利用无金属碳纳米管螺纹氧化g-C3N4光耦合电催化氧还原成过氧化氢

Qiong Zhu, Jinchen Fan, Yingle Tao, Huan Shang, Jingcheng Xu, Dieqing Zhang, Guisheng Li, Hexing Li
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引用次数: 8

摘要

过氧化氢(H2O2)在环境清洁、医院消毒和化工等领域有着广泛的应用。与传统的蒽醌氧化方法相比,电催化双电子氧还原反应(2e-ORR)生产H2O2因其绿色、安全、可靠而成为一种很有前途的替代方法。然而,由于4e-ORR与H2O的竞争性反应,其反应动力学缓慢,选择性低,限制了其工业应用。本文制备了一种基于氧化g-C3N4/碳纳米管(OCN/CNTs)的新型光响应性无金属电催化剂,并引入外部光场,实现了高性能电催化2e-ORR生成H2O2。令人印象深刻的是,OCN/CNT电催化剂的H2O2产率为30.7 mmol/gcat/h,法拉第H2O2效率高达95%。OCN/CNTs的含氧基团促进了氧中间体的吸附,光耦合电催化同时提高了电子传递效率和电催化选择性。
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Photo-coupled electrocatalytic oxygen reduction to hydrogen peroxide using metal-free CNT-threaded oxidized g-C3N4
Hydrogen peroxide (H2O2) has been widely used in environmental cleaning, hospital disinfecting and chemical engineering. Compared to the traditional anthraquinone oxidation method, the electrocatalytic two-electron oxygen reduction reaction (2e-ORR) to produce H2O2 has become a promising alternative due to its green, safety and reliability. However, its industrial application is still limited by the slow reaction kinetics and low selectivity due to the competitive reaction of the 4e-ORR to H2O. Herein, we prepare a novel photoresponsive metal-free electrocatalyst based on oxidized g-C3N4/carbon nanotubes (OCN/CNTs) and introduce an external light field to realize the high-performance electrocatalytic 2e-ORR to produce H2O2. Impressively, the OCN/CNT electrocatalyst exhibits an outstanding H2O2 productivity of 30.7 mmol/gcat/h with a high faradaic H2O2 efficiency of 95%. The oxygen-containing groups of the OCN/CNTs promote the adsorption of oxygen intermediates and the photo-coupled electrocatalysis simultaneously improves the electron transport efficiency and enhances the electrocatalytic selectivity.
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