This review elaborately summarizes the latest progress in all-pseudocapacitive asymmetric supercapacitors, including aqueous/nonaqueous faradaic electrode materials, the operating principles, system design/engineering, and rational optimization.

In this work, polypyrrole/graphene doped by p-toluenesulfonic is prepared as an active material for supercapacitors, and its capacitance performance is investigated in various aqueous electrolytes including HCl, LiCl, NaCl, and KCl with a concentration of 3 M, respectively. A rising trend of capacitance is observed according to the cationic mobility (Li(+) < Na(+) < K(+) < H(+)), which is due to its effect on the ionic conductivity, efficient ion/charge diffusion/exchange and relaxation time. On the other hand, long-term cycling stability is in the following order: KCl < NaCl < LiCl < HCl, corresponding to the decreasing tendency of cation size (K(+) > Na(+) > Li(+) > H(+)). The reason can be attributed to the fact that the insertion/de-insertion of large size cation brings a significant doping level decrease and an over-oxidation increase during the charging-discharging cycles. Hence, we not only obtain good capacitance performance (280.3 F g(-1) at 5 mV s(-1)), superior rate capability (225.8 F g(-1) at 500 mV s(-1)) and high cycling stability (92.0% capacitance retention after 10,000 cycles at 1 A g(-1)) by employing 3 M HCl as an electrolyte, but also reveal that the electrolyte cations have a significant effect on the supercapacitors' electrochemical performance.

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Nanostructured Fe3O4 is intrinsically prone to aggregation, which hinders insertion and extraction of lithium ions.

High energy density Li2MnO3 is fully activated by F-substitution by decreasing the grain size and improving the Li+ diffusion kinetics.

Coulombic efficiency especially in the first cycle, cycling stability, and high-rate performance are crucial factors for commercial Li-ion batteries (LIBs). To improve them, in this work, Al2O3-coated natural graphite powder was obtained through a low-cost and facile sol-gel method. Based on a comparison of various coated amounts, 0.5 mol % Al(NO3)3 (vs mole of graphite) could bring about a smooth Al2O3 coating layer with proper thickness, which could act as a preformed solid electrolyte interface (SEI) to reduce the regeneration of SEI and lithium-ions consumption during subsequent cycling. Furthermore, we examined the advantages of Al2O3 coating by relating energy levels in LIBs using density functional theory calculations. Owing to its proper bandgap and lithium-ion conduction ability, the coating layer performs the same function as a SEI does, preventing an electron from getting to the outer electrode surface and allowing lithium-ion transport. Therefore, as a preformed SEI, the Al2O3 coating layer reduces extra cathode consumption observed in commercial LIBs.

Electrode materials and electrolytes play a vital role in device-level performance of rechargeable Li-ion batteries (LIBs). However, electrode structure/component degeneration and electrode-electrolyte sur-/interface evolution are identified as the most crucial obstacles in practical applications. Thanks to its congenital advantages, atomic layer deposition (ALD) methodology has attracted enormous attention in advanced LIBs. This review mainly focuses upon the up-to-date progress and development of the ALD in high-performance LIBs. The significant roles of the ALD in rational design and fabrication of multi-dimensional nanostructured electrode materials, and finely tailoring electrode-electrolyte sur-/interfaces are comprehensively highlighted. Furthermore, we clearly envision that this contribution will motivate more extensive and insightful studies in the ALD to considerably improve Li-storage behaviors. Future trends and prospects to further develop advanced ALD nanotechnology in next-generation LIBs were also presented.

Polymer electrode materials (PEMs) have become a hot research topic for lithium-ion batteries (LIBs) owing to their high energy density, tunable structure, and flexibility. They are regarded as a category of promising alternatives to conventional inorganic materials because of their abundant and green resources. Currently, conducting polymers, carbonyl polymers, radical polymers, sulfide polymers, and imine polymers as five kinds of PEMs are studied extensively. This review introduces the latest research progress of PEMs for LIBs from the perspectives of molecular structure, redox mechanism, and electrochemical performance. The synthesis mechanisms and methods are outlined to guide the future design of PEMs. However, the practical application of PEMs is limited by their insufficient conductivity, structural instability, and high solubility. Aiming at these obstacles, reasonable optimization strategies are discussed, including the modification of molecular structure, the control of micromorphology, and the composite of carbon materials. Finally, the development trends and prospects of PEMs are put forward.