垂直生长富含 O 空位的 LDH 原子层作为 OER 敏感反应位点以促进钙钛矿氧化物的整体水分解,ACS Sustainable Chemistry & Engineering

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垂直生长富含 O 空位的 LDH 原子层作为 OER 敏感反应位点以促进钙钛矿氧化物的整体水分解
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-11-29 , DOI: 10.1021/acssuschemeng.2c05498
Enhui Jiang ₁ , Chengqi Guo ₂ , Pengwei Huo ₂ , Yan Yan ₂ , Peng Zhou ₃ , Yongsheng Yan ₂

Affiliation

控制光催化剂活性位点的丰度和调节析氧反应 (OER) 是光催化全水分解最理想但最具挑战性的技术。_{在此，我们展示了具有暴露 (001) 面的富含 O 空位的 NiCo-LDH 原子层（表示为 Vo-LDH）在钙钛矿氧化物立方体（例如，Al–CaTiO 3}和 Al–SrTiO ₃）上垂直生长，这可以提供多个可访问的 OER 敏感活性位点，以提高整体水分解性能。因此，Al–CaTiO ₃ /Vo-LDH (44%) 催化剂上的总水分解产率（H ₂：1.01 mmol·g ^–1 ·h ^–1和 O ₂：0.46 mmol·g ^–1·h ^–1 ) 是原始Al–CaTiO ₃催化剂的2.37倍。_{同时，Al–SrTiO 3} /Vo-LDH (44%) 催化剂的总水分解产率(H ₂ : 0.90 mmol·g ^–1 ·h ^–1和 O ₂ : 0.37 mmol·g ^–1 ·h ^–1 ) 是原始Al–SrTiO ₃催化剂的2.08 倍。就地漫反射红外傅立叶变换光谱表明，富含 O 空位的 NiCo-LDH 原子层可以作为 OER 敏感活性位点，并随 O 空位浓度而变化。动力学分析进一步证实，O 空位引起的水分解 (1612 cm ^–1 ) 是 NiCo-LDH 原子层上最主要的 OER 配置。此外，密度泛函理论 (DFT) 表明 NiCo-LDH 原子层上的 O 空位降低了 OER 步骤的能垒。

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Vertical Growth of O-Vacancy Rich LDH Atomic Layers as OER-Sensitive Reactive Sites to Boost Overall Water Splitting on Perovskite Oxides

Dominating the abundance of active sites of photocatalysts and regulating the oxygen evolution reaction (OER) are the most desired but challenging technologies for photocatalytic overall water splitting. Herein, we demonstrate that O-vacancy-rich NiCo-LDH atomic layers (denoted Vo-LDH) featuring an exposed (001) facet grow vertically on perovskite oxide cubes (e.g., Al–CaTiO₃ and Al–SrTiO₃), which can provide multiaccessible OER-sensitive active sites to boost the overall water splitting performance. As a result, the overall water splitting production rate on the Al–CaTiO₃/Vo-LDH (44%) catalyst (H₂: 1.01 mmol·g^–1·h^–1 and O₂: 0.46 mmol·g^–1·h^–1) is 2.37 times higher than that of the pristine Al–CaTiO₃ catalyst. Meanwhile, the overall water-splitting production rate on the Al–SrTiO₃/Vo-LDH (44%) catalyst (H₂: 0.90 mmol·g^–1·h^–1 and O₂: 0.37 mmol·g^–1·h^–1) is 2.08 times that of the pristine Al–SrTiO₃ catalyst. In situ diffuse reflection infrared Fourier transform spectroscopy reveals that the O-vacancy-rich NiCo-LDH atomic layers can serve as the OER-sensitive active sites and vary with the O-vacancy concentration. The kinetic analysis further confirms that the O-vacancy-induced water decomposition (1612 cm^–1) is the most dominant OER configuration on NiCo-LDH atomic layers. Furthermore, density functional theory (DFT) indicates that O-vacancies on NiCo-LDH atomic layers lower the energy barriers of OER steps.

更新日期：2022-11-29

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