Cao Jiaqi, Chen Weixin, Gao Aosong, Muhtar Dilxat, Du Guangyuan, Qian Guoyu, Lu Xueyi, Xie Fangyan, Sun Yang, Lu Xia
School of Materials, Sun Yat-sen University, Shenzhen, 518107, P.R. China.
Instrumental Analysis & Research Center, Sun Yat-sen University, Guangzhou, 510275, PR China.
Angew Chem Int Ed Engl. 2025 Jan 2;64(1):e202413065. doi: 10.1002/anie.202413065. Epub 2024 Nov 2.
Rationally designing a current collector that can maintain low lithium (Li) porosity and smooth morphology while enduring high-loading Li deposition is crucial for realizing the high energy density of Li metal batteries, but it is still challengeable. Herein, a LiZnCu alloy-modified Cu foil is reported as a stable current collector to fulfill the stable high-loading Li deposition. Benefiting from the in situ alloying, the generated numerous LiZnCu@Cu heterojunctions induce a homogeneous Li nucleation and dense growth even at an ultrahigh capacity of 12 mAh cm. Such a spatial structure endows the overall LiZnCu@Cu electrode with the manipulated steric hindrance and outmost surface electric potential to suppress the side reactions during Li stripping and plating. The resultant Li||LiZnCu@Cu asymmetric cell preserves an ultrahigh average Coulombic efficiency of 99.2 % at 3 mA cm/6 mAh cm over 200 cycles. Moreover, the Li-LiZnCu@Cu||LiFePO cell maintains a cycling stability of 87.5 % after 300 cycles. After coupling with the LiCoO cathode (4 mAh cm), the cell exhibits a high energy density of 407.4 Wh kg with remarkable cycling reversibility at an N/P ratio of 3. All these findings present a doable way to realize the high-capacity, dendrite-free, and dense Li deposition for high-performance Li metal batteries.
合理设计一种集流体,使其在承受高负载锂沉积时能保持低锂孔隙率和光滑形态,这对于实现锂金属电池的高能量密度至关重要,但仍具有挑战性。在此,报道了一种锂锌铜合金改性的铜箔作为稳定的集流体,以实现稳定的高负载锂沉积。得益于原位合金化,即使在12 mAh cm的超高容量下,生成的大量LiZnCu@Cu异质结也能诱导均匀的锂成核和致密生长。这种空间结构赋予整个LiZnCu@Cu电极可控的空间位阻和最外层表面电势,以抑制锂剥离和电镀过程中的副反应。所得Li||LiZnCu@Cu不对称电池在3 mA cm/6 mAh cm下经过200次循环后保持99.2%的超高平均库仑效率。此外,Li-LiZnCu@Cu||LiFePO电池在300次循环后保持87.5%的循环稳定性。与LiCoO阴极(4 mAh cm)耦合后,该电池在N/P比为3时表现出407.4 Wh kg的高能量密度和显著的循环可逆性。所有这些发现为高性能锂金属电池实现高容量、无枝晶和致密锂沉积提供了一种可行的方法。