Coupling Curvature and Hydrophobicity: A Counterintuitive Strategy for Efficient Electroreduction of Nitrate into Ammonia

Jianan Gao, Qingquan Ma, Yihan Zhang, Shan Xue, Joshua Young, Mengqiang Zhao, Zhiyong Jason Ren, Jae Hong Kim, Wen Zhang

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

The electrochemical upcycling of nitrate (NO3-) to ammonia (NH3) holds promise for synergizing both wastewater treatment and NH3 synthesis. Efficient stripping of gaseous products (NH3, H2, and N2) from electrocatalysts is crucial for continuous and stable electrochemical reactions. This study evaluated a layered electrocatalyst structure using copper (Cu) dendrites to enable a high curvature and hydrophobicity and achieve a stratified liquid contact at the gas-liquid interface of the electrocatalyst layer. As such, gaseous product desorption or displacement from electrocatalysts was enhanced due to the separation of a wetted reaction zone and a nonwetted zone for gas transfer. Consequently, this electrocatalyst structure yielded a 2.9-fold boost in per-active-site activity compared with that with a low curvature and high hydrophilic counterpart. Moreover, a NH3 Faradaic efficiency of 90.9 ± 2.3% was achieved with nearly 100% NO3- conversion. This high-curvature hydrophobic Cu dendrite was further integrated with a gas-extraction membrane, which demonstrated a comparable NH3 yield from the real reverse osmosis retentate brine.

Original languageEnglish (US)
Pages (from-to)10302-10311
Number of pages10
JournalACS Nano
Volume18
Issue number14
DOIs
StatePublished - Apr 9 2024

All Science Journal Classification (ASJC) codes

  • General Materials Science
  • General Engineering
  • General Physics and Astronomy

Keywords

  • ammonia production
  • electrochemical nitrate reduction
  • hierarchically structured dendrites
  • mass transfer
  • microenvironment
  • nanoarray

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