It has been known that use of the hydrogen selective membrane as a reactor (MR) could potentially improve the efficiency of the water shift reaction (WGS), one of the least efficient unit operations for production of high purity hydrogen from syngas. However, no membrane reactor technology has been reduced to industrial practice thus far, in particular for a large-scale operation. This implementation and commercialization barrier is attributed to the lack of a commercially viable hydrogen selective membrane with (1) material stability under the application environment and (2) suitability for large-scale operation. Thus, in this project, we have focused on (1) the deposition of the hydrogen selective carbon molecular sieve (CMS) membrane we have developed on commercially available membranes as substrate, and (2) the demonstration of the economic viability of the proposed WGS-MR for hydrogen production from coal-based syngas. The commercial stainless steel (SS) porous substrate (i.e., ZrO{sub 2}/SS from Pall Corp.) was evaluated comprehensively as the 1st choice for the deposition of the CMS membrane for hydrogen separation. The CMS membrane synthesis protocol we developed previously for the ceramic substrate was adapted here for the stainless steel substrate. Unfortunately no successful hydrogen selective membranes had been prepared during Yr I of this project. The characterization results indicated two major sources of defect present in the SS substrate, which may have contributed to the poor CMS membrane quality. Near the end of the project period, an improved batch of the SS substrate (as the 2nd generation product) was received from the supplier. Our characterization results confirm that leaking of the crimp boundary no longer exists. However, the thermal stability of the ZrO{sub 2}/SS substrate through the CMS membrane preparation condition must be re-evaluated in the future. In parallel with the SS membrane activity, the preparation of the CMS membranes supported on our commercial ceramic membrane for large-scale applications, such as coal-based power generation/hydrogen production, was also continued. A significant number (i.e., 98) of full-scale membrane tubes have been produced with an on-spec ratio of >76% during the first production trial. In addition, we have verified the functional performance and material stability of this hydrogen selective CMS membrane with a hydrocracker purge gas stream at a refinery pilot testing facility. No change in membrane performance was noted over the >100 hrs of testing conducted in the presence of >30% H{sub 2}S, >5,000 ppm NH{sub 3} (estimated), and heavy hydrocarbons on the order of 25%. The excellent stability of our hydrogen selective CMS membrane opens the door for its use in WGS-MR with a significantly reduced requirement of the feedstock pretreatment.
