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DTSTART:20260907T130000Z
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TRANSP:OPAQUE
LOCATION:ICFO Auditorium
SUMMARY:ICFO | ADRIAN PINILLA
CLASS:PUBLIC
DESCRIPTION:Electrochemical technologies offer a route to decarbonize key i
 ndustries\, such as energy\, chemical and fertilizer manufacturing\, by co
 nverting abundant chemicals like carbon dioxide (CO₂) and nitrate into f
 uels and feedstocks using renewable electricity. Realizing this potential 
 requires electrocatalytic systems that achieve technoeconomic viability\, 
 which is linked to performance metrics such as activity\, selectivity\, an
 d stability. Their deployment is constrained by two coupled challenges: in
 complete mechanistic understanding of dynamic electrochemical interfaces a
 nd slow manual workflows that cannot efficiently explore the high-dimensio
 nal design spaces of catalysts\, electrolytes\, and operating parameters. 
 In electrochemical reactions\, performance across its many dimensions emer
 ges from the evolving interplay of catalyst structure and local reaction e
 nvironment at polarized interfaces. Advancing electrocatalytic performance
  therefore requires tools that can both reveal and enable control over the
  evolving catalyst-electrolyte interface during operation. This thesis add
 resses these challenges by combining operando surface-enhanced Raman spect
 roscopy (SERS)\, automated data-analysis frameworks\, and self-driving lab
 oratory approaches to accelerate electrocatalyst development under technol
 ogically relevant conditions for CO₂ and nitrate electroreduction reacti
 ons.\nOperando SERS probes acidic CO₂ electroreduction on copper-based g
 as diffusion electrodes up to 0.2 A cm⁻&sup2\;\, showing how interfacial
  species like sulfate\, hydroxide\, carbon monoxide (CO)\, and carbon-cont
 aining intermediates evolve with potential and pH. Our findings suggest th
 at strongly adsorbed sulfate blocks active sites and delays CO₂E onset a
 t low overpotentials\, while co-adsorbed hydroxide and carbon on reconstru
 cted copper surfaces stabilize *CO coverages that favor C-C coupling and m
 ulticarbon product formation. These results identify electrolyte anions an
 d local alkalization as key levers for tuning the onset potential\, interm
 ediate stabilization\, and selectivity in acidic CO₂ electroreduction\, 
 opening new strategies for rational system-level design of catalysts and e
 lectrolytes.To handle the complexity of operando experiments\, the thesis 
 introduces SERSFlow\, a modular framework for structured operando SERS dat
 a and reusable analysis pipelines. Implemented as a local-first Python ser
 vice with a web interface\, it combines preprocessing\, feature extraction
 \, and multivariate analysis in deterministic workflows that reproduce exp
 ert trends while reducing analysis time from hours to minutes. Benchmarkin
 g shows that baseline subtraction alone can shift fitted peak areas by 40&
 ndash\;100% for weak or overlapping bands\, and spatiotemporal mapping rev
 eals micron-scale heterogeneity in adsorbate populations and double-layer 
 structure.Finally\, the Autoammonia platform&mdash\;a distributed self-dri
 ving laboratory for nitrate-to-ammonia reduction&mdash\;is developed with 
 two active nodes in different institutions. It integrates in situ catalyst
  electrodeposition\, flow-cell nitrate electroreduction\, and automated am
 monia quantification within a closed-loop workflow managed by orchestratio
 n\, planning\, and safety software. Autonomous campaigns with copper-based
  catalysts show that self-driving experimentation is feasible in realistic
  flow-cell architectures and complex electrolytes using accessible hardwar
 e and open-source software.Collectively\, the thesis shows that mechanisti
 c operando characterization\, reproducible data workflows\, and autonomous
  experimentation are mutually reinforcing components of a coherent strateg
 y for advancing electrocatalysis. The concepts and tools developed here pr
 ovide a foundation for more systematic\, data-rich\, and scalable approach
 es to the design and optimization of electrocatalysts and electrochemical 
 interfaces for sustainable\, electrified chemical production.\nThesis Dire
 ctor: Prof. Dr. Francisco Pelayo
DTSTAMP:20260901T194417Z
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