Abstract:Nickel-rich layered electrode material has been attracting
significant
attention owing to its high specific capacity as a cathode for lithium-ion
batteries. Generally, the high-nickel ternary precursors obtained
by traditional coprecipitation methods are micron-scale. In this work,
the submicrometer single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM) cathode is efficiently prepared
by electrochemically anodic oxidation followed by a molten-salt-assisted
reaction without the need of extreme alkaline environments and compl… Show more
“…Similar to sodium salts, lithium salts have also been widely utilized as flux agents for lowering the melting point of reactants, such as Li 2 MoO 4 , [62] LiCl, [63][64][65] LiNO 3 , [66][67][68] Li 2 O 2 [69] and Li 2 SO 4 . [70][71][72][73] For instance, Li 2 MoO 4 , possessing a melting point of 704 °C, has been utilized as a flux agent in the preparation of SC-NCM111.…”
Li(NixCoyMnz)O2 (x + y + z = 1, NCM), as one of the most dominant cathode materials in electric vehicle (EV) batteries, faces the challenges of poor cycling stability and safety concerns with the increase of Ni content and charge/discharge capacity. Single crystalline NCM (SC‐NCM) materials have been developed to mitigate these challenges, owing to their lower surface areas, fewer grain boundaries, and better morphological stability. Here, the preparation strategies of SC‐NCM are summarized, including continuous high‐temperature sintering (CHTS), molten salt method, pulse high‐temperature sintering (PHTS), and controllable growth with special orientations or sizes. CHTS produces irregular SC‐NCM particles, but is accompanied by Li‐volatilization and agglomeration during long‐term sintering. The molten salt helps to lower calcination temperature and generate well‐defined crystalline material, but generally causes large capacity loss due to the Li/H exchange in the following water rinsing procedure. To address the above challenges, the PHTS strategy has recently been recently proposed, which mitigates Li‐loss through shortened high‐temperature stage and avoids further water rinsing steps. For improving the C‐rate performance, controllable crystal growth with specific sizes and crystal orientations is highly desired, which calls for further investigation and upgrading of current large‐scale preparation technology.
“…Similar to sodium salts, lithium salts have also been widely utilized as flux agents for lowering the melting point of reactants, such as Li 2 MoO 4 , [62] LiCl, [63][64][65] LiNO 3 , [66][67][68] Li 2 O 2 [69] and Li 2 SO 4 . [70][71][72][73] For instance, Li 2 MoO 4 , possessing a melting point of 704 °C, has been utilized as a flux agent in the preparation of SC-NCM111.…”
Li(NixCoyMnz)O2 (x + y + z = 1, NCM), as one of the most dominant cathode materials in electric vehicle (EV) batteries, faces the challenges of poor cycling stability and safety concerns with the increase of Ni content and charge/discharge capacity. Single crystalline NCM (SC‐NCM) materials have been developed to mitigate these challenges, owing to their lower surface areas, fewer grain boundaries, and better morphological stability. Here, the preparation strategies of SC‐NCM are summarized, including continuous high‐temperature sintering (CHTS), molten salt method, pulse high‐temperature sintering (PHTS), and controllable growth with special orientations or sizes. CHTS produces irregular SC‐NCM particles, but is accompanied by Li‐volatilization and agglomeration during long‐term sintering. The molten salt helps to lower calcination temperature and generate well‐defined crystalline material, but generally causes large capacity loss due to the Li/H exchange in the following water rinsing procedure. To address the above challenges, the PHTS strategy has recently been recently proposed, which mitigates Li‐loss through shortened high‐temperature stage and avoids further water rinsing steps. For improving the C‐rate performance, controllable crystal growth with specific sizes and crystal orientations is highly desired, which calls for further investigation and upgrading of current large‐scale preparation technology.
The difficulty in matching cathode and anode kinetics due to slow ion transport in anodes constrains the development of lithium‐ion capacitors. Heterogeneous structures with built‐in electric field can promote lithium‐ion migration and improve the anode reaction kinetics. However, the valence evolution of metal elements in heterostructures during charging/discharging processes is often overlooked. Inspired by theoretical calculations, transition metal selenides heterostructures (FeSe2/CoSe2) with low migration energy barriers (E
b = 0.35 eV) are successfully engineered and fabricated. As expected, the designed heterostructure material exhibits outstanding rate performance (512 mAh g−1 at 30 A g−1) and ultra‐high pseudocapacitance contribution (98.02% at 1.0 mV s−1), exceeding the state‐of‐the‐art values for anodes. Impressively, synchrotron X‐ray absorption spectroscopy (SXAS) and ex situ XPS find that the valence states of the Fe and Co elements in the heterogeneous structure gradually increase as charging and discharging proceeds, inducing a continuous climb in reversible specific capacity, while further reducing the migration energy barrier in the heterogeneous structure (E
b = 0.20 eV). This work reveals that the valence states of iron and cobalt elements increase as charging and discharging proceeds, providing theoretical guidance for improving the anode kinetics and revealing the capacity rise mechanism of other transition metal compounds.
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