路易斯酸位铝促进的 CoAl2O4/CoO 电催化剂用于高效电化学生产 H2O2 以实现现场污染物降解,ACS Sustainable Chemistry & Engineering

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路易斯酸位铝促进的 CoAl2O4/CoO 电催化剂用于高效电化学生产 H2O2 以实现现场污染物降解
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-12-21 , DOI: 10.1021/acssuschemeng.3c05426
Suqin Wu ₁ , Daijie Deng ₁ , Jian-Chun Wu _{1,

2} , Linhua Zhu ₃ , Cheng Yan ₄ , Li Xu ₁ , Henan Li ₁

Affiliation

双氧水（H ₂ O ₂）作为一种环保化工材料，可用于环境修复领域去除水污染物。电化学二电子氧还原反应是一种环保、经济、安全的生产H ₂ O ₂的方法。然而，2电子过程的选择性难以控制。本文通过程序加热双金属CoAl层状双氢氧化物合成了CoAl ₂ O _{4 /CoO电催化剂。}密度泛函理论计算表明，Lewis酸位Al可以调节Co活性位点的电子结构，从而降低2电子氧还原反应途径的吉布斯自由能垒。_{因此，CoAl 2} O ₄ /CoO催化剂上的氧还原反应可以通过2电子途径进行。因此，CoAl ₂ O ₄ /CoO催化剂在0.2-0.6 V电压范围内的H ₂ O _{2选择性在0.1 M KOH中在1600 rpm时达到85%，在400 rpm时达到94%，并且具有优异的稳定性。}CoAl ₂ O ₄ /CoO催化剂的H ₂ O ₂产率可达1.446 mol h ^–1 g ^–1。_{CoAl 2} O ₄ /CoO对10 mg L ^–1罗丹明B（RhB）溶液的降解率也可以在110 min内达到100%。_{这种路易斯酸位点活化策略为设计具有高H 2} O ₂选择性的双金属氧化物电催化剂提供了合理的方法，可用于污染物的现场降解。

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Lewis Acid Site Al-Promoted CoAl2O4/CoO Electrocatalyst for Efficient Electrochemical Production of H2O2 toward On-Site Pollutant Degradation

As an environmentally friendly chemical material, hydrogen peroxide (H₂O₂) can be used in the field of environmental remediation to remove water pollutants. The electrochemical 2-electron oxygen reduction reaction is an environmentally friendly, economical, and safe method to produce H₂O₂. However, the selectivity of the 2-electron process is difficult to control. Herein, a CoAl₂O₄/CoO electrocatalyst was synthesized by programmed heating bimetallic CoAl-layered double hydroxide. Density functional theory calculations reveal that the Lewis acid site Al can regulate the electronic structure of the Co active site, thereby reducing the Gibbs free energy barrier of the 2-electron oxygen reduction reaction pathway. Thus, the oxygen reduction reaction on the CoAl₂O₄/CoO catalyst can be carried out through the 2-electron pathway. Consequently, the H₂O₂ selectivity of the CoAl₂O₄/CoO catalyst at the voltage range of 0.2–0.6 V can reach 85% at 1600 rpm and 94% at 400 rpm in 0.1 M KOH with excellent stability. The H₂O₂ yield of the CoAl₂O₄/CoO catalyst can reach 1.446 mol h^–1 g^–1. The degradation rate of CoAl₂O₄/CoO to 10 mg L^–1 rhodamine B (RhB) solution also can reach 100% within 110 min. This Lewis acid site activation strategy provides a reasonable method to design bimetallic oxide electrocatalysts with high H₂O₂ selectivity, which can be used for on-site degradation of pollutants.

更新日期：2023-12-21

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