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In this work, we developed a very facile strategy, i.e. dual dynamic crosslinking, to prepare a high performance injectable hydrogel. Poly(vinyl alcohol) (PVA) was crosslinked by 4-carboxyphenylboronic acid (CPBA) through the generation of borate bonding and ionic interaction to bridge the polymer chains in the presence of calcium ions. The dynamic gathering of CPBA could induce a self-reinforcing effect inside the hydrogel matrix, leading to high tensile and compressive moduli of the hydrogel over 1.0 MPa including the highest compressive modulus up to 5.6 MPa. Meanwhile, the mechanical properties of the hydrogel can be broadly and accurately tuned. And owing to the flexible PVA network, the hydrogel is ultra-tough, showing maximum tensile strain, tensile and compressive fracture energies up to 1600%, 600 kJ m−2 and 25 kJ m−2, respectively. Besides, the dynamic bonding overcomes the barriers to forming an injected strong hydrogel, e.g. to obtain a modulus and a fracture energy exceeding 1.0 MPa and 40 kJ m−2, by using a commercial dual-syringe kit under physiological conditions. Such a mild gelation procedure benefits the administration, 3D encapsulation and proliferation of cells of the hydrogels. The application of the PVA hydrogel was demonstrated by effective cartilage repair.

The inferior cycle performance of All-solid-state lithium batteries (ASSLBs) resulting from the low mixed ionic and electronic conductivity in the electrodes, as well as the large interfacial resistance between the electrodes and the electrolyte need to be overcome urgently for commercial applications. Here, an advanced cell construction strategy has been proposed, in which a cohesive and highly conductive poly(oxyethylene) (PEO)-based electrolyte is employed both in the cathode layer and in the interface of the electrolyte/anode, leading to an ASSLB with superior interfacial contact between the electrolyte and the electrodes, and forming a three-dimensional ionic conductive network in the cathode layer. Especially, the NASICON-type ionic conductor covered with the PEO-based polymer, integrating the advantages of an inorganic electrolyte and organic electrolyte, presents an enhanced electrochemical stability and an excellent compatibility with the Li electrode. Consequently, the ASSLBs of LiFePO4 (LFP)/Li with this advanced construction strategy exhibit excellent interfacial compatibility, ultralong cycle life and high capacity, i.e., a reversible discharge capacity maintained at 127.8 mA h g−1 for the 1000th cycle at 1C with a retention of 96.6%, and an initial discharge capacity of 153.4 mA h g−1 with a high retention of 99.9% after 200 cycles at 0.1C. Besides, the high-voltage monopolar stacked batteries with a bipolar structure can be fabricated conveniently, showing an open circuit voltage (OCV) of 6.63 V with a good cycle performance. In particular, the ASSLBs present outstanding safety in terms of nail penetration and burning in fire. Therefore, this advanced cell construction strategy may generate tremendous opportunities in the search for novel emerging solid-state lithium metal batteries.