Modulating Pt States through Hydroxyl Control for Low-Temperature Aqueous Phase Reforming of Methanol

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-03-26 DOI:10.1021/acscatal.5c00357

Yuyao Yang, Xuan Bie, Xiaoying Qi, Yongqing Xu, Qinghai Li, Yanguo Zhang, Hui Zhou

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引用次数: 0

Abstract

Aqueous phase reforming of methanol (APRM) offers a method for releasing H₂ from the liquid phase, by which H₂ can be stored in methanol safely. It is an efficient way to design high-performance catalysts by controlling the hydroxyl (OH) groups, but its mechanism for affecting the APRM is still unclear. Herein, we loaded Pt on three types of Al₂O₃ (nanopolyhedron, nanosheet, and nanorod Al₂O₃) with different OH contents and types. Among them, Pt/nanorod Al₂O₃ exhibited the highest H₂ production rate of 20.4 μmol g^–1 s^–1 with 96.6% H₂ selectivity at a low temperature of 190 °C. This was attributed to the roles of hydroxyl groups in modulating Pt states. On nanopolyhedron, nanosheet, and nanorod Al₂O₃, the bonding of Pt with O atoms became more favorable as the dehydroxylation happened. In particular, on nanorod Al₂O₃, the dehydroxylation process generated a high density of five-coordinated Al (Al_V) sites, facilitating the dispersion and anchoring of Pt particles. Moreover, the special OH groups (hydrogen bond donor) on nanorod Al₂O₃ promoted Pt particle reduction via the movement of electrons. Ultimately, the results demonstrated the influence of OH groups on the dispersion and reduction of active metals, offering perspectives for designing catalysts for APRM through hydroxyl control.

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甲醇的水相重整（APRM）提供了一种从液相中释放 H2 的方法，通过这种方法可以将 H2 安全地储存在甲醇中。通过控制羟基（OH）来设计高性能催化剂是一种有效的方法，但其影响 APRM 的机理尚不清楚。在此，我们将铂负载在三种具有不同羟基含量和类型的 Al2O3（纳米多面体、纳米片和纳米棒 Al2O3）上。其中，铂/纳米棒 Al2O3 在 190 ℃ 的低温下表现出最高的 H2 产率（20.4 μmol g-1 s-1）和 96.6% 的 H2 选择性。这归因于羟基在调节铂态中的作用。在纳米多面体、纳米片和纳米棒状 Al2O3 上，随着脱羟基作用的发生，铂与 O 原子的结合变得更加有利。特别是在纳米棒 Al2O3 上，脱羟基过程产生了高密度的五配位 Al（AlV）位点，有利于铂粒子的分散和锚定。此外，纳米棒 Al2O3 上的特殊 OH 基团（氢键供体）通过电子移动促进了铂粒子的还原。最终，研究结果证明了羟基对活性金属的分散和还原的影响，为通过羟基控制设计 APRM 催化剂提供了前景。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.