贺泓院士领衔!南昌大学余运波/生态环境研究中心刘智/赣江创新研究院鄢勇:从溶剂选择到催化性能:重新定义羟基介导结构工程中的洗涤步骤

（点击文末“阅读原文”，可直达原文链接）

This work redefines the washing step in conventional precipitation synthesis, elevating it from a routine purification procedure to a decisive handle for engineering the microstructure of heterogeneous catalysts. Beyond merely preserving texture, we find that replacing water with ethanol induces a critical chemical effect: it selectively stabilizes hydroxyl groups in the zirconium hydroxide precipitate. This modification initiates a deterministic structural evolution: it directs the formation of phase-pure monoclinic ZrO₂ upon calcination, which subsequently templates the assembly of supported PdO nanoparticles enriched with active edge/step sites at twin boundaries. The resulting Architecture-arising from this tailored precursor chemistry-simultaneously enhances C−H activation and water tolerance, endowing Pd/ZrO₂ with exceptional low-temperature activity and sustained durability for methane oxidation. The generality of this approach, rooted in hydroxyl-chemistry control, is demonstrated by its successful extension to CeO₂ and TiO₂ supports, where ethanol washing similarly refines the microstructure and enriches PdO edge/step sites, thereby boosting methane oxidation activity. Its broad applicability is further validated by the consistently superior CO oxidation performance across all ethanol-washed catalysts. Consequently, our work establishes a general design paradigm wherein solvent selection during post-precipitation washing serves as a primary, chemical, scalable lever for the precise construction of high-performance catalytic architectures.

要点1. 本文研究发现，用乙醇替代水进行洗涤不仅仅是保留织构性质，还会引发关键的化学效应：它选择性地稳定了氢氧化锆沉淀中的羟基基团。这一改性引发了决定性的结构演化：在煅烧过程中导向形成纯相单斜ZrO₂，进而以此为模板，组装得到富含孪晶边界处活性边/台阶位点的负载型PdO纳米颗粒。这种源于前驱体化学裁剪的独特结构，同时增强了C-H键活化和耐水性，赋予Pd/ZrO₂在甲烷氧化反应中优异的低温活性和持久稳定性。

要点2. 该方法基于羟基化学调控的普适性，已成功拓展至CeO₂和TiO₂载体：乙醇洗涤同样细化了其微观结构并富集了PdO边/台阶位点，从而提升了甲烷氧化活性。所有经乙醇洗涤的催化剂在CO氧化反应中均表现出持续优越的性能，进一步验证了该方法的广泛适用性。

要点3. 本工作建立了一个通用的设计范式，即后沉淀洗涤过程中的溶剂选择可作为一项首要的、化学层面的、可规模化的杠杆，用于精确构筑高性能催化结构。

Min Xiao, Zidi Yan, Tiancheng Fang, Yanshuang Zhang, Zhi Liu,* Yong Yan,* Yunbo Yu,* and Hong He. From Solvent Choice to Catalytic Performance: Redefining the Washing Step for Hydroxyl-Mediated Architecture Engineering. J. Am. Chem. Soc. 2026.

DOI: 10.1021/jacs.6c03484

https://doi.org/10.1021/jacs.6c03484

（点击文末“阅读原文”，可直达原文链接）

往期推荐