Metal‐Organic Frameworks (MOFs) recently emerged as a new platform for the realization of integrated devices for artificial photosynthesis. However, there remain few demonstrations of rational tuning of such devices for improved performance. Here, a fast molecular water oxidation catalyst working via water nucleophilic attack is integrated into the MOF MIL‐142, wherein Fe3O nodes absorb visible light, leading to charge separation. Materials are characterized by a range of structural and spectroscopic techniques. New, [Ru(tpy)(Qc)(H2O)]+ (tpy = 2,2′:6′,2″‐terpyridine and Qc = 8‐quinolinecarboxylate)‐doped Fe MIL‐142 achieved a high photocurrent (1.6 × 10−3 A·cm−2) in photo‐electrocatalytic water splitting at pH = 1. Unassisted photocatalytic H2 evolution is also reported with Pt as the co‐catalyst (4.8 µmol g−1 min−1). The high activity of this new system enables hydrogen gas capture from an easy‐to‐manufacture, scaled‐up prototype utilizing MOF deposited on FTO glass as a photoanode. These findings provide insights for the development of MOF‐based light‐driven water‐splitting assemblies utilizing a minimal amount of precious metals and Fe‐based photosensitizers.

中文翻译：

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用于人工光合作用的改良含钌铁基金属有机骨架（MOF）光阳极的合理设计


金属有机框架（MOF）最近成为实现人工光合作用集成装置的新平台。然而，为了提高性能而对此类设备进行合理调整的示范仍然很少。在这里，通过水亲核攻击起作用的快速分子水氧化催化剂被集成到 MOF MIL-142 中，其中 Fe3O 节点吸收可见光，导致电荷分离。材料通过一系列结构和光谱技术来表征。新的[Ru(tpy)(Qc)(H2O)]+（tpy = 2,2′:6′,2″-三联吡啶和Qc = 8-喹啉羧酸盐）掺杂的Fe MIL-142实现了高光电流（1.6 × 10−3 A·cm−2) 在 pH = 1 的光电催化水分解中。还报道了以 Pt 作为助催化剂 (4.8 µmol g−1 min−1) 无辅助光催化析氢。该新系统的高活性使得能够利用沉积在 FTO 玻璃上的 MOF 作为光阳极，从易于制造的放大原型中捕获氢气。这些发现为利用最少量的贵金属和铁基光敏剂开发基于 MOF 的光驱动水分解组件提供了见解。