The discord between the insufficient abundance and the excellent electrocatalytic activity of Pt urgently requires its atomic-level engineering for minimal Pt dosage yet maximized electrocatalytic performance. Here we report the design of ultrasmall triphenylphosphine-stabilized Pt6 nanoclusters for electrocatalytic hydrogen oxidation reaction in alkaline solution. Benefiting from the self-optimized ligand effect and atomic-precision structure, the nanocluster electrocatalyst demonstrates a high mass activity, a high stability, and outperforms both Pt single atoms and Pt nanoparticle analogues, uncovering an unexpected size optimization principle for designing Pt electrocatalysts. Moreover, the nanocluster electrocatalyst delivers a high CO-tolerant ability that conventional Pt/C catalyst lacks. Theoretical calculations confirm that the enhanced electrocatalytic performance is attributable to the bifold effects of the triphenylphosphine ligand, which can not only tune the formation of atomically precise platinum nanoclusters, but also shift the d-band center of Pt atoms for favorable adsorption kinetics of *H, *OH, and CO.

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As an emerging post-lithium battery technology, aluminum ion batteries (AIBs) have the advantages of large Al reserves and high safety, and have great potential to be applied to power grid energy storage. But current graphite cathode materials are limited in charge storage capacity due to the formation of stage-4 graphite-intercalated compounds (GICs) in the fully charged state. Herein, we propose a new type of cathode materials for AIBs, namely polycyclic aromatic hydrocarbons (PAHs), which resemble graphite in terms of the large conjugated π bond, but do not form GICs in the charge process. Quantum chemistry calculations show that PAHs can bind AlCl 4À through the interaction between the conjugated π bond in the PAHs and AlCl 4 À , forming onplane interactions. The theoretical specific capacity of PAHs is negatively correlated with the number of benzene rings in the PAHs. Then, under the guidance of theoretical calculations, anthracene, a three-ring PAH, was evaluated as a cathode material for AIBs. Electrochemical measurements show that anthracene has a high specific capacity of 157 mAh g À 1 (at 100 mA g À 1 ) and still maintains a specific capacity of 130 mAh g À 1 after 800 cycles. This work provides a feasible "theory guides practice" research model for the development of energy storage materials, and also provides a new class of promising cathode materials for AIBs.

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Rechargeable aluminum-ion batteries (RAIBs) are highly sought after due to the extremely high resource reserves and theoretical capacity (2980 mA h/g) of metal aluminum. However, the lack of ideal cathode materials restricts its practical advancement. Here, we report a conductive polymer, polyphenylene, which is produced by the polymerization of molecular benzene as a cathode material for RAIBs with an excellent electrochemical performance. In electrochemical redox, polyphenylene is oxidized and loses electrons to form radical cations and intercalates with [AlCl4]− anion to achieve electrical neutrality and realize electrochemical energy storage. The stable structure of polyphenylene makes its discharge specific capacity reach 92 mA h/g at 100 mA/g; the discharge plateau is about 1.4 V and exhibits an excellent rate performance and long cycle stability. Under the super high current density of 10 A/g (∼85 C), the charging can be completed in 25 s, and the capacities have almost no decay after 30,000 cycles. Aluminum polyphenylene batteries have the potential to be used as low-cost, easy-to-process, lightweight, and high-capacity superfast rechargeable batteries for large-scale stationary power storage.