Highly efficient electrosynthesis of hydrogen peroxide through reversible transformation between catechol and o-benzoquinone on polydopamine modified carbon black

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2024-10-25 DOI:10.1016/j.cej.2024.157070

Yuexin Cui, Meng Qiao, Shen Zhao, Kaifeng Wang, Yi Liu, Hongshuai Kan, Xu Zhao

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引用次数: 0

Abstract

Carbon-based materials are more promising catalysts for H₂O₂ electrochemical production. However, the common method for modifying carbon-based materials is surface functionalization with harsh and uncontrollable reaction conditions, hindering the precise regulation of the active sites. Herein, we proposed a carbon-based material modified by polydopamine (CB-PDA) that was easily prepared and used in air diffusion electrode system for H₂O₂ production. The rapid and reversible transformation between catechol and o-benzoquinone on PDA could improve the H₂O₂ selectivity from 75.5 % to 97.0 % during the electrocatalytic process. The detection of adsorbed *HOOH and *OOH in oxygen reduction reaction proved the preference of CB-PDA for the two-electron pathway. The H₂O₂ formation rate constant of CB-PDA increased significantly from 25.85 to 60.82 mM h⁻¹. The highest cumulative H₂O₂ concentration could reach 10200 mg L⁻¹ in 9 h. Long-term operation tests proved the good operational stability. Furthermore, this system was cost-effective without additional aeration energy consumption and could achieve rapid disinfection in 10 min, which would have great potential to be used in environmental remediation.

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通过邻苯二酚和邻苯醌在聚多巴胺改性炭黑上的可逆转化高效电合成过氧化氢

碳基材料是更有前途的 H2O2 电化学生产催化剂。然而，常用的碳基材料改性方法是表面功能化，反应条件苛刻且不可控，阻碍了活性位点的精确调节。在此，我们提出了一种由多巴胺修饰的碳基材料（CB-PDA），该材料易于制备，可用于空气扩散电极系统生产 H2O2。儿茶酚与邻苯醌在 PDA 上的快速可逆转化可将电催化过程中的 H2O2 选择性从 75.5% 提高到 97.0%。在氧还原反应中检测吸附的 *HOOH 和 *OOH 证明了 CB-PDA 对双电子途径的偏好。CB-PDA 的 H2O2 生成速率常数从 25.85 mM h-1 显著增加到 60.82 mM h-1。最高累积 H2O2 浓度可在 9 小时内达到 10200 mg L-1。长期运行测试证明，该系统具有良好的运行稳定性。此外，该系统无需消耗额外的曝气能耗，成本效益高，可在 10 分钟内实现快速消毒，在环境修复方面具有很大的应用潜力。

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来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.