阳极电氧化抗坏血酸耦合制氢的催化剂设计与性能研究

       氢能是一种高能量密度，环境友好的能源。电催化水分解制氢技术由可再生的电能驱动， 一种十分环保的氢能制取方法。但是电解水过程中阳极的析氧反应（Oxygen Evolution Reaction， OER）是一个复杂的四电子过程，极大地限制了电解水产氢效率。从热力学角度上，生物质材料的氧化电位低于水的分解电位，有着代替 OER 过程实现低电压大电流产氢的潜力。
       本文设计了一种新的电化学产氢体系，在阳极采用氧化抗坏血酸反应代替OER。并且针对该体系，开发出高熵合金催化剂用于电催化抗坏血酸氧化耦合制氢。在该催化剂作用下，阳极半反应仅需施加 0.5 V 的电压即可实现 10 mA cm^-2 的电流密度，远低于 OER 反应的理论电位（1.23 V）。进一步地，采用高温烧结的方法制备出单原子 Fe 催化剂，用于阳极氧化抗坏血酸制氢体系。在该催化剂的作用下，抗坏血酸氧化反应达到 10 mA cm^-2 的过电势仅有 12 mV，因而在室温下施加 0.75V 的电压即可达到 1 A cm^-2 的电流密度。红外光谱和核磁共振氢谱等测试结果表明，阳极反应产物仅有脱氢抗坏血酸，且阴极产氢的法拉第效率接近 100%。理论计算指出，单原子 Fe 为该反应的催化活性位点，其在费米能级展现出高电子态且在 Fe-3d 轨道和抗坏血酸中 O-2p 轨道之间有很强的电子杂化，这使得单原子 Fe 展现出高的氧化活性。为证明这一体系的实用性，本文在两电极的电解槽装置中测试了电化学制氢性能。结果表明，该体系在 60 ℃下仅需 1.1 V 便可达到 2 A cm^-2 的电流密度，其制氢电耗只有电解纯水的一半左右。
       本论文开发的电化学产氢体系不仅可以大幅度降低电压，在阳极还可以生产有价值的副产物，提高体系的经济价值。该体系推动了电化学氧化生物质材料耦合制氢的发展，同时也为解决电解水制氢电耗高、阳极产物价值低等难题提供了新的解决思路。

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