TITLE: Novel process for methanol synthesis. Final report.

AUTHOR: J. W. Tierney;   I. Wender.

INST.  AUTHOR: Pittsburgh Univ., PA. Dept. of Chemical and Petroleum Engineering.

SPONSOR: Department of Energy, Washington, DC.

LANGUAGE: English

PUB.  TYPE: Technical Report

PUB.  COUNTRY: United States

SOURCE: Department of Energy [DE],  25 Jan 94,  150p.

NTIS ORDER NO.: DE94017111INW

ABSTRACT:

The use of methanol (MeOH) as a fuel additive and in MTBE production has renewed interest in the search for improved MeOH processes. Commercial processes are characterized by high pressures and temperatures with low per pass conversion (10--12%). Efforts are underway to find improved MeOH synthesis processes. A slurry phase ''concurrent'' synthesis of MeOH/methyl formate (MeF) which operates under relatively mild conditions (100 C) lower than present commercial processes) was the subject of investigation in this work. Evidence for a reaction scheme involving the carbonylation of MeOH to MeF followed by the hydrogenolysis of MeF to two molecules of MeOH -- the net result being the reaction of H(sub 2) with CO to give MeOH via MeF, is presented. Up to 90% per pass conversion and 98% selectivity to methanol at rates comparable to commercial processes have been obtained in spite of the presence of as much as 10,000 ppM CO(sub 2) and 3000 ppM H(sub 2)O in the gas and liquid respectively. The effect of process parameters such as temperature, pressure, H(sub 2)/CO ratio in the reactor, flow rate and catalyst loading were also investigated. The use of temperatures above 170(degrees)C at a pressure of 50 atm results in MeF being the limiting reactant. Small amounts of CH(sub 4) are also formed.  Significant MeOH synthesis rates at a pressure in the range of 40--50 atm makes possible the elimination of an upstream shift reactor and the use of an air-blown syngas generator. The nature of the catalysts was studied and correlated with the behavior of the various species in the concurrent synthesis.

REPORT  NUMBER: DOE/PC/89786-T18

CONTRACT  NUMBER: FG22-89PC89786