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Title: Progress toward Biomass and Coal-Derived Syngas Warm Cleanup: Proof-of-Concept Process Demonstration of Multicontaminant Removal for Biomass Application

Journal Article · · Industrial and Engineering Chemistry Research, 52(24):8125-8138
DOI:https://doi.org/10.1021/ie4004927· OSTI ID:1089611

Systems comprising of multiple sorbent and catalytic beds have been developed for the warm syngas cleanup of coal- and biomass-derived syngas. Tailored specifically for biomass application the process described here consists of six primary unit operations: 1) Na2CO3 bed for HCl removal, 2) two regenerable ZnO beds for bulk H2S removal, 3) ZnO bed for H2S polishing, 4) NiCu/SBA-16 sorbent for trace metal (e.g. AsH3) removal, 5) steam reforming catalyst bed for tars and light hydrocarbons reformation and NH3 decomposition, and a 6) Cu-based LT-WGS catalyst bed. Simulated biomass-derived syngas containing a multitude of inorganic contaminants (H2S, AsH3, HCl, and NH3) and hydrocarbon additives (methane, ethylene, benzene, and naphthalene) was used to demonstrate process effectiveness. The efficiency of the process was demonstrated for a period of 175 hours, during which no signs of deactivation were observed. Post-run analysis revealed small levels of sulfur slipped through the sorbent bed train to the two downstream catalytic beds. Future improvements could be made to the trace metal polishing sorbent to ensure complete inorganic contaminant removal (to low ppb level) prior to the catalytic steps. However, dual, regenerating ZnO beds were effective for continuous removal for the vast majority of the sulfur present in the feed gas. The process was effective for complete AsH3 and HCl removal. The steam reforming catalyst completely reformed all the hydrocarbons present in the feed (methane, ethylene, benzene, and naphthalene) to additional syngas. However, post-run evaluation, under kinetically-controlled conditions, indicates deactivation of the steam reforming catalyst. Spent material characterization suggests this is attributed, in part, to coke formation, likely due to the presence of benzene and/or naphthalene in the feed. Future adaptation of this technology may require dual, regenerable steam reformers. The process and materials described in this report hold promise for a warm cleanup of a variety of contaminant species within warm syngas.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1089611
Report Number(s):
PNNL-SA-92772; 35214; 32705; 32704; 46194; BM0101010
Journal Information:
Industrial and Engineering Chemistry Research, 52(24):8125-8138, Journal Name: Industrial and Engineering Chemistry Research, 52(24):8125-8138
Country of Publication:
United States
Language:
English