Although Pt has been verified as the most active catalyst for hydrogen production, it is highly desirable to minimize the usage of Pt while boost the catalytic performance of catalysts considering the low availability and high price of Pt. Herein, we propose a morphology and surface-electronic-structure reconstruction strategy to realize the anchoring of Pt nanoparticles (NPs) on Co₃O_4-δ-carbon matrix via the co-reduction of Pt precursor and Co₃O₄-carbon formed by direct pyrolysis of an aerogel composed of cobalt nitrate, chitosan, and urea. The transformation of the porous-network to hierarchically porous structure consisted of Co₃O_4-δ-carbon nanosheets, deposition of electron-rich Pt NPs, and generation of abundant oxygen-vacancy are facilely achieved through flexible co-reduction of Pt(IV) ions and Co₃O₄-carbon with ammonia borane (AB). The achieved Pt/Co₃O_4-δ-UC with an ultralow Pt loading (0.1 wt%) exhibits an ultrahigh activity for hydrolytic AB dehydrogenation with turnover frequencies of 7700 min⁻¹ in aqueous solution at 25 ℃. This catalyst also has a high durability with 71.3% remained activity after ten repetitive cycles. The morphology and surface-electronic-structure reconstruction engaged formation of electron-efficient Pt species could accelerate the oxidative cleavage of O − H bond in H₂O and greatly boost the hydrogen generation from hydrolytic AB dehydrogenation. This strategy presented herein offers a new pathway for constructing ultra-highly active supported metal NPs toward hydrogen evolution reaction.

尽管 Pt 已被证实是最活跃的制氢催化剂，但考虑到 Pt 的低可用性和高价格，在提高催化剂催化性能的同时尽量减少 Pt 的使用是非常可取的。在此，我们提出了一种形态和表面电子结构重建策略，通过 Pt 前体和形成的 Co ₃ O ₄ -碳的共还原来实现 Pt 纳米粒子 (NPs) 在 Co ₃ O _{4-δ -}碳基体上的锚定。通过直接热解由硝酸钴、壳聚糖和尿素组成的气凝胶。多孔网络向分级多孔结构的转变由 Co ₃ O _{4-δ组成通过 Pt(IV) 离子和 Co 3} O ₄ -碳与氨硼烷 (AB)的灵活共还原，可以轻松实现 - 碳纳米片、富电子 Pt NPs 的沉积和大量氧空位的产生。所获得的Pt/Co ₃ O _4-δ -UC 具有超低Pt 负载量（0.1 wt%），在25 ℃的水溶液中表现出超高的水解AB 脱氢活性，转换频率为7700 min ^{-1 。}该催化剂还具有高耐久性，在十次重复循环后仍保持 71.3% 的活性。形态和表面电子结构重建参与了电子高效 Pt 物种的形成，可以加速 H _{2中 O - H 键的氧化裂解}O 并大大促进水解 AB 脱氢产生的氢气。本文提出的这一策略为构建用于析氢反应的超高活性负载金属纳米粒子提供了一条新途径。