Iron-Complex-Based Supramolecular Framework Catalyst for Visible-Light-Driven CO2 Reduction
Iron-Complex-Based Supramolecular Framework Catalyst for Visible-Light-Driven CO2 Reduction
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DOI：
10.1021/jacs.3c00783
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发表时间：
2023-04-06
影响因子：
15
通讯作者：
Masaoka, Shigeyuki
中科院分区：
文献类型：
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作者：
Kosugi, Kento;Akatsuka, Chiharu;Masaoka, Shigeyuki
不含贵金属的分子基多相光催化剂是可见光驱动CO2还原最具吸引力的体系之一。然而，关于这类光催化剂的报道仍然有限，与含有贵金属的光催化剂相比，它们的活性相当低。在此，我们报道了一种铁络合物基多相光催化剂，用于高活性的CO2还原。我们成功的关键是使用一个超分子框架组成的铁卟啉配合物轴承芘部分在meso位置。该催化剂在可见光照射下具有较高的CO 2还原活性（CO生成量为29100 μ mol g-1 h-1，选择性为99.9%），是相关体系中最高的。该催化剂的性能也是优秀的表观量子产率CO生产（0.298%，在400 nm）和稳定性（长达96小时）。这项研究提供了一种简单的策略，可以在不使用贵金属的情况下制造一种高活性、选择性和稳定的光催化剂来减少二氧化碳。
Molecule-based heterogeneous photocatalysts without noble metals are one of the most attractive systems for visible light-driven CO2 reduction. However, reports on this class of photocatalysts are still limited, and their activities are quite low compared to those containing noble metals. Herein, we report an iron-complex-based heterogeneous photocatalyst for CO2 reduction with high activity. The key to our success is the use of a supramolecular framework composed of iron porphyrin complexes bearing pyrene moieties at meso positions. The catalyst exhibited high activity for CO2 reduction under visible-light irradiation (29100 mu mol g-1 h-1 for CO production, selectivity 99.9%), which is the highest among relevant systems. The performance of this catalyst is also excellent in terms of apparent quantum yield for CO production (0.298% at 400 nm) and stability (up to 96 h). This study provides a facile strategy to create a highly active, selective, and stable photocatalyst for CO2 reduction without utilizing noble metals.