Efficient Photocatalytic Nitrogen Fixation over Cuδ+‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets,Advanced Energy Materials

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Efficient Photocatalytic Nitrogen Fixation over Cuδ+‐Modified Defective ZnAl‐Layered Double Hydroxide Nanosheets
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-01-15 , DOI: 10.1002/aenm.201901973
Shuai Zhang _{1,

2} , Yunxuan Zhao _{1,

2} , Run Shi ₁ , Chao Zhou ₁ , Geoffrey I. N. Waterhouse ₃ , Li‐Zhu Wu ₁ , Chen‐Ho Tung ₁ , Tierui Zhang _{1,

2}

Affiliation

The photocatalytic reduction of nitrogen (N₂) with water (H₂O) as the reducing agent holds great promise as a sustainable future technology for the synthesis of ammonia (NH₃). Herein, the effect of oxygen vacancies and electron‐rich Cu^δ⁺ on the performance of zinc‐aluminium layered double hydroxide (ZnAl‐LDH) nanosheet photocatalysts for N₂ reduction to NH₃ under UV–vis excitation is systematically explored. Results show that a 0.5%‐ZnAl‐LDH nanosheet photocatalyst (containing 0.5 mol% Cu by metal basis) affords a remarkable NH₃ production rate of 110 µmol g⁻¹ h⁻¹ and excellent stability in pure water. The X‐ray absorption spectroscopy, electron paramagnetic resonance, and density functional theory calculations reveal that Cu addition imparts oxygen vacancies and coordinatively unsaturated Cu^δ⁺ (δ < 2) with electron‐rich property in the ZnAl‐LDH nanosheets, both of which readily contribute to efficient separation and transfer of photogenerated electrons and holes and promote N₂ adsorption, thereby both activating N₂ and facilitating its multielectrons reduction to NH₃.

中文翻译：

Cuδ+修饰的有缺陷的ZnAl层状双氢氧化物纳米片上的高效光催化固氮

以水（H ₂ O）为还原剂光催化还原氮（N ₂）具有广阔的前景，有望作为未来可持续的合成氨（NH ₃）技术。在本文中，系统地研究了氧空位和富电子^Cuδ⁺对锌铝层状双氢氧化物（ZnAl-LDH）纳米片光催化剂在UV-vis激发下将N ₂还原为NH _{3的性能的影响}。结果表明，0.5％‐ZnAl‐LDH纳米片光催化剂（以金属计含0.5 mol％的Cu）提供了110 µmol g ^-1 h ^-1的显着NH ₃生产率。在纯水中具有出色的稳定性。X射线吸收光谱，电子顺磁共振和密度泛函理论计算表明，Cu的添加使ZnAl-LDH纳米片中的氧空位和配位不饱和的^Cuδ⁺（δ<2）具有丰富的电子特性。有助于有效分离和转移光生电子和空穴，并促进N ₂吸附，从而活化N ₂并促进其多电子还原为NH ₃。

更新日期：2020-02-25

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