Process for light-driven hydrocarbon oxidation at ambient temperatures

Shelnutt, John A

Title: Process for light-driven hydrocarbon oxidation at ambient temperatures

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Abstract

A photochemical reaction for the oxidation of hydrocarbons uses molecular oxygen as the oxidant. A reductive photoredox cycle that uses a tin(IV)- or antimony(V)-porphyrin photosensitizer generates the reducing equivalents required to activate oxygen. This artificial photosynthesis system drives a catalytic cycle, which mimics the cytochrome P.sub.450 reaction, to oxidize hydrocarbons. An iron(III)- or manganese(III)-porphyrin is used as the hydrocarbon-oxidation catalyst. Methylviologen can be used as a redox relay molecule to provide for electron-transfer from the reduced photosensitizer to the Fe or Mn porphyrin. The system is long-lived and may be used in photo-initiated spectroscopic studies of the reaction to determine reaction rates and intermediates.

Inventors:

Shelnutt, John A ^[1]

Tijeras, NM

Issue Date:: 1990-01-01

Research Org.:: AT&T

OSTI Identifier:: 867340

Patent Number(s):: 4917784

Assignee:: United States of America as represented by United States (Washington, DC)

Patent Classifications (CPCs):: B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS

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B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY
B01J2531/52 - Antimony
B01J2531/025 - Ligands with a porphyrin ring system or analogues thereof, e.g. phthalocyanines, corroles

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS
C07C45/33 - of CHx-moieties
C07C29/50 - with molecular oxygen only

B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY
B01J31/1815 - {with more than one complexing nitrogen atom, e.g. bipyridyl, 2-aminopyridine}

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS
C07C2601/16 - the ring being unsaturated

B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY
B01J19/121 - {Coherent waves, e.g. laser beams
B01J2531/842 - Iron

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS
C07C35/18 - with unsaturation at least in the ring

B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY
B01J2531/42 - Tin

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS
C07C31/125 - containing five to twenty-two carbon atoms
C07C45/34 - in unsaturated compounds

B - PERFORMING OPERATIONS B01 - PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL B01J - CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY
B01J19/122 - {Incoherent waves
B01J2231/70 - Oxidation reactions, e.g. epoxidation,

C - CHEMISTRY C07 - ORGANIC CHEMISTRY C07C - ACYCLIC OR CARBOCYCLIC COMPOUNDS
C07C45/36 - in compounds containing six-membered aromatic rings

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DOE Contract Number:: AC04-76DP00789

Resource Type:: Patent

Country of Publication:: United States

Language:: English

Subject:: process; light-driven; hydrocarbon; oxidation; ambient; temperatures; photochemical; reaction; hydrocarbons; molecular; oxygen; oxidant; reductive; photoredox; cycle; antimony; -porphyrin; photosensitizer; generates; reducing; equivalents; required; activate; artificial; photosynthesis; drives; catalytic; mimics; cytochrome; 450; oxidize; iron; iii; manganese; hydrocarbon-oxidation; catalyst; methylviologen; redox; relay; molecule; provide; electron-transfer; reduced; mn; porphyrin; long-lived; photo-initiated; spectroscopic; studies; determine; rates; intermediates; reaction rate; ambient temperature; chemical reaction; photochemical reaction; oxidation catalyst; reaction rates; ambient temperatures; molecular oxygen; spectroscopic studies; artificial photosynthesis; hydrocarbon oxidation; /204/

Citation Formats


                    Shelnutt, John A. Process for light-driven hydrocarbon oxidation at ambient temperatures.  United States: N. p., 1990. 
        Web.

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                    Shelnutt, John A. Process for light-driven hydrocarbon oxidation at ambient temperatures.  United States.

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                    Shelnutt, John A. Mon .  
        "Process for light-driven hydrocarbon oxidation at ambient temperatures".  United States.  https://www.osti.gov/servlets/purl/867340.

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@article{osti_867340,

  title        = {Process for light-driven hydrocarbon oxidation at ambient temperatures},

  author       = {Shelnutt, John A},

  abstractNote = {A photochemical reaction for the oxidation of hydrocarbons uses molecular oxygen as the oxidant. A reductive photoredox cycle that uses a tin(IV)- or antimony(V)-porphyrin photosensitizer generates the reducing equivalents required to activate oxygen. This artificial photosynthesis system drives a catalytic cycle, which mimics the cytochrome P.sub.450 reaction, to oxidize hydrocarbons. An iron(III)- or manganese(III)-porphyrin is used as the hydrocarbon-oxidation catalyst. Methylviologen can be used as a redox relay molecule to provide for electron-transfer from the reduced photosensitizer to the Fe or Mn porphyrin. The system is long-lived and may be used in photo-initiated spectroscopic studies of the reaction to determine reaction rates and intermediates.},

  doi          = {},

  journal      = {},
number       = ,

  volume       = ,

  place        = {United States},

  year         = {1990},

  month        = {1}

}

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