Au‐coverage‐dependent coordination engineering of PdAu catalysts for ambient direct synthesis of H 2 O 2 in pure water

IF 4.4 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2026-09-21 DOI:10.1002/aic.70658

Qian Wang, Linxing Xie, Jiacheng Xie, Yao Qin, Liwen Mu, Zengxi Wei, Shuangliang Zhao

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Abstract

Au alloying tunes Pd coordination to enhance selectivity for direct synthesis of H 2 O 2 (DSHP), but the structure–activity relationship remains unclear. We fabricated Pd@Au x core–shell catalysts with controlled Au coverage via H 2 purging and evaluated them in a microreactor under ambient conditions in pure water. H 2 O 2 formation shows a volcano‐shaped trend vs. Pd/Au ratio. The optimal Pd/Au≈1:1 gives 1785 ppm H 2 O 2 and a yield of 190.8 mol·kgcat −1 ·h −1 . DFT calculations reveal a similar volcano‐shaped trend for Au loading. Pd–Au 3 exhibits the lowest free energy for O 2 protonation to OOH (Δ G = −0.15 eV) and the highest barrier for the four‐electron side reaction (1.31 eV), achieving optimal activity and selectivity. This originates from a moderate d‐band center at −1.80 eV, lying in the Sabatier regime. This work provides insights into Au‐loading regulation on Pd, guiding rational catalyst design.

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PdAu催化剂在纯水环境下直接合成h2o2的Au覆盖依赖性配位工程

Au合金通过调节Pd配位来提高直接合成h2o2 （DSHP）的选择性，但构效关系尚不清楚。我们通过h2净化制备了具有可控Au覆盖的Pd@Au x核壳催化剂，并在纯水环境条件下的微反应器中对其进行了评价。h2o2地层与Pd/Au比值呈火山状变化趋势。在Pd/Au≈1:1的条件下，得到1785 ppm h2o2，产率为190.8 mol·kgcat−1·H−1。DFT计算显示了类似的火山状Au加载趋势。Pd-Au 3具有o2质子化成OOH的最低自由能（Δ G = - 0.15 eV）和四电子侧反应的最高势垒（1.31 eV），具有最佳的活性和选择性。这源于- 1.80 eV的中等d波段中心，位于Sabatier区。这项工作为钯上Au的负载规律提供了见解，指导了催化剂的合理设计。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

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