Nonbattery behavior related phase transition of electrodes is usually not favorable for any batteries because it results in performance degradation at all times. Here, we demonstrate a zinc hybrid-ion battery (ZHIB) with an unusual capacity enhancement even within 18 000 cycles by employing V2CTX MXene as the cathode, enormously differing from all reported counterparts with capacity degradation initiated within hundreds of cycles. The dominated mechanisms are determined to be MXene delamination and an unexpected phase transition during cycling. Both the original cathode and secondary derivative contribute to capacity simultaneously, resulting in the unusual capacity enhancement. Consequently, the specific capacity of 508 mAh g–1 (highest for all reported aqueous zinc-ion batteries) and high energy density of 386.2 Wh kg–1 are realized. Also, the quasi-solid-state batteries fabricated can output stably at −20 °C and in bending, twisting, stabbing, and cutting conditions. Our work brings an effective approach, that is, utilizing “unstable” electrode materials, which should usually be avoided, to achieve continuously enhanced performance of a battery. The idea to use both original and secondary materials for energy storage may be developed to be a general method to achieve extraordinary cycling stability of batteries.
Minxia Jiang,Minxi Li,Chang Cui,Jie Wang,Yang Cheng,Yixin Wang,Xing Zhang,Jinwen Qin,Minhua Cao
Ti3C2Tx MXene often suffers from poor lithium storage behaviors due to its electrochemically unfavorable OH terminations. Herein, we propose molecular-level interfacial chemistry regulation of Ti3C2Tx MXene with phytic acid (PA) to directly activate its OH terminations. Through constructing hydrogen bonds (H-bonds) between oxygen atoms of PA and OH terminations on Ti3C2Tx surface, interfacial charge distribution of Ti3C2Tx has been effectively regulated, thereby enabling sufficient ion-storage sites and expediting ion transport kinetics for high-performance energy storage. The results show that Li ions preferably bind to H-bond acceptors (oxygen atoms from PA), and the flexibility of H-bonds therefore renders their interactions with adsorbed Li ions chemically “tunable”, thus alleviating undesirable localized geometric changes of the OH terminations. Meanwhile the H-bond-induced microscopic dipoles can act as directional Li-ion pumps to expedite ion diffusion kinetics with lower energy barrier. As a result, the as-designed Ti3C2Tx/PA achieves a 2.4-fold capacity enhancement compared with pristine Ti3C2Tx (even beyond theoretical capacity), superior long-term cyclability (220.0 mAh g–1 after 2000 cycles at 2.0 A g–1), and broad temperature adaptability (−20 to 50 °C). This work offers a promising interface engineering strategy to regulate microenvironments of inherent terminations for breaking through the energy storage performance of MXenes.
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