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Interfacial covalent bonding enables transition metal phosphide superior lithium storage performance

High theoretical capacity and moderate redox potential enable transition metal phosphide (TMP) sparkle under a spotlight as viable anode materials for lithium-ion batteries (LIBs). However, TMP suffers from severe voltage hysteresis and poor reversibility due to the breaking and formation of TM-P and Li-P bonds during lithiation/delithiation processes, resulting in significant energy dissipation and rapid capacity decay. Besides, traditional thermal phosphorization involves generation of toxic PH3, which contradicts green chemistry concept. Herein, Ni2[email protected] composite is successfully achieved under plasma activation with Ni MOF-74 and red phosphide as the starting materials. The monodispersed Ni2P nanoparticles are uniformly anchored within carbon matrix through covalent chemical bonding of C-O-Ni and C-P. Systematic experimental analysis and theoretical calculation indicates that such efficient interfacial chemical linkage could weaken TM-P bonds and bridge the gap between Ni2P nanoparticles and carbon matrix, thus promoting the conversion reversibility during charge/discharge reactions. Benefited from the unique structure, voltage hysteresis of Ni2[email protected] is significantly suppressed, the reversible lithium storage capacity and cycling stability is greatly enhanced. By employing Ni2[email protected] and commercial LiFePO4 as anode and cathode, the full LIBs delivers a high reversible capacity of 0.6 mAh cm?2 after 300 cycles at 1.7?mA?cm?2. This strategy is expected to shed more light on interfacial chemical linkage towards rational design of advanced materials for LIBs.

» Author: Guoling Li, Hui Chen, Bin Zhang, Heng Guo, Shunpeng Chen, Xinghua Chang, Xiaohui Wu, Jie Zheng, Xingguo Li

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