接触起电在水-固界面产生 H2O2 的机理,Advanced Materials

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接触起电在水-固界面产生 H2O2 的机理
Advanced Materials ( IF 27.4 ) Pub Date : 2023-07-24 , DOI: 10.1002/adma.202304387
Andy Berbille _{1,

2} , Xiao-Fen Li _{1,

3} , Yusen Su _{1,

2} , Shunning Li ₄ , Xin Zhao ₁ , Laipan Zhu _{1,

2} , Zhong Lin Wang _{1,

2,

5,

6}

Affiliation

最近对水-固界面接触带电及其在物理化学过程中的作用的研究不断深入，人们认识到水-固接触带电过程中的电子转移可以驱动化学反应。这种机制称为接触电催化（CEC），允许化学惰性氟化聚合物发挥单电极电化学系统的作用。这项研究表明，使用氟化乙烯丙烯 (FEP) 作为催化剂，通过超声波驱动的 CEC，从空气和去离子水中生成过氧化氢 ( H ₂ O _{2 )。}当催化剂与溶液质量比为1:10000时，20℃下，H ₂ O ₂析出动力学速率达到58.87 mmol L ^-1 g _cat^-1 h ^-1。电子顺磁共振 (EPR) 显示，在超声处理过程中，带电 FEP 在溶液中发射出电子。EPR和同位素标记实验表明H ₂ O ₂是由CEC产生的羟基自由基(HO ^• )或两个超氧自由基(O ₂^•− )形成。最后，传统上认为此类自由基在反应前通过布朗扩散在溶液中迁移。然而，从头算分子动力学计算表明，自由基可以通过水的氢键网络交换质子和电子进行反应，即由于格罗特胡斯机制。_{该机制可与从空气和水中产生H 2} O ₂的其他人工或自然系统相关。

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Mechanism for Generating H2O2 at Water-Solid Interface by Contact-Electrification

The recent intensification of the study of contact-electrification at water-solid interfaces and its role in physicochemical processes lead to the realization that electron transfers during water-solid contact-electrification can drive chemical reactions. This mechanism, named contact-electro-catalysis (CEC), allows chemically inert fluorinated polymers to act like single electrode electrochemical systems. This study shows hydrogen peroxide (H₂O₂) is generated from air and deionized water, by ultrasound driven CEC, using fluorinated ethylene propylene (FEP) as the catalyst. For a mass ratio of catalyst to solution of 1:10000, at 20 °C, the kinetic rate of H₂O₂ evolution reaches 58.87 mmol L⁻¹ g_cat⁻¹ h⁻¹. Electron paramagnetic resonance (EPR) shows electrons are emitted in the solution by the charged FEP, during ultrasonication. EPR and isotope labelling experiments show H₂O₂ is formed from hydroxyl radicals (HO^•) or two superoxide radicals (O₂^•−) generated by CEC. Finally, it is traditionally believed such radicals migrate in the solution by Brownian diffusion prior to reactions. However, ab-initio molecular dynamic calculations reveal the radicals can react by exchanging protons and electrons through the hydrogen bonds network of water, i.e., owing to the Grotthuss mechanism. This mechanism can be relevant to other systems, artificial or natural, generating H₂O₂ from air and water.

更新日期：2023-07-24

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