期刊
CHEMCATCHEM
卷 10, 期 21, 页码 4908-4913出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201801257
关键词
periodic mesoporous organosilica; hydrogen evolution; [FeFe]-hydrogenase; diiron complex; photocatalysis
资金
- JST ACT-C, Japan [JPMJCR12Y1]
- Ramon Areces Foundation
A diiron [FeFe]-hydrogenase model complex tethered with a maleimide group, FeFe1, was covalently grafted on the pore surface of a periodic mesoporous organosilica with thiol groups (SH-PMO) to form an efficient heterogeneous hydrogen (H-2)-evolution catalyst FeFe1@PMO. The coordination structure of the FeFe1 complex and the ordered pore structure were almost completely preserved even after immobilization of FeFe1 on SH-PMO. The FeFe1@PMO promoted photocatalysis for H-2 evolution in water containing a photosensitizer [Ru(bpy)(3)](2+), with a turnover number (TON) of 310 over 120 min. The TON was greater than those of an analogous homogeneous FeFe1 catalyst (TON=180) and conventional diiron complexes immobilized on solid supports (TON=6-18). The increased TON for FeFe1@PMO compared to the homogeneous FeFe1 was attributed to the improvement in the stability of the FeFe1 complex by immobilization on the pore surface of SH-PMO. A [Ru(bpy)(3)](2+) photosensitizer tethered with a maleimide (Ru1) was prepared and co-immobilized on FeFe1@PMO to form an all-solid-state photocatalyst FeFe1-Ru1@PMO. FeFe1-Ru1@PMO evolved H-2 without the additional [Ru(bpy)(3)](2+) photosensitizer, suggesting efficient photoinduced electron transfer from the immobilized Ru1 to the immobilized FeFe1.
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