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UID:6ae6b7aa73ffa
DTSTART:20261102T090000Z
SEQUENCE:0
TRANSP:OPAQUE
LOCATION:Auditorium
SUMMARY:ICFO | APARNA M. DAS  
CLASS:PUBLIC
DESCRIPTION:Rising atmospheric CO2 levels\, driven primarily by anthropogen
 ic emissions\, are a central contributor to global climate change and envi
 ronmental instability. Electrocatalytic reactions provide a promising path
 way for CO2 emission reduction through electricity-driven conversion of CO
 2 and/or water into value-added chemicals and fuels. In this context\, cat
 alysts are widely recognized as the key determinants of performance. This 
 thesis takes the discussion a step further by examining how\, in specific 
 reactions\, not only the catalyst itself but also the surrounding environm
 ent becomes crucial in defining performance matrices. More specifically\, 
 it investigates dynamic catalyst-electrolyte interfaces in water electroly
 sis and direct bicarbonate reduction\, with a particular emphasis on inter
 facial dynamics and their correlation with activity.\nThe thesis first out
 lines the fundamental aspects of water electrolysis and bicarbonate reduct
 ion\, and then presents new concepts and findings on the role of dynamic c
 atalyst-electrolyte interfaces in these systems. To do so\, several in sit
 u and operando techniques are employed\, including Raman spectroscopy\, X-
 ray absorption spectroscopy\, electrochemical impedance spectroscopy\, and
  quantitative bubble analysis\, complemented by other electrochemical meth
 ods to establish correlations with performance.\nIn the case of water elec
 trolysis\, the thesis focus on the oxygen evolution reaction\, which repre
 sents the largest energetic penalty in the system. Correlations spanning a
 tomic to microscale features are identified\, collectively shaping the per
 formance landscape of the reaction. Using complementary in situ probes\, t
 hese correlations are shown to go beyond simple cause-and-effect relations
 hips\, highlighting the importance of uncovering the underlying mechanisms
  rather than relying solely on performance metrics.\nIn direct bicarbonate
  reduction\, performance is strongly influenced by the availability of CO2
  at the interface\, which is in turn linked to the local pH. Through opera
 ndo Raman spectroscopy\, a descriptor for the interfacial buffering state 
 is identified\, providing indirect insight into instantaneous CO2 availabi
 lity. This hypothesis is further validated by engineering the catalyst-ele
 ctrolyte interface to actively tune this descriptor\, resulting in a three
 fold improvement in performance. This demonstrates how mechanistic underst
 anding of the catalyst-electrolyte interface can guide informed hypotheses
  that are ultimately deterministic\, reducing the experimental parameter s
 pace and improving optimization efficiency.\nOverall\, the thesis emphasiz
 es the importance of understanding why performance improves\, rather than 
 simply attributing progress to &ldquo\;better catalysts&rdquo\;. A deeper 
 understanding of these systems\, especially at high current densities\, ca
 n lead to more coherent design principles and challenge existing assumptio
 ns about major factors governing the electrochemical performance. The resu
 lts show that the catalyst surface cannot be considered a static entity\, 
 but rather a dynamic system whose structure and reactivity are continuousl
 y modulated by external factors. These insights provide a more detailed me
 chanistic picture of electrochemical interfaces and help identify key desc
 riptors for catalyst design.
DTSTAMP:20261101T035314Z
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