Process for recovery and regeneration of deactivated catalysts used in dialkyl carbonate synthesis

Patent metadata

Field	Value
Publication number	US-11110449-B2
Application number	US-201615562044-A
Country	US
Kind code	B2
Filing date	Mar 23, 2016
Priority date	Mar 27, 2015
Publication date	Sep 7, 2021
Grant date	Sep 7, 2021

Abstract

The present invention discloses a process for recovery and regeneration of rare earth metals or salts thereof used as catalyst and which is conveniently integrated within the overall flow sheets of manufacturing dialkyl carbonates. Alkyl carbamate, alcohol and a rare earth metal salt as catalyst selected from the lanthanide series are added in a reactor to afford dialkyl carbonate. The rare earth metal catalyst is selected from samarium, cerium, lanthanum, neodymium, ytterbium, europium and gadolinium. Ammonia is added to a portion of the reaction mixture to precipitate the catalyst and the separated deactivated catalyst is dissolved in acid to afford regenerated catalyst, e.g., in triflic acid in the case of samarium triflate catalyst.

First claim

We claim:

1. A process for recovery and regeneration of a deactivated catalyst comprising the steps of:
(a) adding a reaction mixture including an alkyl carbamate, an alcohol and a rare earth metal salt including a lanthanide series element in a reactor;
(b) partially removing the reaction mixture of step (a) from a bottom of the reactor;
(c) separating the deactivated catalyst from the partially removed reaction mixture of step (b);
(d) dissolving the deactivated catalyst in acid;
(e) recovering a regenerated active catalyst from the dissolving step; and
(f) directly sending the regenerated active catalyst of step (e) to a reactor for synthesizing dialkyl carbonate.

2. The process as claimed in claim 1 , further comprising adding ammonia to the partially removed reaction mixture of step (b) in a pressure range of 1 to 25 bar and a temperature ranging from 60 to 200° C. to precipitate the deactivated catalyst.

3. The process as claimed in claim 1 , wherein said dialkyl carbonate is selected from di methyl carbonate, di ethyl carbonate, di propyl carbonate, and di butyl carbonate.

4. The process as claimed in claim 1 , wherein said lanthanide series element is selected from Samarium (Sm), Cerium (Ce), Lanthanum (La), Neodymium (Nd), Ytterbium (Yb), Europium (Eu) and Gadolinium (Gd).

5. The process as claimed in claim 1 , wherein said salt is selected from methane sulphonate, triflate, nitrate, chloride and para toluene sulphonate.

6. The process as claimed in claim 1 , wherein said dialkyl carbonate is di methyl carbonate and said rare earth metalsalt is samanum trifluoromethanesulfonate.

7. The process as claimed in claim 1 , wherein said acid is selected from methane sulphonic acid, trifluoromethanesulfonic acid, nitric acid, para toluene sulfonic acid and hydrochloric acid.

8. A process consisting of:
(a) providing a reaction mixture including an alkyl carbamate, an alcohol and a rare earth metal salt including a lanthanide series element in a reactor;
(b) partially removing the reaction mixture of step (a) from a bottom of the reactor;
(c) separating a deactivated catalyst from the partially removed reaction mixture of step (b);
(d) dissolving the deactivated catalyst in acid;
(e) recovering a regenerated active catalyst from the dissolved deactivated catalyst of step (d); and
(f) directly sending the regenerated active catalyst of step (e) to a reactor for synthesizing dialkyl carbonate.

Assignees

• Council Scient Ind Res

Inventors

• Ranade Vivek Vinayak
• Kelkar Ashutosh Anant
• Rane Vilas Hari
• Kinage Anil Kisan
• Shingote Savita Kiran
• Roy Lalita Sanjib
• Mote Dhananjay Ravindra

Classifications

• B01J38/60

  using acids · CPC title

• Y02P20/584

  Recycling of catalysts · CPC title

• B01J23/10 Primary

  of rare earths · CPC title

• B01J23/92

  of catalysts comprising metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 · CPC title

• B01J38/66

  using ammonia or derivatives thereof · CPC title