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A Successive Conversion–Deintercalation Delithiation Mechanism for Practical Composite Lithium Anodes

Peng ShiBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaLi‐Peng HouBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaChengbin JinBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaYe XiaoAdvanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaYuxing YaoBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaJin XieBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, ChinaBo‐Quan LiAdvanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaXue‐Qiang ZhangAdvanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, ChinaQiang ZhangBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
2021en
ABI

Аннотация

Lithium (Li) metal anodes are attractive for high-energy-density batteries. Dead Li is inevitably generated during the delithiation of deposited Li based on a conversion reaction, which severely depletes active Li and electrolyte and induces a short lifespan. In this contribution, a successive conversion-deintercalation (CTD) delithiation mechanism is proposed by manipulating the overpotential of the anode to restrain the generation of dead Li. The delithiation at initial cycles is solely carried out by a conversion reaction of Li metal. When the overpotential of the anode increases over the delithiation potential of lithiated graphite after cycling, a deintercalation reaction is consequently triggered to complete a whole CTD delithiation process, largely reducing the formation of dead Li due to a highly reversible deintercalation reaction. Under practical conditions, the working batteries based on a CTD delithiation mechanism maintain 210 cycles with a capacity retention of 80% in comparison to 110 cycles of a bare Li anode. Moreover, a 1 Ah pouch cell with a CTD delithiation mechanism operates for 150 cycles. The work ingeniously restrains the generation of dead Li by manipulating the delithiation mechanisms of the anode and contributes to a fresh concept for the design of practical composite Li anodes.

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