Chicken fat for catalysis: a scaffold is as important for molecular complexes for energy transformations as it is for enzymes in catalytic function

2019 ◽  
Vol 3 (12) ◽  
pp. 3260-3278 ◽  
Author(s):  
Joseph A. Laureanti ◽  
Molly O'Hagan ◽  
Wendy J. Shaw
Keyword(s):  
Coordination Sphere ◽  
Molecular Complexes ◽  
Catalytic Performance ◽  
Chicken Fat ◽  
Catalytic Function ◽  
Outer Coordination Sphere

The outer coordination sphere, sometimes called chicken fat, is essential to achieving the best catalytic performance for energy transductions.

Phenol Reduces Nitrite to NO at Copper(II): Role of a Proton-Responsive Outer Coordination Sphere in Phenol Oxidation

2020 ◽  
Vol 142 (4) ◽  
pp. 1726-1730 ◽  
Author(s):  
Aditesh Mondal ◽  
Kiran P. Reddy ◽  
Jeffery A. Bertke ◽  
Subrata Kundu
Keyword(s):  
Coordination Sphere ◽  
Phenol Oxidation ◽  
Outer Coordination Sphere

Macromolecular Engineering of the Outer Coordination Sphere of [2Fe-2S] Metallopolymers to Enhance Catalytic Activity for H2 Production

2018 ◽  
Vol 7 (11) ◽  
pp. 1383-1387 ◽  
Author(s):  
William P. Brezinski ◽  
Metin Karayilan ◽  
Kayla E. Clary ◽  
Keelee C. McCleary-Petersen ◽  
Liye Fu ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Coordination Sphere ◽  
H2 Production ◽  
Outer Coordination Sphere

scholarly journals Metallopolymerization as a Strategy to Translate Ligand-Modulated Chemoselectivity to Porous Catalysts

2019 ◽  
Author(s):  
Wen-Yang Gao ◽  
Andrew A. Ezazi ◽  
Chen-Hao Wang ◽  
Jisue Moon ◽  
Carter Abney ◽  
...  
Keyword(s):  
Coordination Sphere ◽  
Nir Spectroscopy ◽  
Molecular Complexes ◽  
Allylic Amination ◽  
X Ray ◽  
Porous Catalysts ◽  
Nitrene Transfer ◽  
Synthetic Strategy ◽  
Formidable Challenge ◽  
Molecular Catalysts

<div> <div> <div> <p>Porous catalysts have garnered substantial interest as potential platforms for group-transfer catalysis due to the ability to site-isolate catalysts and to non-covalently co- localize substrates in proximity to reactive intermediates. In contrast to soluble molecular catalysts, the limited synthetic toolbox available to prepare porous catalysts presents a formidable challenge to controlling the primary coordination sphere of lattice-confined catalysts and thus modulating the electronic structures of reactive catalyst intermediates. Here, we utilize Sonogashira cross-coupling chemistry to prepare a family of porous metallopolymers, in which the primary coordination sphere of Ru2 sites is systematically varied. The newly synthesized materials are characterized by IR, elemental analysis, gas sorption, powder X-ray diffraction, thermogravimetric analysis, X-ray absorption spectroscopy, and diffuse-reflectance UV-vis-NIR spectroscopy. The resulting porous materials are catalysts for nitrene-transfer chemistry and the chemoselectivty for allylic amination of olefin aziridination can be tuned by modulating the primary coordination sphere of the catalyst sites. The demonstration of metallopolymerization as a rational synthetic strategy allows to translate ligand-modulated chemoselectivity to porous catalysts, which represents a new opportunity to tailor the functionality of heterogeneous analogues of molecular complexes. </p> </div> </div> </div>

scholarly journals Metallopolymerization as a Strategy to Translate Ligand-Modulated Chemoselectivity to Porous Catalysts

2019 ◽  
Author(s):  
Wen-Yang Gao ◽  
Andrew A. Ezazi ◽  
Chen-Hao Wang ◽  
Jisue Moon ◽  
Carter Abney ◽  
...  
Keyword(s):  
Coordination Sphere ◽  
Nir Spectroscopy ◽  
Molecular Complexes ◽  
Allylic Amination ◽  
X Ray ◽  
Porous Catalysts ◽  
Nitrene Transfer ◽  
Synthetic Strategy ◽  
Formidable Challenge ◽  
Molecular Catalysts

<div> <div> <div> <p>Porous catalysts have garnered substantial interest as potential platforms for group-transfer catalysis due to the ability to site-isolate catalysts and to non-covalently co- localize substrates in proximity to reactive intermediates. In contrast to soluble molecular catalysts, the limited synthetic toolbox available to prepare porous catalysts presents a formidable challenge to controlling the primary coordination sphere of lattice-confined catalysts and thus modulating the electronic structures of reactive catalyst intermediates. Here, we utilize Sonogashira cross-coupling chemistry to prepare a family of porous metallopolymers, in which the primary coordination sphere of Ru2 sites is systematically varied. The newly synthesized materials are characterized by IR, elemental analysis, gas sorption, powder X-ray diffraction, thermogravimetric analysis, X-ray absorption spectroscopy, and diffuse-reflectance UV-vis-NIR spectroscopy. The resulting porous materials are catalysts for nitrene-transfer chemistry and the chemoselectivty for allylic amination of olefin aziridination can be tuned by modulating the primary coordination sphere of the catalyst sites. The demonstration of metallopolymerization as a rational synthetic strategy allows to translate ligand-modulated chemoselectivity to porous catalysts, which represents a new opportunity to tailor the functionality of heterogeneous analogues of molecular complexes. </p> </div> </div> </div>

Outer Coordination Sphere Proton Relay Base and Proximity Effects on Hydrogen Oxidation with Iron Electrocatalysts

2019 ◽  
Vol 38 (6) ◽  
pp. 1391-1396 ◽  
Author(s):  
Neeraj Kumar ◽  
Jonathan M. Darmon ◽  
Charles J. Weiss ◽  
Monte L. Helm ◽  
Simone Raugei ◽  
...  
Keyword(s):  
Coordination Sphere ◽  
Hydrogen Oxidation ◽  
Proximity Effects ◽  
Proton Relay ◽  
Outer Coordination Sphere

Active Hydrogenation Catalyst with a Structured, Peptide-Based Outer-Coordination Sphere

ACS Catalysis ◽  
2012 ◽  
Vol 2 (10) ◽  
pp. 2114-2118 ◽  
Author(s):  
Avijita Jain ◽  
Garry W. Buchko ◽  
Matthew L. Reback ◽  
Molly O’Hagan ◽  
Bojana Ginovska-Pangovska ◽  
...  
Keyword(s):  
Coordination Sphere ◽  
Hydrogenation Catalyst ◽  
Outer Coordination Sphere

scholarly journals Cover Picture: The Role of a Dipeptide Outer-Coordination Sphere on H2 -Production Catalysts: Influence on Catalytic Rates and Electron Transfer (Chem. Eur. J. 6/2013)

2013 ◽  
Vol 19 (6) ◽  
pp. 1837-1837
Author(s):  
Matthew L. Reback ◽  
Bojana Ginovska-Pangovska ◽  
Ming-Hsun Ho ◽  
Avijita Jain ◽  
Thomas C. Squier ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Coordination Sphere ◽  
H2 Production ◽  
Outer Coordination Sphere

Using the Outer Coordination Sphere to Tune the Strength of Metal Extractants

2011 ◽  
Vol 50 (10) ◽  
pp. 4515-4522 ◽  
Author(s):  
Ross S. Forgan ◽  
Benjamin D. Roach ◽  
Peter A. Wood ◽  
Fraser J. White ◽  
John Campbell ◽  
...  
Keyword(s):  
Coordination Sphere ◽  
Outer Coordination Sphere

Optimizing conditions for utilization of an H2 oxidation catalyst with outer coordination sphere functionalities

2016 ◽  
Vol 45 (24) ◽  
pp. 9786-9793 ◽  
Author(s):  
Arnab Dutta ◽  
Bojana Ginovska ◽  
Simone Raugei ◽  
John A. S. Roberts ◽  
Wendy J. Shaw
Keyword(s):  
Coordination Sphere ◽  
Oxidation Catalyst ◽  
Outer Coordination Sphere ◽  
H2 Oxidation

[Ni(PCy2NArginine2)2]2+ (CyArg) or [Ni(PCy2NBenzyl2)2]2+ (CyBn) were evaluated for H2 oxidation as a function of temperature, pressure, and solvent. 70 °C and 100 atm H2 result in a TOF of 1.1 × 106 s−1 and an overpotential of 240 mV for CyArg in water. In methanol the rates were 280 s−1 for CyArg and 80 s−1 for CyBn, demonstrating the importance of water and the outer coordination sphere (OCS).

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