Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

Xin Li; Guangtong Hai; Daniel H. C. Wan; Yiwen Liao; Zhangyi Yao; Fenglin Zhao; Lingzhi Huang; Jinsong Zhou; Gang Li; Gao-Feng Chen; Feng Ryan Wang; Michael K. H. Leung; Haihui Wang

doi:10.1021/jacs.4c17380

Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

Xin Li (Co-first Author)
, Guangtong Hai (Co-first Author)
, Daniel H. C. Wan
, Yiwen Liao
, Zhangyi Yao
, Fenglin Zhao
, Lingzhi Huang
, Jinsong Zhou
, Gang Li
, Gao-Feng Chen^*
, Feng Ryan Wang^*
, Michael K. H. Leung^*
, Haihui Wang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

9 Citations (Scopus)

Abstract

Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO₂ emissions. Sustainable NO₃^- production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst’s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52% under 8 atm air, with an impressive increase in FE (41.56%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O₂-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields. © 2025 American Chemical Society.

Original language	English
Pages (from-to)	8587-8596
Number of pages	10
Journal	Journal of the American Chemical Society
Volume	147
Issue number	10
Online published	27 Feb 2025
DOIs	https://doi.org/10.1021/jacs.4c17380
Publication status	Published - 12 Mar 2025

Funding

We gratefully acknowledge the funding from the National Key R&D Program of China (Grant No. 2022YFB4002602), the Natural Science Foundation of China (Grant No. 22138005), Tsinghua University Initiative Scientific Research Program (2023Z02JMP001), the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. CityU 11206520), Ningbo Municipal Government Innovation 2025 Scheme (No. 2018B10023), the Shenzhen Knowledge Innovation Program (Basic Research, JCYJ20190808181205752), and the New Cornerstone Science Foundation through the XPLORER PRIZE. We acknowledge the BL01B1 beamline at SPring-8 (Japan) for the XAS experiments.

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This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

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RGC-funded

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title = "Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion",

abstract = "Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO2 emissions. Sustainable NO3- production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst{\textquoteright}s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52\% under 8 atm air, with an impressive increase in FE (41.56\%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O2-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields. {\textcopyright} 2025 American Chemical Society.",

author = "Xin Li and Guangtong Hai and Wan, \{Daniel H. C.\} and Yiwen Liao and Zhangyi Yao and Fenglin Zhao and Lingzhi Huang and Jinsong Zhou and Gang Li and Gao-Feng Chen and Wang, \{Feng Ryan\} and Leung, \{Michael K. H.\} and Haihui Wang",

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doi = "10.1021/jacs.4c17380",

language = "English",

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journal = "Journal of the American Chemical Society",

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}

Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion. / Li, Xin (Co-first Author); Hai, Guangtong (Co-first Author); Wan, Daniel H. C. et al.
In: Journal of the American Chemical Society, Vol. 147, No. 10, 12.03.2025, p. 8587-8596.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

AU - Li, Xin

AU - Hai, Guangtong

AU - Wan, Daniel H. C.

AU - Liao, Yiwen

AU - Yao, Zhangyi

AU - Zhao, Fenglin

AU - Huang, Lingzhi

AU - Zhou, Jinsong

AU - Li, Gang

AU - Chen, Gao-Feng

AU - Wang, Feng Ryan

AU - Leung, Michael K. H.

AU - Wang, Haihui

PY - 2025/3/12

Y1 - 2025/3/12

N2 - Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO2 emissions. Sustainable NO3- production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst’s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52% under 8 atm air, with an impressive increase in FE (41.56%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O2-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields. © 2025 American Chemical Society.

AB - Current nitrate production involves a two-step thermochemical process that is energy-intensive and generates substantial CO2 emissions. Sustainable NO3- production via the nitrogen electrooxidation reaction powered by renewable electricity is highly desirable, but the Faradaic efficiency (FE) at high production rates is unsatisfactory due to competition from the oxygen evolution reaction (OER). In this study, we propose reengineering the catalyst’s microstructure-to-macroenvironment interface by particularly utilizing the previously considered unfavored oxygen from the OER. We demonstrate that the re-engineered interface facilitates a record-breaking FE of 35.52% under 8 atm air, with an impressive increase in FE (41.56%) observed during a continuous electrochemical process lasting for 60 h due to the in situ formation of the O2-rich macro-interface environment. The revelation is anticipated to furnish groundbreaking perspectives for the reaction systems design in electrochemical nitrate production and other electrocatalytic fields. © 2025 American Chemical Society.

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DO - 10.1021/jacs.4c17380

M3 - RGC 21 - Publication in refereed journal

C2 - 40015978

SN - 0002-7863

VL - 147

SP - 8587

EP - 8596

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 10

ER -

Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

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GRF: Rational Design of MoS2 Electrocatalyst for pH-universal Hydrogen Evolution: Mechanisms, Kinetics and Optimization

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Favoring the Originally Unfavored Oxygen for Enhancing Nitrogen-to-Nitrate Electroconversion

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Funding

UN SDGs

RGC Funding Information

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GRF: Rational Design of MoS2 Electrocatalyst for pH-universal Hydrogen Evolution: Mechanisms, Kinetics and Optimization

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