1673-159X

CN 51-1686/N

基于3,4-二氨基呋咱氧化偶氮反应的低能耗电解水制氢耦合体系

The Low-energy Consumption Hydrogen Production Coupling System for Water Electrolysis Based on the Oxidation Azo Reaction of 3,4-diaminofurazan

  • 摘要: 动力学较慢、产物经济价值低的氧析出反应(OER)使电解水制氢总反应能量转换效率和实际应用的经济效益严重降低,因此,选用电位较低、价值较高的氧化反应代替OER能够有效降低制氢槽电压和能耗,提升能量转换效率,同时可以得到高附加值的化工产品。文章建立一种基于3,4-二氨基呋咱氧化偶氮反应的低能耗电解水制氢新型耦合体系,采用碳布负载NiS2催化剂(CC@NiS2)作为阴极氢析反应催化剂,利用氧化铜纳米催化剂驱动阳极反应,实验测试与分析结果表明,该体系驱动10 mA·cm–2的电流密度仅需1.45 V槽电压,比传统水电解体系(1.78 V)降低了330 mV。其中,碳布负载NiS2催化剂作为阴极氢析反应催化剂只需190.5 mV的过电位即可稳定运行20 h以上,驱动电流密度为10 mA·cm−2;同时,阳极可实现电合成3、3'-二氨基-4、4'-偶氮呋咱含能材料,在氧化铜纳米催化剂的驱动下,避免了在常规有机合成中出现的高危险、高污染、高成本等问题。该研究为安全生产含能有机化合物和低能耗绿色制备高纯氢气提供了一种新策略。

     

    Abstract:
    The oxygen evolution reaction (OER), which has a slow kinetics and low economic value of the product, seriously reduces the energy conversion efficiency of the overall water electrolysis for hydrogen production and the economic benefits of its practical applications. Therefore, replacing OER with an oxidation reaction that has a lower potential and higher value can effectively reduce the cell voltage and energy consumption for hydrogen production, improve the energy conversion efficiency, and at the same time obtain high-value-added chemical products.
    This paper establishes a new low-energy-consumption water electrolysis for hydrogen production coupling system based on the oxidative azo coupling reaction of 3,4-diaminofurazan. The specific method is to use a carbon cloth-supported NiS2 catalyst(CC@NiS2) as the cathode hydrogen evolution reaction catalyst and utilize a copper oxide nanocatalyst to drive the anode reaction, thereby constructing the entire coupling system and conducting relevant experimental tests and analyses.
    This system only requires a cell voltage of 1.45 V to drive a current density of 10 mA·cm−2, which is 330 mV lower than that of the traditional water electrolysis system (1.78 V). Among them, the carbon cloth-supported NiS2 catalyst as the cathode hydrogen evolution reaction catalyst can stably operate for more than 20 hours with an overpotential of only 190.5 mV when driving a current density of 10 mA·cm−2. Meanwhile, the anode can achieve the electrosynthesis of 3,3'-diamino-4,4'-azofurazan energetic materials. Driven by the copper oxide nanocatalyst, problems such as high danger, high pollution, and high cost that occur in conventional organic synthesis are avoided. This paper provides a new strategy for the safe production of energetic organic compounds and the low-energy-consumption and green preparation of high-purity hydrogen.

     

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