Azide molecule mediated electrolyte engineering for selective photoelectrochemical azo coupling and efficient and stable water splitting,Journal of Materials Chemistry A

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Azide molecule mediated electrolyte engineering for selective photoelectrochemical azo coupling and efficient and stable water splitting
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-07-14 , DOI: 10.1039/d2ta04559a
Shutao Li ₁ , Min Li ₂ , Fang Chen ₁ , Hongwei Huang ₁

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Low-performance and instability severely limit photoelectrochemical (PEC) water splitting and organic synthesis of photoanodes. Electrolyte regulation as a facile and scalable route receives less attention, and always requires oxygen evolution catalysts (OECs). Herein, we report azide molecule mediated electrolyte regulation to achieve OEC-free selective PEC reactions over a BiVO₄ (BVO) photoanode. pH-sensitive 5-aminotetrazolium (5AT) acts as not only a substrate for the PEC azo coupling reaction but also a “liquid phase cocatalyst” to substantially facilitate charge transfer at the photoanode-electrolyte interface. In 5AT/Na₂SO₄ electrolyte, the azo coupling reaction occurs at pH > 4, whereas the water splitting reaction takes place at pH < 4, and polyaniline passivated BVO (BVO-PANI) exhibits a photocurrent density of 4.22 mA cm⁻² at 1.23 V_RHE with an onset potential of 0.34 V_RHE and stable photocurrent density for 4 h. Meanwhile, 5AT as a “liquid phase cocatalyst” is universal for a variety of photoanodes, such as α-Fe₂O₃. Further, 5AT/NaVO₃/Na₂SO₄ ternary electrolyte solution allows BVO-PANI to exhibit a photocurrent density of 5.1 mA cm⁻² at 1.23 V_RHE with an onset potential of 0.27 V_RHE and stable PEC performance for 10 h. This work opens up a new avenue of electrolyte regulation to promote PEC performance and stability of photoanodes.

中文翻译：

叠氮化物分子介导的电解质工程用于选择性光电化学偶氮偶联和高效稳定的水分解

低性能和不稳定性严重限制了光电化学 (PEC) 水分解和光阳极的有机合成。电解质调节作为一种简便且可扩展的途径受到的关注较少，并且总是需要析氧催化剂（OEC）。_{在此，我们报告了叠氮化物分子介导的电解质调节，以在 BiVO 4} (BVO) 光阳极上实现无 OEC 的选择性 PEC 反应。pH 敏感的 5-氨基四唑 (5AT) 不仅充当 PEC 偶氮偶联反应的底物，而且充当“液相助催化剂”，以显着促进光阳极 - 电解质界面处的电荷转移。在 5AT/Na ₂ SO ₄在电解质中，偶氮偶联反应在 pH > 4 时发生，而水分解反应在 pH < 4 时发生，聚苯胺钝化 BVO (BVO-PANI) 在 1.23 V RHE 下的光电流密度为4.22 mA _cm^-2电位为 0.34 V _RHE，光电流密度稳定 4 h。同时，5AT 作为“液相助催化剂”对于各种光阳极，如α-Fe ₂ O ₃是通用的。此外，5AT/NaVO ₃ /Na ₂ SO ₄三元电解质溶液使 BVO-PANI在 1.23 V _{RHE和 0.27 V}_RHE的起始电位下表现出 5.1 mA cm ^{-2的光电流密度}和稳定的 PEC 性能 10 小时。这项工作为电解质调节开辟了一条新途径，以提高光阳极的 PEC 性能和稳定性。

更新日期：2022-07-14

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