通过电化学产生的过氧化氢和原子氢的反应产生羟基自由基：污染物氧化的有效过程？,Environmental Science & Technology

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通过电化学产生的过氧化氢和原子氢的反应产生羟基自由基：污染物氧化的有效过程？
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-04-20 , DOI: 10.1021/acs.est.2c00405
Yang Li ₁ , Christopher J Miller ₂ , Lei Wu _{1,

2} , T David Waite _{1,

2}

Affiliation

使用能够同时催化析氢反应 (HER) 和氧还原反应 (ORR) 的催化阴极展示了电化学高级氧化过程 (EAOP)，从而原位产生原子氢 (H*) 和过氧化氢 (H ₂ O ₂ )。钯包覆的碳-PTFE 气体扩散电极 (Pd/C GDE) 用作催化阴极，羟基自由基 ( ^• OH) 是由电生成的 H* 与 H ₂ O ₂反应形成的。由于 HER 和 ORR 都可以被诱导在同一阴极发生，因此与传统的 H*/H ₂ O相比，H*/GDE 工艺可以更有效地降解有机污染物₂过程涉及直接添加 H ₂ O ₂。在中性 pH 值下，在 -1.0 V vs Ag/AgCl 的施加电位下处理 2 小时后，82.7% 的添加甲酸盐降解，生成的 H ₂ O ₂残留在溶液中的浓度相对较低。我们还表明，H* 和 H ₂ O ₂（以及因此^• OH）可以在很宽的 pH 值范围（3.2-7.0）内有效地电生成。这些结果表明，通过原位生成 H* 和 H ₂ O ₂，H*/GDE 工艺能够产生大量的^•OH 无需外部化学添加，因此提供了一种减少水性有机污染物的替代方法。

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Hydroxyl Radical Production via a Reaction of Electrochemically Generated Hydrogen Peroxide and Atomic Hydrogen: An Effective Process for Contaminant Oxidation?

An electrochemical advanced oxidation process (EAOP) is demonstrated with a catalytic cathode capable of simultaneously catalyzing the hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR) with resultant in situ generation of atomic hydrogen (H*) and hydrogen peroxide (H₂O₂). A palladium-coated carbon-PTFE gas diffusion electrode (Pd/C GDE) was used as a catalytic cathode with hydroxyl radical (^•OH) formed as a result of the reaction of electrogenerated H* with H₂O₂. As both the HER and ORR can be induced to occur at the same cathode, the H*/GDE process results in more effective degradation of organic contaminants than can be achieved by a conventional H*/H₂O₂ process involving direct addition of H₂O₂. At circumneutral pH, 82.7% of added formate was degraded after 2 h treatment at an applied potential of −1.0 V vs Ag/AgCl with relatively low concentrations of generated H₂O₂ remaining in the solution. We also show that H* and H₂O₂ (and thus ^•OH) can be electrogenerated effectively over a wide range of pH (3.2–7.0). These results suggest that by in situ generation of H* and H₂O₂, the H*/GDE process is able to produce significant amounts of ^•OH without external chemical addition and thus offers an alternative method for abatement of aqueous organic contaminants.

更新日期：2022-04-20

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