Zhaojie Fang,Zetong Liu,Joe Yeang Cheah,Xinyi Guan,Huijuan Li,Tao Jiang,Shengping Wang,Xinbin Ma
A novel core–shell CaO based adsorbent with Al-Zr co-modification was synthesized via a facile one-pot calcination method. The CO 2 capture capacity and long-term stability of the adsorbents with different Ca/Al/Zr molar ratios were investigated. The co-doping strategy significantly enhanced the CO 2 capture capacity of the calcium-based adsorbents. Specifically, the optimized Ca24Al1Zr0.3 adsorbent exhibited excellent CO 2 adsorption performance in long-term adsorption–desorption cycles, with the CO 2 capacity of 0.53 g-CO 2 /g-ads after 40 cycles. The synergistic effects of Al-Zr co-doping were analyzed from a microstructural perspective. The core–shell Ca24Al1Zr0.3 adsorbent with a CaZrO 3 outer shell featured minimized particle size, abundant mesoporous and macroporous structures, and uniformly distributed doping components. Under the combined effects of structural modification and metal doping, it manifested enhanced CO 2 capture capacity. Based on the CO 2 adsorption mechanism of CaO, this study revealed that Al-Zr co-doping promotes oxygen vacancy generation and improves CO 2 adsorption performance. The Ca24Al1Zr0.3 adsorbent demonstrated the highest oxygen vacancy content and the most pronounced positive shift in Ca 2p binding energy. This shift enhanced electron-donating capability of calcium, effectively facilitating O 2− migration and CO 2 diffusion. Furthermore, the Ca24Al1Zr0.3 adsorbent exhibited superior carbonation reaction kinetics during long-term cyclic operation.
Ou Xing,Liu Tongchao,Zhong Wentao,Fan Xinming,Guo Xueyi,Huang Xiaojing,Cao Liang,Hu Junhua,Zhang Bao,Chu Yong S.,Hu Guorong,Lin Zhang,Dahbi Mouad,Alami Jones,Amine Khalil,Yang Chenghao,Lu Jun
High-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNi 0.88 Co 0.09 Mn 0.03 O 2 (SNCM) cathode material to circumvent the instability issue. We found that soluble Al ions are adequately incorporated in the SNCM lattice while the less soluble Zr ions are prone to aggregate in the outer SNCM surface layer. The synergistic effect of Al/Zr co-doping in SNCM lattice improve the Li-ion mobility, relief the internal strain, and suppress the Li/Ni cation mixing upon cycling at high cut-off voltage. These features improve the cathode rate capability and structural stabilization during prolonged cell cycling. In particular, the Zr-rich surface enables the formation of stable cathode-electrolyte interphase, which prevent SNCM from unwanted reactions with the non-aqueous fluorinated liquid electrolyte solution and avoid Ni dissolution. To prove the practical application of the Al/Zr co-doped SNCM, we assembled a 10.8 Ah pouch cell (using a 100 μm thick Li metal anode) capable of delivering initial specific energy of 504.5 Wh kg −1 at 0.1 C and 25 °C.
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