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H2NEW: Hydrogen (H2) from Next-generation Electrolyzers of Water H2NEW LTE: Manufacturing, Scale-Up, and Integration Nemanja Danilovic, LBNL; Mike Ulsh, NREL; Alexey Serov, ORNL
Date: June 7-11, 2021 Project ID # P196C DOE Hydrogen Program 2021 Annual Merit Review and Peer Evaluation Meeting
This presentation does not contain any proprietary, confidential, or otherwise restricted information.
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H2NEW Task 3a,b: Manufacturing, Scale-Up, and Integration Overview
• Start date (launch): October 1, 2020• Awarded through September 30, 2025• FY21 DOE funding: $1.75M• Annual budget adjustments anticipated
Timeline and Budget
• Durability• Cost• Performance
Barriers
National Lab Consortium Task Team
Deputy Director: Nemanja Danilovic (LBNL) Task Liaisons: Mike Ulsh (NREL)Alexey Serov (ORNL)Subtask Leads: Adam Weber (LBNL)Scott Mauger (NREL)Erin Creel (ORNL)Mike Tucker (LBNL)
H2NEW: Hydrogen from Next generation Electrolyzers of Water 2
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Project Goals
Goal: H2NEW will address components, materials integration, and manufacturing R&D to enable manufacturable electrolyzers that meet required cost, durability, and performance targets, simultaneously, in order to enable $2/kg hydrogen.
Water
H2 production Low-Temperature target <$2/kg Electrolysis (LTE)
High-Temperature Electrolysis (HTE) Hydrogen
H2NEW has a clear target of establishing and utilizing experimental, analytical, and modeling tools needed to provide the scientific understanding of electrolysis cell performance, cost, and durability tradeoffs of electrolysis systems under predicted future operating modes
H2NEW: Hydrogen from Next generation Electrolyzers of Water 3
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Relevance and Impact
Electrolyzer Stack Goals by 2025 LTE PEM
Capital Cost Electrical Efficiency (LHV)
Lifetime
$100/kW 70% at 3 A/cm2
80,000 hr
• Task 3 specifically focuses on enabling high throughput fabrication techniques and componentlevel structure property relationships that enable improved cost, performance and durability:
• Understanding inks• Catalyst layer optimization and fabrication• Porous transport layer (PTL) Design and Optimization
• However, the MEAs, PTLs and other components developed within Task 3 crosscut with Tasks 2and 3
H2NEW: Hydrogen from Next generation Electrolyzers of Water 4
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Approach: Task 3 Work Breakdown
Task 3a: MEA fabrication, Interface engineering i. Inks
• Determine how ink constituent interactions, rheology and mixing defines catalyst-ionomer interaction in the ink and subsequent electrode structure
ii. Electrodes• How does the electrode morphology, porosity and distribution of ionomer affect the
durability and performance• How does the substrate affect the manufacturability/structure and properties of
electrodesiii. Cell Integration and Interfaces
• Impact of component/subcomponent interfaces on performance and durabilityTask 3b: Components
i. Porous Transport Layers• Develop understanding of structure and function, aid in design of new structures
ii. Recombination Layers• Develop understanding of structure and function, aid in design of new structures
H2NEW: Hydrogen from Next generation Electrolyzers of Water 5
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Approach: Year 1 Milestones
Milestone Name/Description Due Date Type Status
Finalize standard, state-of-the-art MEA material set, fabrication process, and/or source to be utilized in baseline studies including those for durability, performance, and scale-up/integration – All Labs
12/31/2020 QPM Complete
Identify and source commercially available PTL materials and establish one candidate as baseline material based on suitability. Labs – NREL, LBNL, ORNL. 3/30/2021 QPM Complete
Provide comments to HFTO on appropriateness of 5-year stack level LTE targets based on TEA, systems analysis, and experimental studies included in H2NEW activities. Labs – NREL, ANL, LANL, LBNL. 9/30/2021 QPM On Track
Establish a baseline of anode fabrication using scalable processes that matches or exceeds the performance of a spray-coated anode with a loading of 0.5 mg Ir/cm2. For example, demonstrating a maximum cell voltage of 1.9V at 2.0 A/cm2 when using a Nafion 117 membrane and tested in a cell at 80 C. NREL, ORNL, ANL, LBNL.
9/30/2021 QPM On Track
Establish and validate single cell performance testing protocols on SOA MEAs with PGM loading of <0.8 mg/cm2 and membranes <100 µm demonstrating a minimum performance of 2 A/cm2 at 1.8 V and demonstrate ability to perform voltage loss breakdown modeling as verified by agreement within 10% across at least 3 labs.
9/30/2021 Milestone On Track
H2NEW: Hydrogen from Next generation Electrolyzers of Water 6
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H2NEW: Hydrogen from Next generation Electrolyzers of Water 7
H2NEW Goals with Scale Up and Integration
2020
Crosscuts
---------------------2025
• Shift focus from laboratory (model) to scalable processes or structures– Understanding of structure-function relationships – Impacts on performance and
• Ink (PFSA-catalyst) durability• Electrode (Mesostructure and interfaces) • Tasks 2
• In situ/Ex situ/Operando • PTLs (Structure and interfaces)Characterization – New Structures • Modeling
• Engineered PTL Structures • Tasks 1• Novel coatings • Degradation processes• Engineered Electrode Structures • Mitigation Strategies• Recombination Layers – Including defects and non-
idealities
Image Source: Julie Fornaciari
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Understanding and Evaluation
Solutions
H2NEW’s Approach MEA Fabrication Scale Up
• Dilute ink • Viscous ink • Viscous Ink
• Serves as a model • Translate subscale• Homogenous Ir • Heterogenous Ir distribution • Very high throughput
distribution• Low throughput high throughput deposition learnings
2025 100 $/kW Understanding/Legacy Model/Scalable Fabrication Engineered @Scale/H2NEW
technique
Spray Coating Slot Die Coating R2R Coating
Ink Vehicles Ink Mixing Electrode Structure/Function Substrates
Study the impact of Study the impact of ink vehicle composition, mixing on the ink solids content, I/C ratio stability and and solvent types agglomeration
Ink Rheology
Study the relationships between ink composition, rheology and the of ink rheology on
Impact of ink, deposition technique on the catalyst layer structure, ionomer distribution, catalyst distribution, agglomerate size on performance and durability.
Impact of substrate type and deposition method on structure and function of the resulting catalyst layers. Downselect based on technoeconomic and manufacturing considerations.
H2NEW: Hydrogen from Next generation Electrolyzers of Water 8
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Transition from Lab-Scale to Scalable Electrode Production La
b Sc
ale
– U
ltras
onic
Spr
ayLarge Scale – Roll-to-Roll (R2R)
Scale Up
Used to demonstrate new materials and for fundamental studies Conditions • Dilute ink (~0.6 wt% solids)• Ultrasonic mixing• Sequential build up of layers• Heated substrate• Vacuum substrate
Variables Viscosity and solids
Coating Physics Mixing
Mesostructure Substrate
Needed to demonstrate scalability of materials, MEA/cell designs, and industrial relevanceConditions • Concentrated ink (~4.5-15 wt% solids)• Shear mixing• Single layer• Room temp. substrate• Convective drying
H2NEW: Hydrogen from Next generation Electrolyzers of Water 9
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Approach: Inks
• Inks form the basis for thestructures and properties ofresulting electrodes, areas of inkconstituent interactions studyinclude• morphology:• agglomeration,• stability,• ionomer adsorption,• rheology
H2NEW: Hydrogen from Next generation Electrolyzers of Water 10
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Approach: Electrode Processing Methodologies
Ultrasonic spray coating
Medium viscosity ink
• Understand how concentratedink process physics differ fromthat for dilute ink
• Understand how processingconditions, dryingtemperature/environmentdiffer
• How does the resultingelectrode structure change andwhat is impact of performanceand durability
Slot Die Coating
Gravure Coating Mayer Rod Coating
Blade Coating
Highly dilute ink High viscosity ink
H2NEW: Hydrogen from Next generation Electrolyzers of Water Mali et al. Nanoscale Advances 1.2 (2019) www.holoeast.com Howard et al. Advanced Materials 31.25 (2019) 11
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0.1
Accomplishment: Ink Baselining
• Baseline ink formulation has been characterized Ink Rheology • Inks are Newtonian and the ink viscosities are reasonably 0.1
consistent between the labs
Mixing Effects 0.01
Shea
r Visc
osity
[Pa.s
]
Rheology Mixing Ink Composition
Solvent
Ionomer
Catalyst
ORNL LBNL NREL
1 10 100 1000Sonication - 30 min Sonication - 1 h Shear Mixing - 15 min Shear Mixing - 20 min
Shea
r Visc
osity
[Pa.s
]
Shear Rate [s-1]
• Ink rheology, thus agglomerated structure, is sensitive tomixing method and mixing duration
• Mixing parameter needs to be further optimized to0.01 maximize catalyst dispersion1 10 100 1000
Shear Rate [1/s] H2NEW: Hydrogen from Next generation Electrolyzers of Water 12
H2NEW’s Approach to Integration and Components Porous Transport Layer Interfacial Layers Scalable and Engineered
• Evaluate the impact Structures • Evaluate of additive/ • Design scalable PTL
structures withavailable PTLs on the properties tailored porosity,• Mechanical and and function of PTLs tailored interface andtransport properties • Evaluate the PTL
2025100 $/kW Understanding/Commercial Model/Interfaces Engineered
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Understanding and Evaluation SolutionsStructures
commercially microporous layers
Bekaert Mott wetting properties• Performance andCommercial Commercial interface topologyT. Schuler et al, Adv. Energy Mat., 10Ti fiber Ti particle durability on function of PTL (2020), 1903216
Mechanical Properties Coatings Interface Two Phase Transport Fabrication
Leonard et al. Solar Fuels C. Liu et al, Adv Energy Mat., (10.1039/c9se00364a) P. Satjaritanun et al., iScience, 23,11 (2021), 2002926 (2020) 101783.
Study PTL mechanical Study impact and type Study the coherence of and Study the transport of Use 3D printing and properties. Study the of corrosion resistant transport through the
PTL/membrane coatings. Investigate PTL/membrane interface water and oxygen tape casting to make interfacial mechanical non-PGM alternatives and impact on performance through the PTL. PTLs with tailored properties. defects. and durability. characteristics.
H2NEW: Hydrogen from Next generation Electrolyzers of Water 13
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Accomplishment: Titanium PTL/MPL Additive Manufacturing
E-Beam Fusing of Metal Particles• Layer-by-layer electron beam melting process performed at ORNL’s Manufacturing Demonstration Facility (MDF) – Metal particles melted by e-beam to form a 3D porous structure– Adjusting the e-beam focus and movement pattern allows the amount
of void space (porosity) to be tuned.
Tomography of fabricated PTL
• 55 mm x 55 mm x 1 mm proof of concept structuresmanufactured from Ti64 with 25% porosity in the highlightedcenter region of interest measured by micro CT– Ti64 behaves similarly to pure Ti in manufacturing, but the Al and V
impurities make it unsuitable for use in a PTL.
• Next steps: determine upper porosity limit and attempt tomake porosity-graded PTLs using grade 2 (commercially pure)Ti
H2NEW: Hydrogen from Next generation Electrolyzers of Water 14
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Accomplishment: Ti PTL Structure Function Characterization • 20um Fiber diameter Bekeart PTLs, varying thickness
at 56% porosity and varying porosity atfixed thickness
• N117, Fixed catalyst loading of 0.06 mgIr/cm2
• Too porous is bad because the interface suffers• ~50% dense is optimal
• Too thick and too thin is bad as well(maybe mechanical),
• 150 um optimal
• To inform future PTLdesign
Fixed Thickness Fixed Porosity
*Iryna Zenyuk at UCI
H2NEW: Hydrogen from Next generation Electrolyzers of Water 15
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Responses to Previous Year Reviewers’ Comments
• Not Applicable, first year of project
H2NEW: Hydrogen from Next generation Electrolyzers of Water 16
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Collaboration and Coordination
NREL Team Members: Shaun Alia, Carlos Baez-Cotto, Guido Bender, Sunil Khandavalli, Allen Kang, Scott Mauger, Bryan Pivovar, Jason Pfeilsticker, Elliot Padgett, Tobias Schuler, Sarah Shulda, Mike Ulsh, Jason Zack LBNL Team Members: Sarah Berlinger, Nemanja Danilovic, Julie Fornaciari, Grace Lau, Jason Keonhag Lee, Michael Tucker, Adam Weber. ANL Team Members: C. Firat Cetinbas, Nancy Kariuki, Debbie Myers, Jaehyung Park, Xiaohua Wang. LANL Team Members: Siddharth Komini Babu, Rangachary Mukundan, Xiaoxiao Qiao ORNL Team Members:, Erin Creel, Dave Cullen, Michael Kirka, Christopher Ledford, Alexey Serov.
H2NEW: Hydrogen from Next generation Electrolyzers of Water 17
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Proposed Future Work
Task 3a: MEA fabrication, Interface engineering i. Inks
• Determine how ink constituent interactions, rheology and mixing defines catalyst-ionomer interaction in the ink and subsequent electrode structure
ii. Electrodes• How does the electrode morphology, porosity and distribution of ionomer affect the
durability and performance• How does the substrate affect the manufacturability/structure and properties of
electrodesiii. Cell Integration and Interfaces
• Impact of component/subcomponent interfaces on performance and durabilityTask 3b: Components
i. Porous Transport Layers• Develop understanding of structure and function, aid in design of new structures
ii. Recombination Layers• Develop understanding of structure and function, aid in design of new structures
Any proposed future work is subject to change based on funding levels H2NEW: Hydrogen from Next generation Electrolyzers of Water 18
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Summary―Task 3
• The task 3 effort focuses on cell integration and scale-up aspects of the overall H2NEW goals• Task 3 work areas include inks, electrodes, integration and interfaces, PTLs, and
recombination layers– Understand the transition from lab-scale to scalable processing of MEA materials– Understand and optimize structure-performance relationships– Develop novel material structures that will enhance durability and/or reduce cost– These efforts will be highly integrated with the Task 1 durability and Task 2 performance efforts
• Early accomplishments include– Novel metal additive manufacturing studies to explore PTL structures and properties– Ink baselining between labs to establish common processing and measurement methods– Evaluating PTL structure property effects to inform PTL design
H2NEW: Hydrogen from Next generation Electrolyzers of Water 19
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Technical Backup and Additional Information Slides
H2NEW: Hydrogen from Next generation Electrolyzers of Water 20
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Technology Transfer Activities
• No current patent or licensing sought• H2NEW website and marketing material being developed• Interactions with the following OEMs:
– Mott– Bekaert– JM– Heraeus– Chemours– Pajarito Powder– 3M
• IP generation mechanism through CRADAs with industry to be sought during the course ofthe project
H2NEW: Hydrogen from Next generation Electrolyzers of Water 21
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Progress Towards DOE Targets or Milestones
Electrolyzer Stack Goals by 2025
LTE PEM MYRD&D 2020* Capital Cost
Electrical Efficiency (LHV)
Lifetime
$100/kW 70% at 3 A/cm2
80,000 hr
$300/kW 77% (n/a current
density) n/a
*Table 3.1.4 in MYRD&D
H2NEW: Hydrogen from Next generation Electrolyzers of Water 22
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Publications and Presentations
• Capuano C.B., Ayers K., Manco J., Wiles L., Errico S., Zenyuk I.V., Weber A.Z., Kusoglu A.,Danilovic N., Ulsh M., Mauger S.A., Pfeilsticker J., Alia S.M. “High Efficiency PEM WaterElectrolysis Enabled By Advanced Catalysts, Membranes and Processes.” Invited oralpresentation at the Fall ESC Meeting (virtual); October 2020.
• Park J., Kang Z., Bender G., Ulsh M., Mauger S.A. “Direct roll-to-roll coating of catalyst-coatedmembranes for low-cost PEM water electrolyzers.” Oral presentation at the Fall ESC Meeting(virtual); October 2020.
• M.R. Gerhardt, L.M. Pant, J.C.M. Bui, A. R. Crothers, V.M. Ehlinger, J.C. Fornaciari, J. Liu andA.Z. Weber, “Methods—Practices and Pitfalls in Voltage Breakdown Analysis ofElectrochemical Energy-Conversion Systems”, JES, DOI:10.1149/1945-7111/abf061.
H2NEW: Hydrogen from Next generation Electrolyzers of Water 23
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Special Recognitions and Awards
• Bryan Pivovar was awarded the 2021 Energy Technology Division Research Award ofthe Electrochemical Society and the 2021 US Department of Energy Secretary’sHonor Award.
H2NEW: Hydrogen from Next generation Electrolyzers of Water 24