<br>H2转移方法对于全氟辛酸（PFOA）催化加氢脱氟至关重要,Environmental Science & Technology

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H2转移方法对于全氟辛酸（PFOA）催化加氢脱氟至关重要
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2024-01-02 , DOI: 10.1021/acs.est.3c07650
Min Long ₁ , Yu Chen _{2,

3} , Thomas P Senftle _{2,

3} , Welman Elias _{2,

3} , Kimberly Heck _{2,

3} , Chen Zhou _{4,

5} , Michael S Wong _{2,

3} , Bruce E Rittmann ₆

Affiliation

H ₂的有效转移在催化氢化中起着至关重要的作用，特别是对于从水中去除顽固污染物而言。最持久的污染物之一全氟辛酸（PFOA）被用来研究H ₂转移方法如何影响元素钯纳米颗粒（Pd ⁰ NPs）的催化加氢脱氟能力。 Pd ⁰ NPs是通过膜中H ₂驱动的Pd ²⁺原位自催化还原合成的。 Pd ⁰纳米粒子直接沉积在膜纤维上形成催化剂膜。与通过顶部空间输送H ₂相比，通过无孔气体传输膜的壁将H ₂直接输送至Pd ⁰ NP增强了PFOA的加氢脱氟。较高的H ₂流明压力（20 vs 5 psig）也显着增加了脱氟速率，尽管5 psig H ₂通量足以使PFOA完全还原脱氟。使用密度泛函理论(DFT)进行的计算表明，与通过顶部空间输送的H ₂相比，直接从膜输送的地下氢通过在Pd ⁰ NP催化剂上产生更高的活性氢物种覆盖率来增加并加速加氢脱氟。这项研究记录了 H ₂转移方法在 PFOA 催化加氢中的关键作用，并提供了膜传输如何加速加氢脱氟的机制见解。

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Method of H2 Transfer Is Vital for Catalytic Hydrodefluorination of Perfluorooctanoic Acid (PFOA)

The efficient transfer of H₂ plays a critical role in catalytic hydrogenation, particularly for the removal of recalcitrant contaminants from water. One of the most persistent contaminants, perfluorooctanoic acid (PFOA), was used to investigate how the method of H₂ transfer affected the catalytic hydrodefluorination ability of elemental palladium nanoparticles (Pd⁰NPs). Pd⁰NPs were synthesized through an in situ autocatalytic reduction of Pd²⁺ driven by H₂ from the membrane. The Pd⁰ nanoparticles were directly deposited onto the membrane fibers to form the catalyst film. Direct delivery of H₂ to Pd⁰NPs through the walls of nonporous gas transfer membranes enhanced the hydrodefluorination of PFOA, compared to delivering H₂ through the headspace. A higher H₂ lumen pressure (20 vs 5 psig) also significantly increased the defluorination rate, although 5 psig H₂ flux was sufficient for full reductive defluorination of PFOA. Calculations made using density functional theory (DFT) suggest that subsurface hydrogen delivered directly from the membrane increases and accelerates hydrodefluorination by creating a higher coverage of reactive hydrogen species on the Pd⁰NP catalyst compared to H₂ delivery through the headspace. This study documents the crucial role of the H₂ transfer method in the catalytic hydrogenation of PFOA and provides mechanistic insights into how membrane delivery accelerates hydrodefluorination.

更新日期：2024-01-02

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