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A heterogeneous hydrogen-evolution catalyst based on a mesoporous organosilica with a diiron catalytic center modelling [FeFe]-hydrogenase

(2018) CHEMCATCHEM. 10(21). p.4894-4899
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Abstract
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.
Keywords
periodic mesoporous organosilica, hydrogen evolution, [FeFe]-hydrogenase, diiron complex, photocatalysis, METAL-ORGANIC FRAMEWORK, ACTIVE-SITE MIMICS, H-2 PRODUCTION, PHOTOCHEMICAL PRODUCTION, AQUEOUS-SOLUTION, SYSTEM, WATER, ACTIVATION, COMPLEX

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Citation

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Chicago
Himiyama, Tomoki, Minoru Waki, Dolores Esquivel, Akira Onoda, Takashi Hayashi, Pascal Van Der Voort, and Shinji Inagaki. 2018. “A Heterogeneous Hydrogen-evolution Catalyst Based on a Mesoporous Organosilica with a Diiron Catalytic Center Modelling [FeFe]-hydrogenase.” Chemcatchem 10 (21): 4894–4899.
APA
Himiyama, T., Waki, M., Esquivel, D., Onoda, A., Hayashi, T., Van Der Voort, P., & Inagaki, S. (2018). A heterogeneous hydrogen-evolution catalyst based on a mesoporous organosilica with a diiron catalytic center modelling [FeFe]-hydrogenase. CHEMCATCHEM, 10(21), 4894–4899.
Vancouver
1.
Himiyama T, Waki M, Esquivel D, Onoda A, Hayashi T, Van Der Voort P, et al. A heterogeneous hydrogen-evolution catalyst based on a mesoporous organosilica with a diiron catalytic center modelling [FeFe]-hydrogenase. CHEMCATCHEM. 2018;10(21):4894–9.
MLA
Himiyama, Tomoki, Minoru Waki, Dolores Esquivel, et al. “A Heterogeneous Hydrogen-evolution Catalyst Based on a Mesoporous Organosilica with a Diiron Catalytic Center Modelling [FeFe]-hydrogenase.” CHEMCATCHEM 10.21 (2018): 4894–4899. Print.
@article{8585037,
  abstract     = {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.},
  author       = {Himiyama, Tomoki and Waki, Minoru and Esquivel, Dolores and Onoda, Akira and Hayashi, Takashi and Van Der Voort, Pascal and Inagaki, Shinji},
  issn         = {1867-3880},
  journal      = {CHEMCATCHEM},
  keywords     = {periodic mesoporous organosilica,hydrogen evolution,[FeFe]-hydrogenase,diiron complex,photocatalysis,METAL-ORGANIC FRAMEWORK,ACTIVE-SITE MIMICS,H-2 PRODUCTION,PHOTOCHEMICAL PRODUCTION,AQUEOUS-SOLUTION,SYSTEM,WATER,ACTIVATION,COMPLEX},
  language     = {eng},
  number       = {21},
  pages        = {4894--4899},
  title        = {A heterogeneous hydrogen-evolution catalyst based on a mesoporous organosilica with a diiron catalytic center modelling [FeFe]-hydrogenase},
  url          = {http://dx.doi.org/10.1002/cctc.201801257},
  volume       = {10},
  year         = {2018},
}

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