Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine

Dandan Guo; Fengyu Liu; Tianqi Liu; Zhaoqi Ji; Xiaolei Fan; Bin Sun; Peili Zhang; Fei Li; Fusheng Li

doi:10.1021/acscatal.5c02322

Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine

Dandan Guo
, Fengyu Liu
, Tianqi Liu
, Zhaoqi Ji
, Xiaolei Fan
, Bin Sun
, Peili Zhang
, Fei Li
, Fusheng Li

Research output: Journal Publication › Article › peer-review

3 Citations (Scopus)

Abstract

Efficient ammonia oxidation electrocatalysis is crucial for converting the chemical energy in ammonia molecules into electricity and for valorizing ammonia into value-added chemicals. This work introduces the single-site catalyst Ru-pdcPy₂ with a pentadentate carboxamide ligand for ammonia oxidation, which is capable of oxidizing ammonia directly to hydrazine, possibly via a single-site N-N bond formation mechanism. The combination of nuclear magnetic resonance spectroscopy, mass spectrometry, and electrochemical technique was utilized to investigate the catalytic behavior of the catalyst. Under optimal conditions, the Ru-pdcPy₂ achieves a TOF of 32.6 h^-1 for N₂ generation and a TOF of 8.4 h^-1 for N₂H₄ synthesis during bulk electrolysis.

Original language	English
Pages (from-to)	8166-8173
Number of pages	8
Journal	ACS Catalysis
DOIs	https://doi.org/10.1021/acscatal.5c02322
Publication status	Accepted/In press - 2025
Externally published	Yes

Free Keywords

ammonia oxidation
carboxamide ligand
electrocatalysis
hydrazine
molecular catalyst

ASJC Scopus subject areas

Catalysis
General Chemistry

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10.1021/acscatal.5c02322

Cite this

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title = "Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine",

abstract = "Efficient ammonia oxidation electrocatalysis is crucial for converting the chemical energy in ammonia molecules into electricity and for valorizing ammonia into value-added chemicals. This work introduces the single-site catalyst Ru-pdcPy2 with a pentadentate carboxamide ligand for ammonia oxidation, which is capable of oxidizing ammonia directly to hydrazine, possibly via a single-site N-N bond formation mechanism. The combination of nuclear magnetic resonance spectroscopy, mass spectrometry, and electrochemical technique was utilized to investigate the catalytic behavior of the catalyst. Under optimal conditions, the Ru-pdcPy2 achieves a TOF of 32.6 h-1 for N2 generation and a TOF of 8.4 h-1 for N2H4 synthesis during bulk electrolysis.",

keywords = "ammonia oxidation, carboxamide ligand, electrocatalysis, hydrazine, molecular catalyst",

author = "Dandan Guo and Fengyu Liu and Tianqi Liu and Zhaoqi Ji and Xiaolei Fan and Bin Sun and Peili Zhang and Fei Li and Fusheng Li",

note = "Publisher Copyright: {\textcopyright} 2025 American Chemical Society.",

year = "2025",

doi = "10.1021/acscatal.5c02322",

language = "English",

pages = "8166--8173",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

}

TY - JOUR

T1 - Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine

AU - Guo, Dandan

AU - Liu, Fengyu

AU - Liu, Tianqi

AU - Ji, Zhaoqi

AU - Fan, Xiaolei

AU - Sun, Bin

AU - Zhang, Peili

AU - Li, Fei

AU - Li, Fusheng

PY - 2025

Y1 - 2025

N2 - Efficient ammonia oxidation electrocatalysis is crucial for converting the chemical energy in ammonia molecules into electricity and for valorizing ammonia into value-added chemicals. This work introduces the single-site catalyst Ru-pdcPy2 with a pentadentate carboxamide ligand for ammonia oxidation, which is capable of oxidizing ammonia directly to hydrazine, possibly via a single-site N-N bond formation mechanism. The combination of nuclear magnetic resonance spectroscopy, mass spectrometry, and electrochemical technique was utilized to investigate the catalytic behavior of the catalyst. Under optimal conditions, the Ru-pdcPy2 achieves a TOF of 32.6 h-1 for N2 generation and a TOF of 8.4 h-1 for N2H4 synthesis during bulk electrolysis.

AB - Efficient ammonia oxidation electrocatalysis is crucial for converting the chemical energy in ammonia molecules into electricity and for valorizing ammonia into value-added chemicals. This work introduces the single-site catalyst Ru-pdcPy2 with a pentadentate carboxamide ligand for ammonia oxidation, which is capable of oxidizing ammonia directly to hydrazine, possibly via a single-site N-N bond formation mechanism. The combination of nuclear magnetic resonance spectroscopy, mass spectrometry, and electrochemical technique was utilized to investigate the catalytic behavior of the catalyst. Under optimal conditions, the Ru-pdcPy2 achieves a TOF of 32.6 h-1 for N2 generation and a TOF of 8.4 h-1 for N2H4 synthesis during bulk electrolysis.

KW - ammonia oxidation

KW - carboxamide ligand

KW - electrocatalysis

KW - hydrazine

KW - molecular catalyst

UR - https://www.scopus.com/pages/publications/105004056262

U2 - 10.1021/acscatal.5c02322

DO - 10.1021/acscatal.5c02322

M3 - Article

AN - SCOPUS:105004056262

SN - 2155-5435

SP - 8166

EP - 8173

JO - ACS Catalysis

JF - ACS Catalysis

ER -

Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine

Abstract

Free Keywords

ASJC Scopus subject areas

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