DELIVERABLES
WP1
 
- D1.1 - Project shared workspace implemented and operational - CONFIDENTIAL
To fulfil two fundamental internal project communication requirements: i) efficient exchange between partners of information about CRESCENDO project ii) decentralised and secured archiving of the documents generated, one independent and secured web-based communication tool: Project Shared Workplace – PSW has been implemented with a restricted access for project partners only. Among all the functionalities installed on this PSW, for now partners have a total access to the following tools: Document sharing and archiving ; Meeting organization ; General project communication ; Online working document ;  Project management.
The PSW maintenance is therefore an on-going activity that will go along with the project lifetime
- D1.2 - TRUST reporting year 2 - CONFIDENTIAL
The TRUST on-line data collection application was populated with results on single cell performance on H2/air of a membrane electrode assembly comprising a non-PGM cathode catalyst, and Pt anode catalyst.
- D1.3 - Mid-term progress report submitted - CONFIDENTIAL
Parts A and B of the RP1 progress reporting were submitted according to schedule.
- D1.4 - TRUST reporting year 3 - CONFIDENTIAL
The TRUST on-line data collection application was populated with results on single cell performance on H2/air of a membrane electrode assembly comprising a non-PGM cathode catalyst, and Pt anode catalyst.
- D1.7 - Progress Report M19-M36
Excellent technical progress has continued to be made towards the final fuel cell performance targets, with significant improvements made in the catalyst kinetic activity through new modifications to catalyst synthesis in WP3. In WP4, two non-PGM oxides have been identified as having a stabilising role in the fuel cell over the initial tens of hours of operation, and the use of ultra-low (μg) amounts of platinum – the most effective and durable means known to date – was further optimised allowing platinum loading to be even further reduced. Catalyst scale-up in WP5 was successful and catalyst ink and catalyst layer development with the scaled-up catalyst will be carried out in early 2021, and the resulting CCMs provided to WP2 for testing. Non-PGM anode catalyst development and catalyst ink formulation have progressed sufficiently well to allow planning for an all-non-PGM (anode and cathode) membrane electrode assembly.

 WP2
 
- D2.1 - Cell and system requirements and cell testing protocols
In this deliverable report the technical specifications for the CRESCENDO single cell components are presented. The specifications are based on the automotive requirements and operating conditions. In addition standard testing protocols and sensitivity tests are defined for the purpose of fair comparison between partners, while integrating European harmonised protocols where relevant.
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- D2.2 - Benchmarking commercial SoA non-PGM CCMs and catalyst
The results of benchmarking the performance of commercial PGM-free based CCMs are presented. The results are in good agreement between different partners, despite the use of different testing hardware. The commercial PGM-free CCMs exhibit lower performance than the project performance targets providing 0.15 A/cm2 @,418 V under operating mode 3, while the performance target is 0.6 A/cm2 @ 0,71 V. This report also provides the results of ex situ RDE electrochemical characterisation of the commercial Fe-N-C catalyst.
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- D2.4 - Cost and life cycle analysis and exploitation potential - CONFIDENTIAL
Deliverable D2.4 describes the cost assessment for the PGM-free stack, based on the assumptions for high volume production of 50,000 fuel cell stacks per year and using the stack design of earlier FCH JU project INSPIRE as baseline for the cost calculation. MEA production costs were estimated and the stack performance needed for the correlation to €/kW was calculated by using test results from small-scale single cell measurements. The cost assessment delivered a normalised stack cost that is significantly higher than the target value of 50 €/kW for automotive applications.

 WP3
 
- D3.1 - Site Density and Turnover Frequency of Selected Benchmark Catalysts
This deliverable report describes the benchmarking of four non-platinum group metal (non-PGM) containing catalysts, consisting of key performance metrics, such as electrocatalytic mass activity (MA), selectivity, site density (SD) and catalytic turnover frequency (TOF). SD and TOF were evaluated using in situ nitrate reduction and ex situ low temperature CO chemisorption in combination with rotating ring disk electrode (RRDE) measurements. The iron coordination environment was determined by 57Fe Mössbauer spectroscopy. Surface area and pore volume were determined from nitrogen adsorption isotherms. Electrochemical measurements were performed with a RRDE to determine the kinetic current and the selectivity of the catalysts to the oxygen reduction reaction (ORR). The properties of these benchmark catalysts will be used as a baseline to guide needs to increase the SD or TOF to reach the activity targets of the project, and to better assess the activity improvements realised with the new non-PGM catalysts prepared in CRESCENDO.
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- D3.2 - Promising non-PGM catalyst activity showing progress toward WP targets - CONFIDENTIAL
This report describes the development of novel non-PGM cathode catalysts in the first 12 months of CRESCENDO. New catalyst were developed with mass activity of 0.66 A/g @ 0.9 V and single cell current density on oxygen of 12.7 mA/cm2 @ 0.9 V.
- D3.3 - Electrochemical activity parameters of new catalysts showing progress toward project targets - CONFIDENTIAL
This report describes the development of novel non-PGM cathode catalysts in the first 18 months of CRESCENDO. New catalyst were developed with mass activity of 0.92 A/g @ 0.9 V and single cell current density on oxygen of 15 mA/cm2 @ 0.9 V.
- D3.5 - Final Report on WP Achievements in Terms of Activity of new Catalysts - CONFIDENTIAL
This report describes the developments in WP3 from project months 24 to 43 in terms of catalyst activity. The main focus in this period was on the catalyst down selection and synthesis upscale, as well as on the further characterization of already developed catalysts and support materials. The main achievements of WP3 include the down selection of a catalyst for upscale and testing in WP5 and WP2. The best performing catalyst at the end of the project achieved a power density of 0.42 W cm-2 at 0.6 V in H2/air, i.e. the final power density goal of the CRESCENDO, albeit at a lower voltage than the targeted 0.7 V.

 WP4
 
- D4.1 - Ex situ AST peroxide protocol definition and its application to selected benchmark catalysts
In this deliverable report a novel protocol is established to investigate the effect of H2O2 on the activity for O2 reduction of Fe-N-C catalysts. The novel protocol involves a continuous addition of a peroxide solution with a peristaltic pump. A well-known Fe-N-C catalyst was selected, for which the effect of H2O2 had previously been investigated by adding peroxide instantaneously. This former protocol may however have led to different effects than when peroxide is added continuously, the latter case better reproducing the conditions occurring in an operating PEM fuel cell. Several parameters of this peroxide-accelerated stress test were investigated, such as the rate of addition of peroxide and the pH. The results show that, for a same cumulative amount of peroxide per mass of Fe-N-C catalyst, a similar decrease in ORR activity is observed for the investigated Fe-N-C catalyst when applying either the novel (continuous addition of peroxide) or the former protocol (instantaneous addition of peroxide). The rate at which peroxide is added with the pump plays only a minor role on the deactivation, in the range investigated so far. The pH of the solution in which the Fenton reaction takes place has a role, with more acidic pH leading to slightly less active catalyst than when deionized water is used.
The novel AST with peroxide proved reproducible and allows an easy control of the cumulative amount of peroxide added and also the rate at which it is added. This protocol will now be applied to other FeNC catalysts (benchmarking study) and also to novel catalysts prepared in CRESCENDO.

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- D4.2 - Effect of addition of ROS on durability improvement - CONFIDENTIAL
A reference Fe-N-C catalyst, containing Fe mostly in the form of atomically-dispersed FeNx active sites for oxygen reduction reaction, was modified by addition of targeted solid-state catalytic ROS scavengers. The benefit toward improving the durability of the reference Fe-N-C material was assessed, first via ex situ peroxide degradation protocol (see D4.1). The results identify lower peroxide production and improved durability with a selected FeNC/additive composite. Future work will focus on more advanced functionalisation of FeNC to improve the additive dispersion and binding to FeNC, as well as verifying improved durability in fuel cell testing of such PGM-free composites.

- D.4.3 - Report on sacrificial organic compounds as ROS scavengers to actively protect Me-N-C catalysts against H2O2 - CONFIDENTIAL
A model Fe-N-C catalyst, containing Fe exclusively in the form of atomically-dispersed FeNx active sites for oxygen reduction reaction, was subjected to the ex situ peroxide degradation protocol (see Deliverable D4.1), in absence and then in presence of three different organic radical scavengers, which were selected for their reported antioxidant properties in the field of chemistry and biochemistry. The benefit toward improved stability of the reference Fe-N-C material after exposure to large amount of H2O2 was assessed by comparing the ORR activity of the Fe-N-C catalyst before and after the ex situ accelerated stress test (AST) peroxide protocol. Initial promising results were obtained with one of the organic radical scavengers. Its addition during the peroxide accelerated stress test resulted in reduced Fenton reactions on the model FeNC catalyst, as deduced from lower %H2O2 during ORR after the AST, when compared to the same FeNC catalyst in absence of the organic radical scavenger during the AST.

- D.4.4 - Durability of platinum-free cathode layers in single cell PEMFC - CONFIDENTIAL
The stabilisation of PGM-free catalysts (Fe-N-C and other metal-N-C) was investigated via the addition of solid-state scavengers for peroxide or reactive oxygen species in the cathode layer, or onto the M-N-C catalysts. ZrO2, zinc-molybdates and MnOx materials were investigated as stabilisers, as well as ultralow amount of Pt. The stabilisation effects induced by the co-catalysts were studied in rotating (ring) disk electrode set-up, ex situ with catalase and peroxidase tests, and in a PEMFC.


 WP5
 

- D5.1 - Identification of the main performance loss mechanisms seen in layers made from reference catalyst - CONFIDENTIAL
This deliverable report presents results obtained with the Reference hybrid 2% Pt/Fe-N-C catalyst. Layers were created with this catalyst and assembled into membrane electrode assemblies with an active area of 50 cm2. State-of-the-art membranes were used with good conductivity and a thickness of 15 mm. Pt/C was
used as an anode catalyst at a loading of 0.20 mg Pt/cm2. The Reference catalyst layer exhibited low performance, compared to state-of-the-art Pt/C cathode catalyst layers, and is currently 400 mV below the ultimate project target at 600 mA/cm2.
This report contains characterisation studies of the catalyst and a series of diagnostic experiments carried out in 50 cm2 fuel cells to gain better understanding of the limitations of the layers made with the Reference catalyst.

- D5.2 - Quantification of the performance improvement achieved by rational re-design of layers using the Reference catalyst - CONFIDENTIAL
This deliverable report presents a detailed optimisation of the cathode catalyst layer that has led to the highest performance in the project so far. This was achieved in 50 cm2 single cells using a second, scaled-up batch of the project Reference hybrid 2%Pt/Fe-N-C catalyst. It was observed that small changes in synthesis led to significant physical differences between the first and second batches of the project Reference catalyst. This was a significant learning exercise that highlights the difficulties in scaling up this type of catalyst. This report gives an in-depth characterisation of the properties of the catalyst and catalyst layers made from the project Reference catalyst, building on methods described in D5.1. It was deduced that a lack of porosity below 100 nm led to low performance at medium to high current densities. It was possible to improve performance, however, with the use of different solvent contents during the inkmaking step and with the addition of different additives. This approach was able to increase the porosity in the catalyst layer at

- D.5.3 - Most promising catalysts from WP3 and WP4 scaled up and shown to match performance of small batch samples - CONFIDENTIAL
This deliverable report presents the different catalyst variants developed in WP3 and WP4 and the selection criteria that identified the candidates for scale up in Task 5.3. From WP3, three FeNC type catalysts were identified and from WP4 three radical scavengers were also identified. In collaboration with the project partners, candidates for scale up at JMFC were selected based on activity, durability and ease of scalability. The team agreed to progress the CNRS (FeNC) cathode catalyst from WP3 with 1 wt% Pt added as a radical scavenger (from WP4). Precursors were sourced at JMFC for the synthesis of a 60-100 g batch size of the FeNC catalyst. JMFC and CNRS started a close collaboration to transfer the synthesis method. Some modifications were made to the CNRS method, mainly for compatibility with the equipment available at JMFC. The first iteration was successful and a 35 g batch was produced. The first batch of scaled-up catalyst was sent back to CNRS for characterisation and validation in the RDE and in MEA. After review of the results with CNRS, the scaled-up catalyst was qualified to progress towards MEA fabrication for activities planned in WP2 and, therefore, met project Milestone 6, ‘Go/no-go decision on catalyst scale-up for industrial-scale single cell with option for short stack’.

- D.5.4 - 50 cm2 active area CCMs fabricated using the most promising catalyst for testing in BMW hardware in WP2 - CONFIDENTIAL
This deliverable reports the optimisation of cathode catalyst layers using the CRESCENDO scaled up catalyst. A set of four different cathode designs were produced using two different coating methods. A series of experimental parameters such as loading, use of an additive and coating method were varied. The additive was aimed at increasing the catalyst layer porosity in the smaller pore region, i.e. <30 nm. The use of spray deposition allowed the creation of higher loading layers, circa 3 mg catalyst/cm2, with acceptable layer quality with respect to crack formation. On the other hand, the use of K-bar coating was better suited for lower loadings, i.e. 1 mg catalyst/cm2. The scaled-up catalyst outperformed the project reference catalyst in the kinetic (low current) region under H2/air. Using layer type 1 however, high mass transport losses were seen, thought to be due to low layer porosity. With layer type 2, the scaled-up catalyst clearly outperformed the reference catalyst, at the same loading and with the same layer configuration and was able to reach high current densities up to 1200 mA/cm2. This good result demonstrates the higher activity of the scaled-up catalyst in an appropriate layer configuration. Out of this work, a set of five different cathode designs were produced and sent to BMW as part of WP2.


 WP6
 
- D.6.1 – Non-PGM anode catalyst with improved performance - CONFIDENTIAL
This report describes the integration of Ni based bio-inspired molecular catalysts to porous electrode matrices for the development of non-PGM based anodes for the hydrogen oxidation reaction (HOR). Several electrode materials and deposition strategies were employed. These lead improved performance and set a new benchmark for heterogeneous molecular HOR, by reaching current densities of 130 mA cm-2 at 0.4 V vs RHE (30 mA cm-2 at 0.1 V and 25 A mgNi-1). Characterisation of the molecular based anode through RDE and FE measurements is also reported.

- D6.2 – Ultra-low PGM anode catalyst with improved resistance to CO poisoning - CONFIDENTIAL
This report describes the development of a novel ultra-low PGM anode catalyst with outstanding tolerance to carbon monoxide (CO) poisoning. When this newly developed catalyst was applied in the anode of a PEMFC, no performance degradation was observed even when cell was operated with hydrogen fuel containing 5000 ppm CO. The performance of this catalyst is closely matching the project targets and will be further optimised to enhance its absolute HOR activity. In parallel, floating electrode studies were carried out using Pt and PtRu catalysts to investigate the CO poisoning behaviour at ultra-low loadings and CO adsorption was modelled using Langmuir-Hill isotherm. It was found that at ultra-low loadings, both Pt and PtRu catalysts lose their activity significantly in the presence of CO. Model fitting revealed that 50% CO surface coverage of Pt is reached with a CO concentration of 14.7 ppm which is less than half of 35.4 ppm needed for PtRu. At a high CO concentration of 200 ppm, more than 90% Pt sites and over 80% PtRu sites are blocked resulting in almost their complete deactivation for hydrogen oxidation reaction (HOR).

- D6.3 – Report on activity, resistance to poisoning and stability under cell reversal conditions of down selected non-PGM and ultra-low PGM anode catalyst - CONFIDENTIAL
This report describes the characterisation of the down selected non-PGM and ultra-low PGM anode catalyst for the Hydrogen Oxidation Reaction (HOR) developed in the first part of the CRESCENDO project. The first part of the report describes the performances for hydrogen oxidation obtained with the Ni based bio-inspired catalyst at CNT modified electrode in aqueous acidic electrolyte (half-cell and floating electrode configuration) as well as in MEA configuration (hydrogen pump). The second part focuses on the characterisation of the ultra-low loading anode, tested in floating electrode configuration and directly in an H2-O2 fuel cell setup. 

 WP7
 
- D7.1 - Project Website
The CRESCENDO project website is designed to fulfil project communication and dissemination needs for the benefit of the whole scientific community and the public through relevant information including:
− project overall objectives, partner & work packages information
− project activities: news, meetings
− project progress: technical publications, conference presentations, public domain reports
− project resources: links, related events …
− project contact information and newsletter subscription
All the partners will collectively participate in the dissemination objective of the website by providing up-to-date information

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- D7.2 - Dissemination and knowledge management protocol - CONFIDENTIAL
This report presents the dissemination protocol for the CRESCENDO project, the procedure for “Open Access” to peer reviewed research articles, internal rules, information on support from the EU members and the strategy for Knowledge Management within the project.
- D7.3 – Dissemination and Communication bundle comprising a package of visual identity tools and project brochure, 2 publications in international journals, 4 conference presentations, 2 annual newsletters
During the first 24 months of the CRESCENDO project the consortium undertook various dissemination and communication measures. Target groups include industry, academia, government bodies and the public.
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- D7.4 - Organisation of an International Conference “Challenges for Zero Platinum for Oxygen Reduction and Hydrogen Oxidation"
CRESCENDO jointly organised with the H2020 CREATE project (http://www.create-h2020energy.eu) the second edition of the Electrolysis and Fuel Cell Discussions conference, EFCD2019, dedicated to catalysts with minimum amount of Critical Raw Materials, and in particular of Platinum Group Metals.
This highly successful international conference was held at La Grande Motte in France, 15-18 September 2019. Attended by 160 international
participants, it provided the opportunity to apprise the state of the art, showcase CRESCENDO and CREATE results and interact with other FCHJU/H2020 funded projects, including PEGASUS, which was invited toshare a special session;

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- D7.5 - Survey of dissemination activities and final plan for dissemination and exploitation of project results
The CRESCENDO consortium undertook numerous dissemination and communication activities throughout the duration of the project despite the pandemic that has mainly impacted the conference attendances and the networking activities in the second period of the project. CRESCENDO consortium was very successful in disseminating the project results, especially with the joint organisation of an international workshop with NMBP CREATE, the publication of 14 articles in peer-reviewed journals and 24 presentations at international conferences and workshops. Various target groups included industry, academia, government bodies and the public were reached. After the end of the project, the consortium will continue to carry out further activities to disseminate and exploit the results. The protection of intellectual rights of results issued from CRESCENDO project will still follow the agreed dissemination protocol, to ensure confidentiality and the legitimate interests of the partners, according to the Grant Agreement article II.30 and the internal dissemination protocol (D7.2).
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