近日，厦门大学秦瑞轩团队实现了磷酸盐通过促进金属-载体界面上的质子/电子转移来促进催化加氢脱氧。2025年10月8日出版的《美国化学会志》发表了这项成果。

含氧化合物的催化加氢和脱氧在合成中起着至关重要的作用。尽管发展了许多氢脱氧（HDO）反应，但许多反应仍然依赖于化学计量还原剂，导致不良副产物和低原子效率。氢气已成为一种环保的替代品，但在温和条件下，其有效利用仍然具有挑战性。

在该研究中，Pt/TiO₂的直接磷酸修饰导致亚砜HDO活性显著提高约250倍。由于Ti–PO₄–Pt界面的存在，Pt/Ti(HPO₄)₂催化剂的产率比原始Pt/TiO₂高出280倍，超过了其他均相和异相催化剂的数量级。在原子尺度上阐明了配位不饱和Ti³⁺、界面磷酸盐和铂的关键作用，强调了界面上促进质子/电子转移的重要性。这项工作为可持续的催化加氢工艺提供了一种有前景的策略，在有机合成中具有广泛的适用性。

附：英文原文

Title: Phosphate Boosts Catalytic Hydrodeoxygenation by Facilitating Proton/Electron Transfer at the Metal–Support Interface

Author: Pengyao You, Liming Wu, Yazhou Zhang, Gang Fu, Lansun Zheng, Ruixuan Qin, Nanfeng Zheng

Issue&Volume: October 8, 2025

Abstract: Catalytic hydrogenation and deoxygenation of oxygenated compounds play an essential role in the synthesis. Despite the development of numerous hydrodeoxygenation (HDO) reactions, many reactions still rely on stoichiometric reducing agents, resulting in undesirable byproducts and a low atomic efficiency. H2 has emerged as an environmentally friendly alternative, but its efficient utilization remains challenging under mild conditions. In this study, the straightforward phosphate modification of Pt/TiO2 led to a remarkable ～250-fold enhancement in the sulfoxide HDO activity. Owing to the presence of the Ti–PO4–Pt interface, the Pt/Ti(HPO4)2 catalyst exhibited an impressive ～280 times higher productivity than pristine Pt/TiO2, surpassing other homogeneous and heterogeneous catalysts by orders of magnitude. The critical roles of coordinatively unsaturated Ti3+ sites, interfacial phosphate, and platinum were elucidated at the atomic scale, highlighting the significance of facilitated proton/electron transfer at the interface. This work offers a promising strategy for sustainable catalytic hydrogenation processes with broad applicability in organic synthesis.

DOI: 10.1021/jacs.5c09850

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c09850