Cerium-based Metal-Organic Layers Catalyze Hydrogen Evolution Reaction through Dual Photoexcitation,Journal of the American Chemical Society

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Cerium-based Metal-Organic Layers Catalyze Hydrogen Evolution Reaction through Dual Photoexcitation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-03-30 , DOI: 10.1021/jacs.0c00679
Yang Song ₁ , Yunhong Pi _{1,

2} , Xuanyu Feng ₁ , Kaiyuan Ni ₁ , Ziwan Xu ₁ , Justin S. Chen ₁ , Zhong Li ₂ , Wenbin Lin ₁

Affiliation

Cerium-based materials such as ceria are increasingly used in catalytic reactions. We report here the synthesis of the first Ce-based metal-organic layer (MOL), Ce6-BTB, comprising Ce6 secondary building units (SBUs) and 1,3,5-benzenetribenzoate (BTB) linkers, and its functionalization for photocatalytic hydrogen evolution reaction (HER). Ce6-BTB was post-synthetically modified with photosensitizing [(MBA)Ir(ppy)2]Cl or [(MBA)Ru(bpy)2]Cl2 (MBA = 2-(5'-methyl-[2,2'-bipyridin]-5-yl)acetate, ppy = 2-phenylpyridine, bpy = 2,2'-bipyridine) to afford Ce6-BTB-Ir or Ce6-BTB-Ru MOLs, respectively. The proximity of photosensitizing ligands and Ce6 SBUs in the MOLs facilitates electron transfer to drive photocatalytic HER under visible light with turnover numbers of 1357 and 484 for Ce6-BTB-Ir and Ce6-BTB-Ru, respectively. Photophysical and electrochemical studies revealed a novel dual photoexcitation pathway whereby the excited photosensitizers in the MOL are reductively quenched and then transfer electrons to Ce6 SBUs to generate CeIII centers which are further photoexcited to CeIII* species for HER.

中文翻译：

铈基金属有机层通过双光激发催化析氢反应

铈基材料如二氧化铈越来越多地用于催化反应。我们在此报告了第一个 Ce 基金属有机层 (MOL) Ce6-BTB 的合成，包括 Ce6 二级构建单元 (SBU) 和 1,3,5-苯三苯甲酸酯 (BTB) 连接体，及其对光催化氢的功能化进化反应（HER）。Ce6-BTB 用光敏 [(MBA)Ir(ppy)2]Cl 或 [(MBA)Ru(bpy)2]Cl2 (MBA = 2-(5'-methyl-[2,2'-联吡啶]-5-基）乙酸酯，ppy = 2-苯基吡啶，bpy = 2,2'-联吡啶）分别提供 Ce6-BTB-Ir 或 Ce6-BTB-Ru MOL。MOL 中光敏配体和 Ce6 SBU 的接近促进电子转移以驱动可见光下的光催化 HER，Ce6-BTB-Ir 和 Ce6-BTB-Ru 的转换数分别为 1357 和 484。

更新日期：2020-03-30

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