Elucidating the Photoredox Nature of Isolated Iron Active Sites on MCM-41

ACS Catalysis ◽  
2017 ◽  
Vol 7 (3) ◽  
pp. 1646-1654 ◽  
Author(s):  
Laura Collado ◽  
Ingrid Jansson ◽  
Ana E. Platero-Prats ◽  
Virginia Perez-Dieste ◽  
Carlos Escudero ◽  
...  
Keyword(s):  
Active Sites ◽  
Iron Active Sites ◽  
Mcm 41

The design and catalytic performance of molybdenum active sites on an MCM-41 framework for the aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran

2019 ◽  
Vol 9 (3) ◽  
pp. 811-821 ◽  
Author(s):  
Zhao-Meng Wang ◽  
Li-Juan Liu ◽  
Bo Xiang ◽  
Yue Wang ◽  
Ya-Jing Lyu ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Active Sites ◽  
Aerobic Oxidation ◽  
Catalytic Performance ◽  
Mcm 41

The catalytic activity decreases as –(SiO)3Mo(OH)(O) > –(SiO)2Mo(O)2 > –(O)4–MoO.

A Pyridinic Fe-N4 Macrocycle Effectively Models the Active Sites in Fe/N-Doped Carbon Electrocatalysts

2020 ◽  
Author(s):  
Travis Marshall-Roth ◽  
Nicole J. Libretto ◽  
Alexandra T. Wrobel ◽  
Kevin Anderton ◽  
Nathan D. Ricke ◽  
...  
Keyword(s):  
Oxygen Reduction ◽  
Active Sites ◽  
Catalytic Properties ◽  
Reduction Reaction ◽  
Iron Phthalocyanine ◽  
Electrochemical Studies ◽  
Onset Potential ◽  
Nitrogen Doped Carbon ◽  
Iron Active Sites

Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum in fuel cells, but their active site structures are poorly understood. A leading postulate is that iron active sites in this class of materials exist in an Fe-N<sub>4</sub> pyridinic ligation environment. Yet, molecular Fe-based catalysts for the oxygen reduction reaction (ORR) generally feature pyrrolic coordination and pyridinic Fe-N<sub>4</sub> catalysts are, to the best of our knowledge, non-existent. We report the synthesis and characterization of a molecular pyridinic hexaazacyclophane macrocycle, (phen<sub>2</sub>N<sub>2</sub>)Fe, and compare its spectroscopic, electrochemical, and catalytic properties for oxygen reduction to a prototypical Fe-N-C material, as well as iron phthalocyanine, (Pc)Fe, and iron octaethylporphyrin, (OEP)Fe, prototypical pyrrolic iron macrocycles. N 1s XPS signatures for coordinated N atoms in (phen<sub>2</sub>N<sub>2</sub>)Fe are positively shifted relative to (Pc)Fe and (OEP)Fe, and overlay with those of Fe-N-C. Likewise, spectroscopic XAS signatures of (phen<sub>2</sub>N<sub>2</sub>)Fe are distinct from those of both (Pc)Fe and (OEP)Fe, and are remarkably similar to those of Fe-N-C with compressed Fe–N bond lengths of 1.97 Å in (phen<sub>2</sub>N<sub>2</sub>)Fe that are close to the average 1.94 Å length in Fe-N-C. Electrochemical studies establish that both (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe have relatively high Fe(III/II) potentials at ~0.6 V, ~300 mV positive of (OEP)Fe. The ORR onset potential is found to directly correlate with the Fe(III/II) potential leading to a ~300 mV positive shift in the onset of ORR for (Pc)Fe and (phen<sub>2</sub>N<sub>2</sub>)Fe relative to (OEP)Fe. Consequently, the ORR onset for (phen<sub>2</sub>N<sub>2</sub>)Fe and (Pc)Fe is within 150 mV of Fe-N-C. Unlike (OEP)Fe and (Pc)Fe, (phen<sub>2</sub>N<sub>2</sub>)Fe displays excellent selectivity for 4-electron ORR with <4% maximum H<sub>2</sub>O<sub>2</sub> production, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data establish (phen<sub>2</sub>N<sub>2</sub>)Fe as a pyridinic iron macrocycle that effectively models Fe-N-C active sites, thereby providing a rich molecular platform for understanding this important class of catalytic materials.<p><b></b></p>

The Selective Oxidation of Hydrocarbons on Isolated Iron Active Sites under Ambient Conditions

2019 ◽  
Vol 41 (6) ◽  
pp. 946-946
Author(s):  
Zhengliang Qi Zhengliang Qi ◽  
Junmei Liu Junmei Liu ◽  
Wanwan Guo and Jun Huang Wanwan Guo and Jun Huang
Keyword(s):  
Ionic Liquid ◽  
Activated Carbon ◽  
Carbon Material ◽  
Active Sites ◽  
High Selectivity ◽  
Good Activity ◽  
Ambient Conditions ◽  
Oxidation Of Hydrocarbons ◽  
Fe Catalysts ◽  
Iron Active Sites

The N-doped carbon material supported Fe catalysts were developed for the oxidation of C-H bond of hydrocarbons to ketones and alcohols. The supported Fe catalysts were prepared by pyrolysis of [CMIM]3Fe(CN)6 ionic liquid in activated carbon. And the Fe(Ⅲ)@CN-600 showed good activity and high selectivity for the oxidation of alfa C-H bond of alkylbenzenes. The isolated Fe(Ⅲ) iron active sites should be responsible for the high activity and selectivity for the oxidation of hydrocarbons to ketones. Several ketones were obtained in good to excellent yields. Moreover, cyclohexanone can also be obtained through the oxidation of cyclohexane.

Dioxygen Activation at Mononuclear Nonheme Iron Active Sites:  Enzymes, Models, and Intermediates

2004 ◽  
Vol 104 (2) ◽  
pp. 939-986 ◽  
Author(s):  
Miquel Costas ◽  
Mark P. Mehn ◽  
Michael P. Jensen ◽  
Lawrence Que
Keyword(s):  
Active Sites ◽  
Nonheme Iron ◽  
Dioxygen Activation ◽  
Iron Active Sites

Acidity and active sites of Al-MCM-41

1999 ◽  
Vol 184 (1) ◽  
pp. 49-60 ◽  
Author(s):  
H Kosslick ◽  
G Lischke ◽  
B Parlitz ◽  
W Storek ◽  
R Fricke
Keyword(s):  
Active Sites ◽  
Mcm 41

Dioxygen Activation at Mononuclear Nonheme Iron Active Sites: Enzymes, Models, and Intermediates

ChemInform ◽  
2004 ◽  
Vol 35 (21) ◽  
Author(s):  
Miquel Costas ◽  
Mark P. Mehn ◽  
Michael P. Jensen ◽  
Lawrence Jr. Que
Keyword(s):  
Active Sites ◽  
Nonheme Iron ◽  
Dioxygen Activation ◽  
Iron Active Sites

scholarly journals Ultrasonic-assisted preparation of highly active Co3O4/MCM-41 adsorbent and its desulfurization performance for low H2S concentration gas

RSC Advances ◽  
2020 ◽  
Vol 10 (50) ◽  
pp. 30214-30222
Author(s):  
Bolong Jiang ◽  
Jiaojing Zhang ◽  
Yanguang Chen ◽  
Hua Song ◽  
Tianzhen Hao ◽  
...  
Keyword(s):  
Surface Area ◽  
Active Sites ◽  
High Surface ◽  
High Surface Area ◽  
Highly Active ◽  
Ultrasonic Assisted ◽  
Sulfur Capacity ◽  
Mcm 41

Co3O4/MCM-41 adsorbent with high surface area and more active sites was successfully prepared by ultrasonic assisted impregnation (UAI) technology and it has been found that the sulfur capacity was improved by 33.2% because of ultrasonication.

scholarly journals Comparison in thermal stability and catalytic performance of H4PMo11VO40 heteropolyacid supported on mesoporous and macroporous silica materials

2020 ◽  
pp. 174751982092599
Author(s):  
Heng Zhang ◽  
Chunhao Yang ◽  
Shengying Zhao ◽  
Tingting Wang ◽  
Wancheng Zhu
Keyword(s):  
Thermal Stability ◽  
Active Sites ◽  
Catalytic Performance ◽  
High Dispersion ◽  
High Exposure ◽  
Macroporous Silica ◽  
One Dimensional ◽  
Ordered Macroporous ◽  
The One ◽  
Mcm 41

Ordered mesoporous silica, SBA-15 and MCM-41, and three-dimensionally ordered macroporous SiO2 were used as the supports of H4PMo11VO40 heteropolyacid for methacrolein oxidation. The dispersion and structural evolutions of the heteropolyacid along with thermal treatment were investigated. It was found that the heteropolyacid entered the one-dimensional mesoporous channels of SBA-15 and MCM-41, and the crystallization and growth were limited, leading to high dispersion of the heteropolyacid. However, the thermal stability was decreased under high dispersion. The migration of the heteropolyacid was observed to the end of the one-dimensional channels of SBA-15 and the outer surface of MCM-41 with calcination, accompanied by the decomposition of the heteropolyacid and the formation of MoO3. In comparison, the crystallization and growth of heteropolyacid were not limited in the open macropores of three-dimensionally ordered macroporous SiO2. Dispersed particles on the surface of the macropores with size of about 5 nm exhibited a higher thermal stability. The decomposition of the heteropolyacid in the SBA-15 and MCM-41 supported catalysts resulted in the loss of strong acid sites, causing low selectivity to methacrylic acid in methacrolein oxidation. High thermal stability with high exposure of the active sites in the three-dimensionally ordered macroporous SiO2 supported catalyst contributed to the enhancement in the catalytic performance.

Theoretical Study on Methane Oxidation Catalyzed by Fe/ZSM-5: The Significant Role of Water on Binuclear Iron Active Sites

2016 ◽  
Vol 120 (48) ◽  
pp. 27422-27429 ◽  
Author(s):  
Miao He ◽  
Jie Zhang ◽  
Xiu-Liang Sun ◽  
Biao-Hua Chen ◽  
Yang-Gang Wang
Keyword(s):  
Methane Oxidation ◽  
Significant Role ◽  
Active Sites ◽  
Theoretical Study ◽  
Iron Active Sites ◽  
Binuclear Iron
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