Alkali Etching of Layered Double Hydroxide Nanosheets for Enhanced Photocatalytic N2 Reduction to NH3,Advanced Energy Materials

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Alkali Etching of Layered Double Hydroxide Nanosheets for Enhanced Photocatalytic N2 Reduction to NH3
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-07-26 , DOI: 10.1002/aenm.202002199
Yunxuan Zhao ₁ , Lirong Zheng ₂ , Run Shi _{1,

3} , Shuai Zhang _{1,

3} , Xuanang Bian _{1,

3} , Fan Wu _{1,

3} , Xingzhong Cao ₂ , Geoffrey I. N. Waterhouse ₄ , Tierui Zhang _{1,

3}

Affiliation

Layered double hydroxide (LDH) nanosheets show good activity in a wide range of photoreactions, with this activity being generally attributable to an abundance of surface oxygen vacancies or coordinatively unsaturated metal cations in the nanosheets which serve as active sites for reactant adsorption and activation. Recently, LDH nanosheets have been shown to be very effective for photocatalytic N₂ reduction to NH₃ using water as the reducing agent. Herein, it is demonstrated that a simple pretreatment of ZnCr‐LDH, ZnAl‐LDH, and NiAl‐LDH nanosheets with aqueous NaOH can greatly enhance the concentration of oxygen vacancies and low coordination metal centers in the nanosheets, thus significantly enhancing their photocatalytic activity for N₂ reduction to NH₃ under UV–vis irradiation (without the need for added sacrificial agents or cocatalysts). The facile alkali etching strategy introduced here is expected to be widely adopted in the future development of high‐performance LDH photocatalysts for ammonia production and other challenging chemical transformations (e.g., CO₂ reduction and water splitting).

中文翻译：

分层双氢氧化物纳米片的碱蚀增强光催化氮还原成NH3的能力

层状双氢氧化物（LDH）纳米片在广泛的光反应中显示出良好的活性，该活性通常归因于纳米片中大量的表面氧空位或配位不饱和金属阳离子，它们充当反应物吸附和活化的活性位点。最近，LDH纳米片已经显示出对于使用水作为还原剂将N ₂光催化还原为NH ₃非常有效。本文证明了用NaOH水溶液对ZnCr-LDH，ZnAl-LDH和NiAl-LDH纳米片进行简单的预处理可以大大提高纳米片中氧空位的浓度和低配位金属中心，从而显着增强了它们的光催化活性。 N ₂还原为NH₃在紫外线可见辐射下（无需添加牺牲剂或助催化剂）。预期本文介绍的简便的碱蚀刻策略将在高性能LDH光催化剂的未来开发中被广泛采用，以用于氨生产和其他具有挑战性的化学转化（例如，CO ₂还原和水分解）。

更新日期：2020-09-08

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