Catalyst Development Needs
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1 Catalyst Development Needs (presented at the NSF Workshop in Washington DC, Nov , 2001) Hubert Gasteiger 1) Mark Mathias 2) Susan Yan 3) Cathode Catalysts cathode related MEA performance losses cathode catalyst development requirements Anode Catalysts pure H 2 applications reformate: current status and development goals 1) hubert.gasteiger@gm.com; 2) mark.mathias@gm.com; 3) susan.yan@gm.com Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 1 by: Mark Mathias & Hubert Gasteiger
2 Effect of Cathode Loading on MEA Performance Experimental MEAs (CCMs): membrane/ionomer:» 50µm Nafion 112» solubilized 1100 EW Nafion catalysts:» 40%wt Pt/Vulcan ETEK catalysts» electrochemically active surface area (HAD of catalyst and MEA): 35 m 2 /g Pt» HAD for state-of-the-art Pt catalysts (at 40%wt Pt/carbon): 60-80m 2 /g Pt factor of 2-3 gain in Pt surface area diffusion media:» hydrophobized Toray with surface treatment MEA Testing: 50cm 2 and large active area (5kW short-stack) H 2 /air at s=2/2; performance evaluated after 15 mins./point determination of E loss contributions in H 2 /air MEAs Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 2 by: Mark Mathias & Hubert Gasteiger
3 ORR Kinetics (50cm 2, 40%Pt/Vulcan-ETEK, Nafion 112, pure O 2 ) Assume: No mass transport resistances (H +, gas) Negligible η H 2 ORR 1st order with respect to p O E IR-free =E cell + I. R Ω E eq -TS. log H 2 /O 2 at s=2/9.5 and 150kPa, T cell =80C, dewpts.=80/80c, 12mins./pt. i [A/cm 2 ] L[mg Pt /cm 2 ]. S [cm 2 /mg Pt ]. p O /0.40 mgpt/cm2 0.40/0.20 mgpt/cm2 EiR-free [V] mv/dec 0.40/0.10 mgpt/cm2 0.40/0.05 mgpt/cm2 δe IR-free δlog(i/l) = TS = 66 mv/dec i [A/mg Pt ] purely kinetic control in 100% O 2 Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 3 by: Mark Mathias & Hubert Gasteiger
4 Ex-Situ Catalyst Charact. MEA Performance Catalyst Utilization Catalyst Activity MEA: H 2 /O 2 at s=2/9.5 and 150kPa, T cell =60C, dewpts.=60/60c RRDE: 14µg Pt /cm 2 in 0.1 M HClO 4 at 100 kpa O 2 and 60C (LBNL) * Current Voltage (V) vs SCE RDE (0.1M HClO 4 ): 30+8m 2 /g CV in single cell : 33+5m 2 /g ca. 100% catalyst utilization EiR-free [V] i [A/mg 10 Pt ] good agreement between MEA performance and RRDE screening RRDE testing can benchmark catalyst development progress * U.A. Paulus, T.J. Schmidt, P.N. Ross, N.M. Markovic (Lawrence Berkeley National Laboratory, Berkeley, CA) Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 4 by: Mark Mathias & Hubert Gasteiger
5 Air vs. O 2 MEA Perf. - Origin of Transport Losses In the kinetic limit: O 2 log δe IR-free δlogp O 2 100% 21% Air: = TS = 0.68 E O2 air = 45mV EiR-free [V] H 2 /O 2 (Air) at s=2/9.5(2.0) and 150kPa, T cell =80C, dewpts.=80/80c kinetic.-limited transport-limited 0.40/0.40 mgpt/cm2 0.40/0.10 mgpt/cm i [A/cm 2 ] Purely kinetically limited below 0.1A/cm 2 Transport limited above 0.1A/cm 2 no difference between 5 and 20µm electrode H + tx limitation unlikely O 2 transport resistance in: gas-phase (pores in electrode or diffusion media)? solid/liquid phase (ionomer, H 2 O film)? Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 5 by: Mark Mathias & Hubert Gasteiger O 2 Air
6 Voltage Loss Contributions in H 2 /Air Assumptions: H 2 /Air at s=2/2 and 150kPa, T cell =80C, dewpts.=80/80c negligible η H 2 only E loss,kinetic at 0.02 A/cm 2 Tafel slope of 66 mv/dec voltage loss [V] /0.4 mg Pt /cm 2 ORR kinetics losses (i 0 =1.7x10-9 A/cm 2 Pt) total ohmic losses mass tx losses i [A/cm 2 ] major η-losses for ORR (0.44V at 1 A/cm 2 37% η-loss (E eq 1.184V)) R Ω,membrane (ca. 0.1 S/cm) for 50 25µm membrane: remaining 0.025V membrane loss (no dry-out effect) note: total ohmic E loss at 1 A/cm V (ca V add. R contact ) unaccounted for tx-losses of ca. 0.07V at 1 A/cm 2 (H +, O 2 ) Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 6 by: Mark Mathias & Hubert Gasteiger
7 Maximum 150kPa/80C H 2 /Air Performance at 1 A/cm 2 Assumptions: future improvements in stable Pt dispersion: m 2 /g Pt (50% dispersion!) L cathode from mg Pt /cm 2 without E loss (S Pt L Pt =const.) η cathode at 1 A/cm 2 and 0.1 mg Pt /cm V R ohmic of 0.050V at 1 A/cm 2 (25µm membr., low R contact, no membrane dry-out) no tx-losses E eq at 80C 1.185V maximum E cell of 0.695V at 1 A/cm 2 and 0.1 mg Pt,ca /cm W/cm 2 at 59% efficiency ca g Pt,cathode /kw el (14 g Pt,cathode /100kW el ) ca g Pt,total /kw el for 0.1/0.1 loading 28 g Pt,total /100kW el Conclusions - Fundamental Research Needs: improvement in stable Pt dispersion (currently 30 m 2 /g Pt ) improved Pt-alloy or non-pt cathode catalysts reduction of MEA transport losses (H +, O 2 ) to zero Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 7 by: Mark Mathias & Hubert Gasteiger
8 Background to Cathode Catalyst Development Efforts 70 s and 80 s: major players:» univ./inst.: Yeager (CWRU), Appleby (Texas A&M), Taylor (Giner), Srinivasan (Texas A&M), Anson» industry: IFC/UTC, various at Johnson Matthey investigated systems:» Pt-transition metal alloys (mainly PAFC) ca. 2x activity over Pt (demonstrated in PAFC)» Pt, Pd, Au alloys no enhancement over Pt» macrocycles (porphyrines, phtalocyanides): 4 N coord. around Co, Fe not stable» fried macrocycles: pyrolysis of macrocycles approaches Pt act., poor stability 90 s to date: very few players:» LBNL: fundamental electrocatalysis work (Pt-alloys, Pd-skins on Pt)» Symyx: initiated very promising combinatorial method development» Penn State: combinatorial approach, but method still being developed» very few other academic institutions and government labs» INRS (Canada): new approach to fried macrocycles» several industrial catalyst developers» some research with carbon structures: nanotube or whisker support most public funding focuses on hardware and MEA manufacturing! Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 8 by: Mark Mathias & Hubert Gasteiger
9 Effect of Anode Loading on H 2 /Air Performance In-house expts. with varying anode Pt-loadings at 150kPa/80C no E cell difference between 0.20 and 0.40 mg Pt /cm 2 10 mv E cell -loss difference for mg Pt /cm 2 10 mv E cell -loss difference for mg Pt /cm 2 HOR kinetics begin to impact H 2 /air performance improved stable Pt dispersion mg Pt /cm 2 without E loss Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 9 by: Mark Mathias & Hubert Gasteiger
10 Reformate/Air Performance - Anode Requirements Status for <25mV loss (40%H 2 /N 2 40%H 2 /20%CO 2 /N 2 +CO) 100ppm CO + 2% air-bleed at 80C with 0.4mg PtRu /cm g PtRu /kw el (assuming 0.7 W/cm 2 ) 60g PtRu /100kW el development of more CO/CO 2 -tolerant catalysts required Reformate catalyst development goals 100ppm CO + 2% air-bleed at 80C with 0.1mg PtRu /cm g PtRu /kw el (assuming 0.7 W/cm 2 ) 15g PtRu /100kW el 1000ppm CO + 2% air-bleed at 80C with 0.1mg PtRu /cm 2 reduced CO clean-up step complexity 10000ppm CO + 2% air-bleed at 80C with 0.1mg PtRu /cm 2 no CO clean-up beyond WGS required (η-gain!) Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 10 by: Mark Mathias & Hubert Gasteiger
11 Catalyst Development Needs - Conclusions Cathode Catalysts performance of a perfect MEA will not reach targets with current catalysts catalyst development requirements:» Pt catalysts with stable high dispersion (50%) other supports» Pt-alloy catalysts with improved performance» non-pt catalysts catalyst development does NOT necessarily require MEA testing! Anode Catalysts ultra-low Pt loadings with pure H 2 require stable high dispersion catalysts current CO-tolerance must be maintained at reduced loadings (0.1mg Pt /cm 2 ) long-term goal of 1000ppm CO-tolerance Date: Nov. 12, 2001 File: NSF Workshop - Catalysts - Nov , revised.ppt page: 11 by: Mark Mathias & Hubert Gasteiger
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