Journal Article PUBDB-2025-01663

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Revealing catalyst restructuring and composition during nitrate electroreduction through correlated operando microscopy and spectroscopy

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2025
Nature Publishing Group Basingstoke

Nature materials 24(5), 762 - 769 () [10.1038/s41563-024-02084-8]
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Abstract: Electrocatalysts alter their structure and composition during reaction, which can in turn create new active/selective phases. Identifying these changes is crucial for determining how morphology controls catalytic properties but the mechanisms by which operating conditions shape the catalyst’s working state are not yet fully understood. In this study, we show using correlated operando microscopy and spectroscopy that as well-defined Cu$_2$O cubes evolve under electrochemical nitrate reduction reaction conditions, distinct catalyst motifs are formed depending on the applied potential and the chemical environment. By further matching the timescales of morphological changes observed via electrochemical liquid cell transmission electron microscopy with time-resolved chemical state information obtained from operando transmission soft X-ray microscopy, hard X-ray absorption spectroscopy and Raman spectroscopy, we reveal that Cu2O can be kinetically stabilized alongside metallic copper for extended durations under moderately reductive conditions due to surface hydroxide formation. Finally, we rationalize how the interaction between the electrolyte and the catalyst influences the ammonia selectivity.

Classification:

Contributing Institute(s):
  1. FS DOOR-User (FS DOOR-User)
Research Program(s):
  1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
  2. DFG project G:(GEPRIS)406944504 - Selektivitätskontrolle unter Bedingungen dynamischer CO2 Elektroreduktion (406944504) (406944504)
  3. DFG project G:(GEPRIS)390540038 - EXC 2008: Unifying Systems in Catalysis "UniSysCat" (390540038) (390540038)
Experiment(s):
  1. PETRA Beamline P64 (PETRA III)

Appears in the scientific report 2025
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 Record created 2025-05-15, last modified 2025-07-23


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