Hydrogen Production with Mixed Protonic-Electronic Conducting Perovskite Membranes
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1 ydrogen roducon wh Mxed roonc-elecronc Conducng erovske Membranes Erc D. achsman UF-DE gh Temperaure Elecrochemsry Cener Deparmen of Maerals Scence and Engneerng Unversy of Florda Ganesvlle, FL 36 UF-DE TEC UF-DE TEC
2 ulne Inroducon Fundamenals and Maerals Developmen Membrane eacor Fabrcaon and esuls ecen Membrane Maerals Advances Conclusons UF-DE TEC
3 Concep - Auohermal Caalyc Membrane eacor for roducon of ure C N-SrCe 3 porous ubular suppor Suppor for hydrogen membrane N caalyzes endohermc seam reformng or waer gas-shf reacon SrCe -x x 3-δ dense hydrogen membrane Mxed proon-elecron conducor ~0 µm dense layer xygen ranspor membrane Exohermc oxdaon of hydrocarbon feed gas Ulmaely can produce pure from any hydrocarbon feed sock: Naural gas Coal based syn gas Bomass UF-DE TEC
4 Cos of ydrogen roducon from Naural Gas* C = C /C C ~ 0.0C$/m 3 ~$0.5/m 3 ~0.05 /ler * Assumes 00% converson and selecvy, ar and waer are free, and gnores capal cos UF-DE TEC
5 DE s Fuure Gen ydrogen and elecrcy co-generaon from coal Zero emssons and C capure ydrogen roducon from Fossl Fuels wh roon and xygen-ion Transpor Membranes, E. D. achsman and M. C. llams, Inerface, Volume 3, No.3, Fall 00 UF-DE TEC
6 ulne Inroducon Fundamenals and Maerals Developmen Membrane eacor Fabrcaon and esuls ecen Membrane Maerals Advances Conclusons UF-DE TEC
7 XIDE-IN CNDUCTING MIEC s ermeaon Membrane arally xdzed ydrocarbon Effluen C, Cnm Vo h N, N ydrocarbon Feed σ and σ e of La 0.8 Sr 0. Co 0.8 Fe 0. 3-d Teraoka, e al (998) J of La 0.6 Sr 0. Co 0.8 B 0. 3-d Teraoka, e al (998) Ionc and elecronc conducvy resuls n permeaon lmed by oxde-on conducvy σ Vo UF-DE TEC
8 XIDE-IN vs. TNIC CNDUCTIN M M x x V xygen ons jump from a flled ( x ) o a vacan (V ) se -bonded proons form an group ( ) roons move around x and jump o neghborng x UF-DE TEC
9 TNIC vs. XIDE-IN CNDUCTS ermeaon Membrane ydrogen Depleed Effluen C, C+ e o C,, C arally xdzed ydrocarbon Feed SrCe 3-δ layer N-GDC porous suppor Iwahara, e al. σ and σ e of La 0.8 Sr 0. Co 0.8 Fe 0. 3-d Teraoka, e al (998) roonc conducors have comparable onc conducvy bu neglgble elecronc conducvy flux lmed by elecronc conducvy (σ e ) UF-DE TEC
10 Addng Elecronc Conducvy o a roon Conducor Add elecronc conducvy by dopng Ce se wh mulvalen caon (M 3+/+ ) ha can be reduced o + M Ce = M Ce + e (n-ype conducon) E. D. achsman and N. Jang, cober, 00, U.S. aen No. 6,96, Mach onc rad for hase sably roon conducvy > 3+/+ Conducvy of BaCe -x M x 3-d as a funcon r M, Iwahara e al (993) UF-DE TEC
11 Flux elaonshp J // // T T =! # ln +! ( + / / / ) ln d # d V V e L F F roon flux across calculaed usng agner equaon: Assumes ha bulk dffuson s rae lmng sep σ s he oal conducvy σ = z q u, ( =, V, e ) Transference number, = σ / σ gh flux requres boh hgh proonc and hgh elecronc conducvy F s Faraday s consan L s he membrane hckness Inegrae boh and poenal gradens UF-DE TEC
12 UF-DE TEC Complex Defec Equlbra n p!! V! / Ce // Ce 6 3 { 6 3 { 6 3 ) ( 6 3 { 6 3 { A Ce // = { { { 3 { A Ce // = 6 3 { A 6 3 { A 6 3 { A 3 { { A // / Ce Ce = 6 3 { A { { { Ce / = { A 8 { 8 { { 8 { 8 { A Ce / = { { { A! { { { A! 8 { A 8 { A { A 8 { A // Ce = 8 { A { { A Charge Neuraly = V n // = V Ce = n / = V Ce A p << A p << A p >> A p >> // = V Ce / = Ce // = Ce // = Ce p Ce = /
13 Modelng Defec Equlbra and Transpor -effec of,, S. J. Song, E. D. achsman, S. E. Dorrs, and U. Balachandran, Sold Sae Ioncs, 9, -0 (00). UF-DE TEC
14 Modelng Defec Equlbra and Transpor σ = z q u UF-DE TEC
15 Selecon of Dopan - Conducvy as a Funcon of n-ype p-ype BaCe 0.85 Gd Neglgble n-ype elecronc conducvy excep a very hgh emperaure >000 C N. Bonanos (99) log σ (S/cm) -.6 ) -.65 m c / S -.7 ( g o! l C 600 C BaCe Sgnfcan n-ype elecronc conducvy a much lower emperaure and hgher J. hodes and E.D. achsman (00) log o UF-DE TEC
16 Flux elaonshp J // // T T =! # ln +! ( + / / / ) ln d # d V V e L F F Flux ~ /membrane hckness (L) YDGEN FLUX (cc/cm -mn) % 0.75 mm 90%.00 mm 90%.00 mm TEMEATUE ( o C) YDGEN FLUX (cc/cm -mn) o C 800 o C 750 o C /TICNESS (mm) A hgh emperaure (>750 C) permeaon s bulk ranspor conrolled Flux s lnear wh /L A lower emperaure permeaon s surface knec conrolled UF-DE TEC
17 ulne Inroducon Fundamenals and Maerals Developmen Membrane eacor Fabrcaon and esuls ecen Membrane Maerals Advances Conclusons UF-DE TEC
18 ydrogen Membrane Cell Fabrcaon Co-frng Slurry Snered coang suppor hydrogen for and membrane hn hn cell flm flm UF-DE TEC
19 Fabrcaon of Membrane eacor UF-DE TEC
20 ydrogen Membrane Evaluaon All ubes are connuously leak checked by Ar racer n feed gas UF-DE TEC
21 ydrogen ermeaon and Leak Tesng Confrms membranes are leak free Capable of producng 00% pury UF-DE TEC
22 ydrogen ermeaon ydrogen flux ~ / UF-DE TEC
23 ydrogen ermeaon (am) average value Acvaon energy,e (ev) Acvaon energy of ~0.9 ev ndcaes flux lmed by σ e σ acvaon energy ~ 0.5 ev UF-DE TEC
24 ydrogen ermeaon Membrane ubes produce 7 cc/mn of pure -3% balance Ar / SrCe /e UF-DE TEC
25 ydrogen ermeaon Area normalzed membrane flux comparable o bes n leraure. owever -3% balance Ar / SrCe /e balance e / SrCe 0.95 Tm / 0% balance e S. Cheng, V.. Gupa, and J. Y. S. Ln, Sold Sae Ioncs 76 (005) 653. % -3% balance e / N-BaCe 0.8 Y 0. 3 / N wh 00ppm C. Zuo, T.. Lee, S.-J. Song, L. Chen, S. E. Dorrs, U. Balachandran, and M. Lu, Elecrochem. Sold-Sae Le., 8 (005) J35 UF-DE TEC
26 ydrogen roducon C / ~ ure produced drecly by nernal seam reformng C flux even hgher han from comparable feed UF-DE TEC
27 ydrogen roducon Converson (%) h permeaon hou permeaon Thermodynamc calculaon ermeaon ydrogen producon and ermeaon Flux (cc/mn) Temperaure ( o C) aer gas shf reacon: C + -> C + 3% C and balance e Sold lnes are /C=, dashed lnes are /C UF-DE TEC
28 ulne Inroducon Fundamenals and Maerals Developmen Membrane eacor Fabrcaon and esuls ecen Membrane Maerals Advances Conclusons UF-DE TEC
29 Conducvy of -doped SrCe o C Log σ roon (Scm - ) o C 700 o C 600 o C Acvaon Energy 0 mol% 0.9 ev 5 mol% 0.5 ev 0 mol% 0.87 ev Dopng concenraon of on SrCe 3 (mol %) Toal conducvy maxmum a ~0% UF-DE TEC
30 roon vs. Elecron Conducvy - roon Conducvy - Elecron Conducvy o C 900 o C Log σ roon (Scm - ) o C 700 o C 600 o C Log σ Elecron (Scm - ) o C 700 o C 600 o C Dopng concenraon of (mol %) Dopng concenraon of (mol %) Increasng concenraon: Decreases σ Increases σ e UF-DE TEC
31 Increased Elecronc Transference Number roon Transference number roon 5 roon 0 Elecron 0 Elecron 5 = e # = + # e # e + # e 0. Elecron Temperaure ( o C) flux lmed by elecronc conducvy UF-DE TEC
32 Conclusons gh emperaure proonc conducors offer remendous poenal for producon Addng elecronc conducvy sgnfcanly ncreases flux Demonsraed permeaon flux of ~0 cc/mn flux s proporonal o / flux s lmed by elecronc conducon Demonsraed pure producon from nernal seam reformed C Demonsraed pure producon from waer-gas-shf reacon Increased producon of membrane reacor - La Chaler Increasng -dopan concenraon wll sgnfcanly ncrease permeaon and producon Demonsraed >0X ncrease n e Should resul n 6 ler/hr producon per ube UF-DE TEC
33 Acknowledgemens NASA Conrac NAG3-930 DE TEC Conrac DE-AC05-76L0830 eesung Yoon Takeun h Janln L Sun Ju Song Jame hodes UF-DE TEC
34 ydrogen roducon, Transpor, and Sorage Symposum B The Elecrochemcal Socey Chcago, May 6-, 007 Absracs should be submed va he ECS webse by January 3, 007. Commens and nqures abou he symposum may be sen o he organzers: E. D. achsman, Unversy of Florda, ewach@mse.ufl.edu M. C. llams, NETL, mark.wllams@nel.doe.gov M. eben, NEL, Mchael_heben@nrel.gov A. Manvannan, NETL, manvana@nel.doe.gov B.. Maupn, U.S. Deparmen of Energy, paul.maupn@scence.doe.gov C. V. aman, Illnos Insue of Technology, raman@.edu UF-DE TEC
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