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

Document Type

Article

Publication Date

4-9-2024

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.

Identifier

85189024932 (Scopus)

Publication Title

ACS Nano

External Full Text Location

https://doi.org/10.1021/acsnano.4c02020

e-ISSN

1936086X

ISSN

19360851

PubMed ID

38537206

First Page

10302

Last Page

10311

Issue

14

Volume

18

Grant

2215387

Fund Ref

National Science Foundation

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