR/COER processes, along with exceptional cycling stability of 2400 cycles (4800 h) at 5 µA cm. Meanwhile, the CP@FeCu with sodium affinity creates a uniform electric field and robust adsorption for Na, making initial nucleation sites more conducive to Na deposition and achieving dendrite-resistant and durable anodes. This work offers a scientific insight into the functionalization design of "two-in-one" electrodes, which is essential for a unified solution to the challenges in sodium anodes and CO cathodes.
尽管钠-二氧化碳电池具有良好的高能量密度和二氧化碳循环利用潜力，但由于二氧化碳阴极上缓慢的二氧化碳还原/析出反应（CORR/COER）动力学以及循环过程中阳极金属钠难以控制的沉积/剥离，其循环性能受到限制。在此，提出了一种具有多尺度缺陷铁铜界面的“二合一”电极（CP@FeCu），它能够改善二氧化碳呼吸阴极的CORR/COER动力学，同时调节钠的沉积行为。实验和理论研究表明，多尺度缺陷铁铜界面是亲钠性和催化性能增强的原因。缺陷和价态振荡效应源于多尺度缺陷铁铜界面，有效地促进了CORR/COER过程中反应物的吸附和NaCO的分解，同时在5 μA cm下具有2400次循环（4800小时）的出色循环稳定性。与此同时，具有钠亲和力的CP@FeCu为钠创造了均匀的电场和强大的吸附作用，使初始成核位点更有利于钠的沉积，并实现抗枝晶和耐用的阳极。这项工作为“二合一”电极的功能化设计提供了科学见解，这对于统一解决钠阳极和二氧化碳阴极的挑战至关重要。
