Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 1, Pages 212-218Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c08606
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Funding
- Beijing Municipal Natural Science Foundation [Z20J00043]
- National Key Research and Development Program [2021YFB2500300]
- National Natural Science Foundation of China [21825501, 22109007, 52103342]
- China Postdoctoral Science Foundation [BX2021136, 2021M691712]
- Shuimu Tsinghua Scholar Program
- Tsinghua University Initiative Scientific Research Program
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This study proposes a successive conversion-deintercalation (CTD) delithiation mechanism to restrain the generation of dead Li by manipulating the overpotential of the anode. The working batteries based on this mechanism show improved cycling performance and capacity retention under practical conditions.
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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