Methods and compositions for the catalytic upgrading of alcohols

Patent metadata

Field	Value
Publication number	US-10882807-B2
Application number	US-201916360155-A
Country	US
Kind code	B2
Filing date	Mar 21, 2019
Priority date	Mar 21, 2018
Publication date	Jan 5, 2021
Grant date	Jan 5, 2021

Abstract

Compositions and methods of use related to metal organic frameworks (MOFs) and/or nanoparticles are generally described. In some embodiments, methods and compositions for the catalytic upgrading of alcohols using MOFs and/or nanoparticles associated with MOFs are generally described. In some embodiments, a catalytic MOF composition is provided, wherein the MOF composition comprises a MOF compound and a plurality of metal catalytic compounds. In some embodiments, an alcohol may be exposed to the MOF composition and/or a plurality of nanoparticles associated with the MOF composition such that the alcohol is converted to a higher order alcohol. Advantageously, in some embodiments, the alcohol conversion occurs at a relatively high turnover frequency and/or with a relatively high selectivity as compared to traditional methods for converting alcohols.

First claim

What is claimed is:

1. A method of upgrading an alcohol, comprising:
exposing a catalytic metal-organic framework (MOF) composition to one or more first alcohols; and
converting at least a portion of the one or more first alcohols to one or more second alcohols, wherein the catalytic MOF composition comprises a MOF compound and a plurality of metal catalytic compounds, wherein the MOF compound comprises a plurality of cobalt atoms or nickel atoms, and at least a portion of the plurality of metal catalytic compounds are bonded with and at least a portion of the cobalt atoms or nickel atoms in the form of an alloy comprising Ru x Co x-1 or Ru x Ni x-1 nanoparticles.

2. The method of claim 1 , wherein the one or more second alcohols are formed at a turnover number of at least about 1,000 Ru −1 , at least about 5,000 Ru −1 , at least about 10,000 Ru −1 , at least about 20,000 Ru −1 , at least about 50,000 Ru −1 , at least about 100,000 Ru −1 , at least about 200,000 Ru −1 , at least about 300,000 Ru −1 , at least about 400,000 Ru −1 , or at least about 500,000 Ru −1 .

3. The method of claim 1 , wherein the one or more second alcohols are formed at a turnover frequency of at least about 100 Ru −1 h −1 , at least about 500 Ru −1 h −1 , at least about 1,000 Ru −1 h −1 , at least about 2,000 Ru −1 h −1 , at least about 3,000 Ru −1 h −1 , at least about 4,000 Ru −1 h −1 , at least about 5,000 Ru −1 h −1 , or at least about 10,000 Ru −1 h −1 .

4. The method of claim 1 , wherein the one or more second alcohols are formed with a selectivity of at least about 80%, at least about 85%, at least about 90%, at least about 95%, at least about 97%, at least about 98%, at least about 99%, at least about 99.5%, at least about 99.8%, or at least about 99.9%.

5. The method of claim 1 , further comprising releasing at least a portion of the alloy from the MOF compound.

6. The method of claim 1 , wherein the one or more first alcohols comprises ethanol.

7. The method of claim 1 , wherein the one or more second alcohols comprises 1-butanol.

8. The method of claim 1 , wherein the one or more first alcohols comprises 1-butanol.

9. The method of claim 1 , wherein the one or more second alcohols comprises 2-ethyl-hexanol.

Assignees

• Massachusetts Inst Technology

Inventors

• Dinca Mircea
• Neumann Constanze Nicole

Classifications

• B01J31/1691 Primary

  Coordination polymers, e.g. metal-organic frameworks [MOF] (preparation of metal complexes containing carboxylic acid moieties C07C51/418; MOF's per se C07F) · CPC title

• C07F15/06

  Cobalt compounds · CPC title

• C07F15/0046

  Ruthenium compounds · CPC title

• B01J23/46

  Ruthenium, rhodium, osmium or iridium · CPC title

• C07F15/04

  Nickel compounds · CPC title