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^*

^*Corresponding author for this work

Research output: Journal Publication › Article › peer-review

6 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
Volume	15
Issue number	10
DOIs	https://doi.org/10.1021/acscatal.5c02322
Publication status	Published - 16 May 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",

month = may,

day = "16",

doi = "10.1021/acscatal.5c02322",

language = "English",

volume = "15",

pages = "8166--8173",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

number = "10",

}

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 - 2025/5/16

Y1 - 2025/5/16

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

VL - 15

SP - 8166

EP - 8173

JO - ACS Catalysis

JF - ACS Catalysis

IS - 10

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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