The aqueous-phase reforming of the methanol (APRM) reaction provides a potential approach for hydrogen (H₂) storage and transportation. However, the limited capacity of Pt nanocatalysts for H₂O activation leads to the drawback of requiring high reaction temperatures (>200 °C) to achieve efficient H₂ generation through the APRM reaction. Herein, the electronic density of Pt nanocatalysts has been regulated by the phase of the Al₂O₃ supports. Mechanism analysis revealed that the α-Al₂O₃ supports with larger lattice fringe spacing resulted in an enhanced electronic density of Pt nanocatalysts, thereby enabling the effective adsorption and activation of H₂O. Consequently, the Pt/α-Al₂O₃ catalysts exhibited a TOF value of 69.8 h^–1 at 30 °C for H₂ generation via APRM reaction. Notably, this H₂ generation rate even suppressed that achieved by previous state-of-the-art homogeneous catalysts. This finding presents a promising avenue toward flexible hydrogen utilization.

中文翻译：

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甲醇和水低温制氢的 Pt 的电子调节


甲醇 （APRM） 反应的水相重整为氢气 （H₂） 的储存和运输提供了一种潜在的方法。然而，Pt 纳米催化剂对 H₂O 活化的能力有限，导致需要高反应温度 （>200 °C） 才能通过 APRM 反应实现高效 H₂ 生成的缺点。在此，Pt 纳米催化剂的电子密度受 Al₂O₃ 载体相的调节。机理分析表明，具有较大晶格条纹间距的 α-Al₂O₃ 载体导致 Pt 纳米催化剂的电子密度增加，从而能够有效吸附和活化 H₂O。因此，Pt/α-Al₂O₃ 催化剂在 30 °C 下通过 APRM 反应生成 H₂ 的 TOF 值为 69.8 h^–1。值得注意的是，这种 H₂ 生成速率甚至抑制了以前最先进的均相催化剂所实现的速率。这一发现为灵活的氢利用提供了一条有前途的途径。