电化学
传质
化学工程
化学
人体净化
电催化剂
润湿
接触角
电极
材料科学
色谱法
物理化学
物理
工程类
核物理学
作者
Zhun Fan,Huachao Zhao,Kaifeng Wang,Ran Wei,Jingbo Sun,Jingfu Liu,Rui Liu
标识
DOI:10.1021/acs.est.2c07462
摘要
Electrochemical reduction (ER) is a promising approach to safely remove pollutants. However, sluggish reaction kinetics and significant side reactions considerably limit the applicability of this green process. Herein, we uncovered the previously ignored role of interfacial hydrophilicity in determining the ER performance through electron microscopy observations, contact angle (CA) analysis, and electrochemical measurements. A Pd/C electrocatalyst forms dense nanopores on the electrode surface, rendering it highly hydrophobic and achieving a CA of up to 145°. This imposes a large mass-transfer barrier for the diffusion of water and pollutants into Pd sites. Moreover, the release of H2 is suppressed, which changes the solid–liquid (Pd–polluted water) interface into a solid–gas (H2)–liquid interface. This further slows down mass transfer and the decontamination process. This dilemma can be easily alleviated by adding hydrophilic polymers like polyethylene glycol to increase hydrophilicity and improve mass transfer. By this way, the activity and Faraday efficiency of Pd/C in the electrochemical hydrodehalogenation of 2,4-dichlorophenol could be increased by 4–5 times. Moreover, this interfacial microenvironment modulation strategy is parallel to other approaches, such as Pd structural engineering, and therefore these strategies can be combined to further increase the electrochemical decontamination performance of electrocatalysts.
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