Interface Engineering of SRu-mC3N4 Heterostructures for Enhanced Electrochemical Hydrazine Oxidation Reactions

Ajay Munde; Priti Sharma; Somnath Dhawale; Ravishankar G. Kadam; Subodh Kumar; Hanumant B. Kale; Jan Filip; Radek Zboril; Bhaskar R. Sathe; Manoj B. Gawande

doi:10.3390/catal12121560

Interface Engineering of SRu-mC₃N₄ Heterostructures for Enhanced Electrochemical Hydrazine Oxidation Reactions

Ajay Munde
, Priti Sharma
, Somnath Dhawale
, Ravishankar G. Kadam
, Subodh Kumar
, Hanumant B. Kale
, Jan Filip
, Radek Zboril
, Bhaskar R. Sathe
, Manoj B. Gawande

Dr. Babasaheb Ambedkar Marathwada University
Palacký University Olomouc
Institute of Chemical Technology
VŠB – Technical University of Ostrava

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Hydrazine oxidation in single-atom catalysts (SACs) could exploit the efficiency of metal atom utilization, which is a substitution for noble metal-based electrolysers that results in reduced overall cost. A well-established ruthenium single atom over mesoporous carbon nitride (SRu-mC₃N₄) catalyst is explored for the electro-oxidation of hydrazine as one of the model reactions for direct fuel cell reactions. The electrochemical activity observed with linear sweep voltammetry (LSV) confirmed that SRu-mC₃N₄ shows an ultra-low onset potential of 0.88 V vs. RHE, and with a current density of 10 mA/cm² the observed potential was 1.19 V vs. RHE, compared with mesoporous carbon nitride (mC₃N₄) (1.77 V vs. RHE). Electrochemical impedance spectroscopy (EIS) and chronoamperometry (i-t) studies on SRu-mC₃N₄ show a smaller charge-transfer resistance (R_Ct) of 2950 Ω and long-term potential, as well as current stability of 50 h and 20 mA/cm², respectively. Herein, an efficient and enhanced activity toward HzOR was demonstrated on SRu-mC₃N₄ from its synergistic platform over highly porous C₃N₄, possessing large and independent active sites, and improving the subsequent large-scale reaction.

Original language	English
Article number	1560
Journal	Catalysts
Volume	12
Issue number	12
DOIs	https://doi.org/10.3390/catal12121560
State	Published - Dec 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2022 by the authors.

Funding

The authors gratefully acknowledge the support by the Operational Program Research, Development and Education—European Regional Development Fund (project no. CZ.02.1.01/0.0/0.0/16_019/0000754) and by the ERDF project “Development of pre-applied research in nanotechnology and biotechnology” (project no. CZ.02.1.01/0.0/0.0/17_048/0007323) of the Ministry of Education, Youth and Sports of the Czech Republic. R.Z. thanks the Czech Science Foundation for financial support (project no. 19-27454X). A.M. is thankful to MJRF (MS) for fellowship-2021-22/1042 (414). H.B.K. would like to gratefully acknowledge the Institute of Chemical Technology, Mumbai for providing a fellowship for doctoral study.

Funders	Funder number
Operational Program Research, Development and Education
Instituto de Tecnología Química
Ministerstvo Školství, Mládeže a Tělovýchovy
Grantová Agentura České Republiky	19-27454X
European Regional Development Fund	CZ.02.1.01/0.0/0.0/17_048/0007323

Keywords

hydrazine oxidation reactions
mesoporous carbon nitride
nanoelectrodes
single-atom catalysts

Access to Document

10.3390/catal12121560

Cite this

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title = "Interface Engineering of SRu-mC3N4 Heterostructures for Enhanced Electrochemical Hydrazine Oxidation Reactions",

abstract = "Hydrazine oxidation in single-atom catalysts (SACs) could exploit the efficiency of metal atom utilization, which is a substitution for noble metal-based electrolysers that results in reduced overall cost. A well-established ruthenium single atom over mesoporous carbon nitride (SRu-mC3N4) catalyst is explored for the electro-oxidation of hydrazine as one of the model reactions for direct fuel cell reactions. The electrochemical activity observed with linear sweep voltammetry (LSV) confirmed that SRu-mC3N4 shows an ultra-low onset potential of 0.88 V vs. RHE, and with a current density of 10 mA/cm2 the observed potential was 1.19 V vs. RHE, compared with mesoporous carbon nitride (mC3N4) (1.77 V vs. RHE). Electrochemical impedance spectroscopy (EIS) and chronoamperometry (i-t) studies on SRu-mC3N4 show a smaller charge-transfer resistance (RCt) of 2950 Ω and long-term potential, as well as current stability of 50 h and 20 mA/cm2, respectively. Herein, an efficient and enhanced activity toward HzOR was demonstrated on SRu-mC3N4 from its synergistic platform over highly porous C3N4, possessing large and independent active sites, and improving the subsequent large-scale reaction.",

keywords = "hydrazine oxidation reactions, mesoporous carbon nitride, nanoelectrodes, single-atom catalysts",

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T1 - Interface Engineering of SRu-mC3N4 Heterostructures for Enhanced Electrochemical Hydrazine Oxidation Reactions

AU - Munde, Ajay

AU - Sharma, Priti

AU - Dhawale, Somnath

AU - Kadam, Ravishankar G.

AU - Kumar, Subodh

AU - Kale, Hanumant B.

AU - Filip, Jan

AU - Zboril, Radek

AU - Sathe, Bhaskar R.

AU - Gawande, Manoj B.

PY - 2022/12

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N2 - Hydrazine oxidation in single-atom catalysts (SACs) could exploit the efficiency of metal atom utilization, which is a substitution for noble metal-based electrolysers that results in reduced overall cost. A well-established ruthenium single atom over mesoporous carbon nitride (SRu-mC3N4) catalyst is explored for the electro-oxidation of hydrazine as one of the model reactions for direct fuel cell reactions. The electrochemical activity observed with linear sweep voltammetry (LSV) confirmed that SRu-mC3N4 shows an ultra-low onset potential of 0.88 V vs. RHE, and with a current density of 10 mA/cm2 the observed potential was 1.19 V vs. RHE, compared with mesoporous carbon nitride (mC3N4) (1.77 V vs. RHE). Electrochemical impedance spectroscopy (EIS) and chronoamperometry (i-t) studies on SRu-mC3N4 show a smaller charge-transfer resistance (RCt) of 2950 Ω and long-term potential, as well as current stability of 50 h and 20 mA/cm2, respectively. Herein, an efficient and enhanced activity toward HzOR was demonstrated on SRu-mC3N4 from its synergistic platform over highly porous C3N4, possessing large and independent active sites, and improving the subsequent large-scale reaction.

AB - Hydrazine oxidation in single-atom catalysts (SACs) could exploit the efficiency of metal atom utilization, which is a substitution for noble metal-based electrolysers that results in reduced overall cost. A well-established ruthenium single atom over mesoporous carbon nitride (SRu-mC3N4) catalyst is explored for the electro-oxidation of hydrazine as one of the model reactions for direct fuel cell reactions. The electrochemical activity observed with linear sweep voltammetry (LSV) confirmed that SRu-mC3N4 shows an ultra-low onset potential of 0.88 V vs. RHE, and with a current density of 10 mA/cm2 the observed potential was 1.19 V vs. RHE, compared with mesoporous carbon nitride (mC3N4) (1.77 V vs. RHE). Electrochemical impedance spectroscopy (EIS) and chronoamperometry (i-t) studies on SRu-mC3N4 show a smaller charge-transfer resistance (RCt) of 2950 Ω and long-term potential, as well as current stability of 50 h and 20 mA/cm2, respectively. Herein, an efficient and enhanced activity toward HzOR was demonstrated on SRu-mC3N4 from its synergistic platform over highly porous C3N4, possessing large and independent active sites, and improving the subsequent large-scale reaction.

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KW - mesoporous carbon nitride

KW - nanoelectrodes

KW - single-atom catalysts

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