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SMARTCAT Report Summary

Project ID: 325327
Funded under: FP7-JTI
Country: France

Periodic Report Summary 2 - SMARTCAT (Systematic, Material-oriented Approach using Rational design to develop break-Through Catalysts for commercial automotive PEMFC stacks)

Project Context and Objectives:
The present consortium will build a new concept of electrodes based on new catalyst design (ternary alloys/core shell clusters) deposited on a new high temperature operation efficient support. In order to enhance the fundamental understanding and determine the optimal composition and geometry of the clusters, advanced computational techniques will be used in direct combination with electrochemical analysis of the prepared catalysts. The use of deposition by plasma sputtering on alternative non-carbon support materials will ensure the reproducible properties of the catalytic layers. Plasma technology is now a well-established, robust, clean, and economical process for thin film technologies. Well-defined chemical synthesis methods will also be used in order to quickly defining the best ternary catalyst composition. MEA preparation and testing, MEA automated fabrication in view of automotive operation will complete the new concepts of catalysts with a considerably lowered Pt content (below 0.1 mg cm-2 and down to 0.01 mg cm-2) and supports for delivering a competitive and industrially scalable new design of PEMFC suitable for automotive applications.
The SMARTCat project is thus organized to provide new trimetallic catalysts (WP2) deposited on new support materials (WP3) expected to operate at high temperatures suitable for car applications. This involves a relevant high temperature membrane, which is developed especially for the project (WP4). Emphasis is also given to automated membrane electrodes assembly with these new materials (WP4). Special care is further devoted to fuel cell tests in automotive conditions with selected MEAs (WP5) in agreement with harmonization protocol discussed with the JRC-IET.
SMARTCat will thus address the following objectives:
- Deliver specifications/requirements for reaching the technical goals as a roadmap.
- Design an efficient new catalyst architecture
- Establish a support selection criteria based on physico-chemical characterization and modelling for defining the most suited electrode support to the defined catalytic system
- Assess the robustness regarding operation conditions and fuel cell efficiency
- Enable to automate the MEA production using state of the art (< 100°C) and high temperature membranes (120°C)
- Build efficient short-stack required for competitive automotive fuel cell operation
- Low cost process and low Pt content will dramatically reduce the fuel cell cost, and which will lead to economically suitable fuel cells for automotive application

Project Results:
a) New trimetallic catalysts
The modelling of trimetallic structures has shown 0.05 eV reduction of OH binding energy on PtAuCo and PtAuNi render them highly active for ORR. Three interesting new candidates, i.e. PtAuCr, PtAuCu and PtAuZn, were identified as displaying high expected ORR activity and the latter two also a stabilizing effect from the Au-Cu and Au-Zn interaction
Addition of small amount of Au is found to increase the stability of the catalysts. Better activity both for exchange current density j0 (mA cm-2), kinetic current density (mA cm-2 @ 0.9V), mass activity (A.gPt-1 @ 0.9V), than Pt alone. The targeted exchange current density in Tafel slope region of 60mV.decade-1 of 10-3 mA cm-2 was reached for Pt3NiAu, Pt3CuAu and Pt3AuCo. Mass activities, at 0.1. mg cm-2 Pt load, are ordered as Pt3NiAu > Pt3NiAu2 > Pt3CoAu2 > Pt3CuAu> Pt3AuCo> Pt5PdAu, Pt3CuAu2 > Pt, respectively. Kinetic current densities jk follow the same trend. RRDE of sputter deposited Au@Pt3Ni of core shell ternary catalysts at 0.6 and 0.01 mgPtcm-2 loadings has been carried out.
Deviation: Ultimate Pt loadings should not be below 0.05 mgPtcm-2 for keeping the target j0 ≥ 10-3 mAcm-2, both by chemical and sputtering means.

b) New supports for high temperature operation.
Computational DFT techniques have been carried out for studying interactions between oxygen vacancy (Ov), doping Sb atom in SnO2, effect of Sb doping on the interaction between small Pt clusters and Ov-SnO2(110) surface. Segregation and transport properties at antimony-doped tin oxide (ATO)/Pt interfaces and at niobium-doped tin oxide (NTO)/Pt interfaces have been examined as well as transport properties of multiple-doped tin oxide/Pt interface. This work has been successfully extended to probe stability and ORR ternary catalysts Pt3NiAu and Pt3CuAu. At low RH the conductivity of the ATO materials has a slight tendency to increase with increasing temperature while at high RH the ATO composite electrodes show a strong increase in conductivity. RRDE and single cell (5 cm2 of selected Pt3NiAu catalysts with the highest activity on ATO/NTO FSP support is in progress as well as ATO/NTO sputtering deposition target fabrication and successive sputtering deposition of ATO/NTO and Pt3NiAu chosen ternary catalyst.

c) Optimization and demonstration of MEA
High temperature polymer membrane is currently developed within the project. Problems and delays were encountered at the materials supplier in generating the required monomer and in scaling-up the polymerization. 1 kg of polymer was finally made and partly used up in experimentation aimed at free-standing, acid-activated membranes. Such acid-activated film is a soft, tacky rubber. We thus recently changed our aims into integrating film- and MEA making and observed dry-conditions,150 oC, proton conductivities in (dummy) MEAs of 100...350 mS/cm depending on doping level in line with the original targets and with historical work on Twaron paper impregnated with our polymer system. Work on this direct MEA making is at a very early stage and at small scale (8 cm2).
Deviation: Supported films will be preferred instead of free-standing.

d) Fuel cell testing
During this period, reference performances obtained with a PEMFC stack developed for automotive application have been provided to WP2 and WP3. This stack was composed of stamped metallic bipolar plates with an active surface area of 220 cm². A complete description of stack was provided to SMARTCat partners during this period. Large area 220 cm2 MEA have been assembled with sputtered Au@Pt3Ni cathode at 0.1 and 0.01 mgPtcm-2 loading. Fuel cell testing is in progress in condition defined by the JRC harmonization protocol. Thus unoptimized MEA with Pt3NiAu ternary catalysts has been tested vs temperature up to 120°C. Max delivered power density is 730 mW cm-2 using PFSA membrane.
Deviation: Short stack tests will be delivered between M41 and M46.

Potential Impact:
SMARTCat project will work on:
• Heavily reducing and optimizing the catalyst platinum loading and hence obtain a substantial cost-reduction
• Catalyst and catalyst stability so as to improve the lifetime of the fuel cell.
• Innovative work on corrosion resistant support materials improving significantly the durability of the fuel cell.
• Compatibility of the new electrode concept with high temperature membranes extending the temperature range of fuel cells for automotive application.
• MEA optimization and manufacturing processes allowing a rapid access to the automotive market.

Scientific and technical impact:
o The coupled modelling/characterisation of tri-metallic clusters morphology and ORR will provide advances in catalysis understanding and will give rise to new developments in the field.
o Highly efficient tri-metallic catalytic nanostructured layers with ultralow Pt loading will be a worldclass breakthrough
o The obtained improved stability of the electrodes (support/catalyst combination) and robustness of MEA leading to increased operation time (up to 5000h) will be an outstanding result.
o The successful new catalyst concept will represent key result for the introduction of fuel cell cars to the mass market as it will incorporate a significant cost-reduction of approximately 35% of the MEAs, considering mass production, and increase MEA lifetime whilst being high-performing.
o The project will prove the concept and compatibility of new HT membranes particularly interesting for the automotive industry
o Highly efficient MEA manufacturing processes at pre-industrial levels will be developed including the new catalyst concept.
o Transfer of innovations to larger scales (corresponding to market needs) is rare since it is expensive and technically difficult. SMARTCat will provide upscaling of HT membranes and automotive MEAs at industrial scales.
o Finally, SMARTCat will increase the offer of high performing and low catalyst loaded PEMFCs for automotive applications.
Impact on European industry and economy:
The main economical impacts are related to the significant cost reduction expected for the new electrode concept, which will be achieved by reducing significantly the Pt-content. Current Pt-loadings will amount to as much as 35% of the total cost of MEA taking into account the cost reduction of mass production and assuming no increase in Pt cost due to the high market demand. Very encouraging results with a significant reduction in Pt (>70%) (M. Mougenot, A. Caillard, P. Brault, S. Baranton, C. Coutanceau, High Performance Plasma Sputtered PdPt Fuel Cell Electrodes with Ultra Low Loading, International Journal of Hydrogen Energy 36 (2011) 8429-8434) has recently been shown by the CNRS with the potential of revolutionizing the catalyst concept for PEMFC. Nevertheless, the intrinsic performance, the stability and the durability of the electrode still need a lot of attention to reach the targets of automotive applications. SMARTCat will address all these issues in a systematic way leading to a new electrode concept with a significant cost reduction but also which exhibits high performance and excellent durability.
. Also, the new generated knowledge transferred from SMARTCat partners to major companies in the transport sector will enable to speed up the market introduction of the fuel cell technology for automotive applications.
A true international competition is starting and SMARTCat will place Europe at the very forefront in the field of PEMFCs for automotive applications. The automotive industry in Europe will highly benefit form the innovative and groundbreaking technologies generated from the project. The partners of the consortium will be acknowledged within their expertise at a European and even international level enabling an extension of both collaborations and market range.

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