Catalytic ammonia synthesis by transition metal molecular complexes
AssigneeCalifornia Institute of Technology
InventorsJonas C. Peters, John S. Anderson, Sidney E. Cruetz, Jonathan D. Rittle
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Abstract
This invention relates to molecular catalysts and chemical reactions utilizing the same, and particularly to catalysts and catalytic methods for reduction of molecular nitrogen. The molecular catalytic platform provided herein is capable of the facile reduction of molecular nitrogen under useful conditions such as room temperature or less and atmospheric pressure or less.
Claims27
A catalytic process for reduction of molecular nitrogen (N2) to generate a reduction product, said process comprising the steps of:
- contacting a transition metal catalyst with a source of protons and a source of electrons in the presence of said molecular nitrogen, thereby generating said reduction product;
- wherein said transition metal catalyst comprises a metal complex comprising a transition metal atom selected from the group consisting of Fe and Co, and a phosphine ligand (L) having the formula (FX1A), (FX1B) or (FX1C):
- wherein:
- X1 is B, C, Si or P;
- each of L1, L2 and L3 is independently a substituted or unsubstituted C1-C10 alkylene, C3-C10 cycloalkylene, C5-C10 arylene, or C5-C10 heteroarylene;
- each of R1, R2, R3, R4, R5, R6 and R7 is independently hydrogen or a substituted or unsubstituted C1-C8 alkyl, C3-C8 cycloalkyl, C5-C8 aryl, C5-C8 heteroaryl, C1-C18 acyl, C2-C8 alkenyl, C2-C8 alkynyl, or —P(OR8)2, wherein each R8 is independently hydrogen, C1-C8 alkyl, C3-C8 cycloalkyl, C5-C8 aryl or C5-C8 heteroaryl.
A catalyst formulation for reduction of molecular nitrogen (N2) to generate a reduction product, said formulation comprising:
- a transition metal catalyst comprising a metal complex comprising a transition metal atom selected from the group consisting of Fe and Co, and a phosphine ligand (L);
- a source of protons comprising one or more acids;
- and
- a source of electrons comprising one or more reductants;
- and
- a phosphine ligand (L) having the formula (FX1A), (FX1B) or (FX1C):
- wherein:
- X1 is B, C, Si or P;
- each of L1, L2 and L3 is independently a substituted or unsubstituted C1-C10 alkylene, C3-C10 cycloalkylene, C5-C10 arylene, or C5-C10 heteroarylene;
- each of R1, R2, R3, R4, R5, R6 and R7 is independently hydrogen or a substituted or unsubstituted C1-C8 alkyl, C3-C8 cycloalkyl, C5-C8 aryl, C5-C8 heteroaryl, C1-C18 acyl, C2-C8 alkenyl, C2-C8 alkynyl, or —P(OR8)2, wherein each R8 is independently hydrogen, C1-C8 alkyl, C3-C8 cycloalkyl, C5-C8 aryl or C5-C8 heteroaryl.
Dependencies are inferred from the claim text.