WP 2: Gas Processing Unit 1 Strictly Confidential Workpackage 2: Gas Processing Unit KTI Review Meeting, May 11, 2005 M. Stutz, N. Hotz, Dr. N. Bieri, and Prof. D. Poulikakos NTB INTERSTAATLICHE HOCHSCHULE FÜR TECHNIK BUCHS

WP 2: Gas Processing Unit 2 Strictly Confidential Contributions to WP 2 NTB NMW Butane Reforming Post CombustionIntegration and Testing Inlet conditionsCompatibility with FC Heat exchange Feed / Exhaust Micromachining Coating NTB NMW Coating Micromachining Coating

WP 2: Gas Processing Unit 3 Strictly Confidential Project Management Thermal System Fuel Cell Gas Processing WP 2: Year 1 Milestones performance 200 mW/cm 550°C external electrical connections butane conversion rate > 90% post-combustor with gas oxidation > 98% battery expert industrial partner thermal insulation concept with T inside 550°C, T outside 50°C, <10 cm 3 structures for validation critical points thermal system demonstrator with simulated 2 W heat source

WP 2: Gas Processing Unit 4 Strictly Confidential Main Achievement after 12 Months Optimized butane reforming performance at 600˚C! Hydrogen Yield: month 12 Month 6

WP 2: Gas Processing Unit 5 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 6 Strictly Confidential Our Main Task in this Project FC System: Reformer: Post Combustor (PC):

WP 2: Gas Processing Unit 7 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 8 Strictly Confidential WP 2.1: Reformer Main Tasks: Understanding the butane reforming at low temperature (600˚C)? –Experiments with packed bed reformer influence of plugs is significant activation/deactivation of catalyst Reforming with the disk reactor: –Coating of the disk reactor –Influence of sealing –Activation/deactivation of catalyst New challenge –Modified product specification (from 1 W to 2.5 W power output) →Build-up of modified test rig

WP 2: Gas Processing Unit 9 Strictly Confidential Month 12: Milestones (MS) month 12: reformer demonstrator with significant butane conversion 600°C and stable for feeds of 0.02 to 0.5 g/h butane incl. gas chromatography (fabrication: NTB, testing: LTNT) –Optimized experiments: packed bed reformer –Modified design in progress (disk reactor) 

WP 2: Gas Processing Unit 10 Strictly Confidential Experimental Results Comparison: Packed bed reactor –Empty tube –Reformer with plugs 'O' (Al 2 O 3 /SiO 2, old) –Reformer with plugs 'N' (SiO 2, new) –Thermodynamic equilibrium

WP 2: Gas Processing Unit 11 Strictly Confidential Reactor Performance Butane conversion for T > 450 °C: →high η for 'plugs N' for T < 450 °C: →high η for 'plugs O' η of empty tube is low →effect of catalyst at T = 600 °C: →η = 69.2 % for 'plugs O' →η = 93.0 % for 'plugs N' POX TOX Total Oxidation (TOX):C 4 H O 2 →5 H 2 O + 4 CO 2 Partial Oxidation (POX):C 4 H O 2 →5 H CO

WP 2: Gas Processing Unit 12 Strictly Confidential Reactor Performance Hydrogen Yield for T > 450 °C: →high ψ for 'plugs N' for T < 450 °C: →high ψ for 'plugs O' ψ is higher than equilibrium at T = 600 °C: →ψ = 45.5 % for 'plugs O' →ψ = 86.6 % for 'plugs N' POX TOX TOX: C 4 H O 2 →5 H 2 O + 4 CO 2 POX: C 4 H O 2 →5 H CO

WP 2: Gas Processing Unit 13 Strictly Confidential Outlet composition Reformer with plugs 'N' (SiO 2, new) Outlet composition: at T = 600 °C: –X H2O = 4.6% –X H2 = 23.0% –X CO = 13.2% →Enhanced FC performance if X H2O ≈ 5% POX TOX → Inlet conditions of FC to NMW / EPFL

WP 2: Gas Processing Unit 14 Strictly Confidential Disk reactor Experimental results of Disk reactor –Coating: Rh (sputtered by NTB) –T = 600°C, d disk = 8 mm, GSV = 25 s -1 PBR DR PBR DR Reason: Sealing? Coating? Butane Conversion: Hydrogen Yield: Alternative: Filling disk space with catalyst particles (packed bed)

WP 2: Gas Processing Unit 15 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 16 Strictly Confidential WP 2.2: Post Combustor (PC) Purpose of PC: Catalytic oxidation of (toxic, flammable) exhaust gases –e.g. C 4 H O 2 → 4 CO H 2 O –e.g. CO O 2 → CO 2 Several studies in literature –Choice of catalyst and support: (Pt Ce 0.5 Zr 0.5 O 2 ) PC design similar to reformer (constraints: stack integration) Composition of gas at inlet? Modified product specification

WP 2: Gas Processing Unit 17 Strictly Confidential Milestones (MS) month 12: first preliminary post-combustor demonstrator aiming for significant oxidation 600°C and stable for feeds of 0.02 to 0.5 g/h butane (fabrication: NTB, testing: LTNT) –Modified product specification (from 1 W to 2.5 W power output → Modified test rig) –Inlet gas composition not known (CO, CH 4, C 4 H 10 conversion in Fuel Cell?) –Reforming with disk reactor not yet satisfied –Catalyst particles are active (and already produced by LTNT) W. J. Stark, J. D. Grunwaldt, M. Maciejewski, S. E. Pratsinis, A. Baiker, "Flame-made Pt/ceria/zirconia for low- temperature oxygen exchange", Chem. Mater., 17 (13) (2005).  ongoing

WP 2: Gas Processing Unit 18 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 19 Strictly Confidential WP 2.3: Integration and Testing month 12: delivery of first reformer and post-combustor designs aiming for compatibility with heat exchanger and hot module processing (LTNT) –Final design: disk reactor –Initial specifications: dimensions determined –Altered Specifications: Dimensions to be determined   ongoing 

WP 2: Gas Processing Unit 20 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 21 Strictly Confidential Validation of Milestones and Deliverables  WP 2.3: Integration and Testing Month 12:delivery of first reformer and post-combustor designs aiming for compatibility with heat exchanger and hot module processing (LTNT) WP 2.2: Post-combustor Month 12:first preliminary post-combustor demonstrator aiming for significant oxidation 600°C and stable for feeds of 0.02 to 0.5 g/h butane (fabrication: NTB, testing: LTNT) WP 2.1: Reformer Month 12:reformer demonstrator with significant butane conversion 600°C and stable for feeds of 0.02 to 0.5 g/h butane incl. gas chromatography (fabrication: NTB, testing: LTNT)   ongoing Previous Milestones and Deliverables: all fullfilled 

WP 2: Gas Processing Unit 22 Strictly Confidential Summary of Results Optimized butane reforming at low temperatures (PBR) Ongoing butane reforming experiments with DR Active catalyst particles for Post-Combustor DR design for integration into hot module

WP 2: Gas Processing Unit 23 Strictly Confidential Overview Our Main Task in this Project WP 2.1: Reformer WP 2.2: Post-Combustor WP 2.3: Integration and Testing Validation of Milestones Next Steps

WP 2: Gas Processing Unit 24 Strictly Confidential Next steps (Year 2) WP 2.1: High performance of disk reactor at T = 600°C: Butane conversion > 80%, hydrogen selectivity > 60% –(Coating in collaboration with NTB and NMW) WP 2.1: Long-term stability tests of reformer at T = 600°C: Butane conversion loss < 10% (after 10 h steady state) WP 2.2: Improved performance of post combustor: exhaust gas oxidation > 98% at T = 600°C and 0.7 g/h butane feed –(Inlet conditions for PC from NMW and EPFL) WP 2.3: Integration of reformer and PC into hot module –(Constructal constraints from NTB and ZHW) NMW NTB NMW NTB

WP 2: Gas Processing Unit 25 Strictly Confidential Next steps (Year 3 / Year 4) WP 2.1: Optimized performance of disk reactor at T = 550°C: Butane conversion > 90%, hydrogen selectivity > 75% –(Inlet gas composition to NMW / EPFL) WP 2.1: Start-up stability tests of reformer: Butane conversion loss < 10% (after 5 cycles from 25°C to 600°C) WP 2.2: Optimized performance of PC at T = 550°C: CO conc. < 25 ppm (TLV, ACGIH). –(Operation parameters from NMW / EPFL, ZHW / NTB) WP 2.2: Start-up stability tests of PC: CO conc. < 25 ppm (after 5 cycles from 25°C to 600°C) NMW NTB

WP 2: Gas Processing Unit 26 Strictly Confidential Questions ? Optimized butane reforming performance at 600˚C! Hydrogen Yield: month 12 Month 6

WP 2: Gas Processing Unit 27 Strictly Confidential Validation of Milestones and Deliverables   WP 2.1: Reformer Month 3:first reformer design available (LTNT) Month 6:modelled and evaluated reformer based on 0.3 g/h butane in 2 cm 3 with T max difference 50°C (reformer modelled for methane): effect of thermal conductivity of the reformer walls on the reformer process, microchannels coated with catalyst vs. porous catalyst (LTNT)   WP 2.2: Post-combustor Month 3:first preliminary post-combustor design available Month 6:improved designs of post-combustors aiming for 0.3 g/h butane feed, fully oxidized in 1 cm 600°C and max. pressure drop of 3 Pa (LTNT)   WP 2.3: Integration and Testing Month 3:design of test rig available (LTNT) Month 6:test rig for reformer and post-combustor for GPU performance incl. gas chromatograph (LTNT) Deliverables: Month 3: reformer design from LTNT  NTB for evaluation Month 6: final reformer design from LTNT  NTB for fabrication Deliverables: Month 6:designs of post-combustor from LTNT  NTB for fabrication Deliverables: Month 3: design from LTNT  NTB Month 6:NTB samples  LTNT (P. Müller checks whether possible in month 6)     