The pH-dependant stabilization and interphase coupling of Pd species during alcohol oxidation

IF 48.3 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2026-06-04 DOI:10.1038/s41929-026-01547-2

Nouf Ali Alnahdi, Bohyeon Kim, Isaac T. Daniel, Samuel Pattisson, Mark Douthwaite, James Spragg, David J. Morgan, Thomas E. Davies, Alex Stenner, Stuart H. Taylor, Steven McIntosh, Graham J. Hutchings

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Abstract

Heterogeneous catalysts consistently suffer from the leaching of active components into the fluid phase, causing loss in activity and lifetime. Here we demonstrate, exemplified with the thermocatalytic oxidation of 1,2-propanediol, a metal stabilization mechanism arising from electrochemical coupling of half reactions between physically separated carbon-supported Au and Pd catalysts. When electrochemically coupled, polarization of each metal to an operating mixed potential occurs as a function of the Au:Pd molar ratio that, at pH 9–10, significantly reduces Pd leaching. At pH 14, where this stabilization no longer holds, we clearly show that an active redox mechanism can exist between disparate catalytic species in the liquid and solid phase, and that this leads to the cycling of Pd speciation as well as considerable enhancements in the rate of oxidation. Metal dissolution is a common cause for catalyst deactivation in heterogenous catalysis. Now, after mapping Pd speciation as a function of pH, a cooperative enhancement mechanism between separated Au/C and Pd/C catalysts and involving solid and dissolved Pd species is identified for alcohol oxidation.

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醇氧化过程中Pd物质的ph依赖性稳定和相间偶联

非均相催化剂一直受到活性成分浸出到流体相的影响，导致活性和寿命的损失。本文以1,2-丙二醇的热催化氧化为例，证明了金属稳定机制是由物理分离的碳负载的Au和Pd催化剂之间的半反应的电化学偶联引起的。当电化学耦合时，每种金属的极化到一个工作混合电位作为Au:Pd摩尔比的函数发生，在pH 9-10时，显著减少Pd浸出。在pH值为14时，这种稳定性不再成立，我们清楚地表明，在液相和固相中不同的催化物种之间可以存在活性氧化还原机制，这导致Pd物种的循环以及氧化速率的显著增强。金属溶解是多相催化中催化剂失活的常见原因。现在，在绘制了Pd形态随pH的函数图之后，我们确定了分离的Au/C和Pd/C催化剂之间的协同增强机制，并涉及固体和溶解的Pd形态。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.