Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory

Genping Yi; Bo Wang; Sen Lu; Liying Zhang; Wenzong Liu; Zheyu Chen; Liming Yang; Xubiao Luo; Ai Jie Wang

doi:10.1016/j.cej.2024.149226

Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory

Genping Yi, Bo Wang, Sen Lu, Liying Zhang, Wenzong Liu^*, Zheyu Chen, Liming Yang, Xubiao Luo, Ai Jie Wang

^*Corresponding author af dette arbejde

Publikation: Bidrag til tidsskrift/Konferencebidrag i tidsskrift /Bidrag til avis › Tidsskriftartikel › Forskning › peer review

7 Citationer (Scopus)

Abstract

Electro-generated atomic hydrogen (H*) plays a crucial role in the electrochemical reduction process, serving as the key species that mediates the electrocatalytic hydrogenation reduction of stubborn contaminants in wastewater treatment. However, precisely identifying and quantifying transient atomic H* presents a significant challenge due to its limited lifespan and its existence solely within the boundary layer at the electrode/solution interface. Herein, we developed the electrodeposition of palladium nanoparticles onto carbon cloth and assessed its effectiveness as a cathode for generating and stabilizing atomic H*. The environmental application of atomic H* was validated through the dechlorination of 2, 4-dichlorophenol wastewater and the reduction of antimonite wastewater. Additionally, the identification of atomic H* was verified by electrochemical measurements, high-resolution mass spectra, and density functional theory. Moreover, introducing an excess of a spin trapping agent (5,5-dimethyl-1-pyrroline-N-oxide) and fast in-situ spin trapping facilitated creating favorable conditions for efficient trapping of atomic H* and subsequent electron spin resonance (ESR) spectroscopy quantification analysis. Subsequently, the quantification of atomic H* was achieved by double integration of the ESR signal of spin adduct and comparison with the external standard agent (4-hydroxy-2,2,6,6-tetramethyl-1-piperidine 1-oxyl). This study introduces a novel method for in-situ spin trapping and quantification of atomic H*, facilitating the advancement of electrochemical reduction technology and its application in wastewater treatment.

Originalsprog	Engelsk
Artikelnummer	149226
Tidsskrift	Chemical Engineering Journal
Vol/bind	483
ISSN	1385-8947
DOI	https://doi.org/10.1016/j.cej.2024.149226
Status	Udgivet - 1 mar. 2024

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title = "Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory",

abstract = "Electro-generated atomic hydrogen (H*) plays a crucial role in the electrochemical reduction process, serving as the key species that mediates the electrocatalytic hydrogenation reduction of stubborn contaminants in wastewater treatment. However, precisely identifying and quantifying transient atomic H* presents a significant challenge due to its limited lifespan and its existence solely within the boundary layer at the electrode/solution interface. Herein, we developed the electrodeposition of palladium nanoparticles onto carbon cloth and assessed its effectiveness as a cathode for generating and stabilizing atomic H*. The environmental application of atomic H* was validated through the dechlorination of 2, 4-dichlorophenol wastewater and the reduction of antimonite wastewater. Additionally, the identification of atomic H* was verified by electrochemical measurements, high-resolution mass spectra, and density functional theory. Moreover, introducing an excess of a spin trapping agent (5,5-dimethyl-1-pyrroline-N-oxide) and fast in-situ spin trapping facilitated creating favorable conditions for efficient trapping of atomic H* and subsequent electron spin resonance (ESR) spectroscopy quantification analysis. Subsequently, the quantification of atomic H* was achieved by double integration of the ESR signal of spin adduct and comparison with the external standard agent (4-hydroxy-2,2,6,6-tetramethyl-1-piperidine 1-oxyl). This study introduces a novel method for in-situ spin trapping and quantification of atomic H*, facilitating the advancement of electrochemical reduction technology and its application in wastewater treatment.",

keywords = "Atomic hydrogen, Electrochemical reduction, Electron spin resonance, Environmental applications, Identification and quantification",

author = "Genping Yi and Bo Wang and Sen Lu and Liying Zhang and Wenzong Liu and Zheyu Chen and Liming Yang and Xubiao Luo and Wang, {Ai Jie}",

note = "Publisher Copyright: {\textcopyright} 2024 Elsevier B.V.",

year = "2024",

month = mar,

day = "1",

doi = "10.1016/j.cej.2024.149226",

language = "English",

volume = "483",

journal = "Chemical Engineering Journal",

issn = "1385-8947",

publisher = "Elsevier B.V.",

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Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory. / Yi, Genping; Wang, Bo; Lu, Sen et al.
I: Chemical Engineering Journal, Bind 483, 149226, 01.03.2024.

Publikation: Bidrag til tidsskrift/Konferencebidrag i tidsskrift /Bidrag til avis › Tidsskriftartikel › Forskning › peer review

TY - JOUR

T1 - Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory

AU - Yi, Genping

AU - Wang, Bo

AU - Lu, Sen

AU - Zhang, Liying

AU - Liu, Wenzong

AU - Chen, Zheyu

AU - Yang, Liming

AU - Luo, Xubiao

AU - Wang, Ai Jie

PY - 2024/3/1

Y1 - 2024/3/1

N2 - Electro-generated atomic hydrogen (H*) plays a crucial role in the electrochemical reduction process, serving as the key species that mediates the electrocatalytic hydrogenation reduction of stubborn contaminants in wastewater treatment. However, precisely identifying and quantifying transient atomic H* presents a significant challenge due to its limited lifespan and its existence solely within the boundary layer at the electrode/solution interface. Herein, we developed the electrodeposition of palladium nanoparticles onto carbon cloth and assessed its effectiveness as a cathode for generating and stabilizing atomic H*. The environmental application of atomic H* was validated through the dechlorination of 2, 4-dichlorophenol wastewater and the reduction of antimonite wastewater. Additionally, the identification of atomic H* was verified by electrochemical measurements, high-resolution mass spectra, and density functional theory. Moreover, introducing an excess of a spin trapping agent (5,5-dimethyl-1-pyrroline-N-oxide) and fast in-situ spin trapping facilitated creating favorable conditions for efficient trapping of atomic H* and subsequent electron spin resonance (ESR) spectroscopy quantification analysis. Subsequently, the quantification of atomic H* was achieved by double integration of the ESR signal of spin adduct and comparison with the external standard agent (4-hydroxy-2,2,6,6-tetramethyl-1-piperidine 1-oxyl). This study introduces a novel method for in-situ spin trapping and quantification of atomic H*, facilitating the advancement of electrochemical reduction technology and its application in wastewater treatment.

AB - Electro-generated atomic hydrogen (H*) plays a crucial role in the electrochemical reduction process, serving as the key species that mediates the electrocatalytic hydrogenation reduction of stubborn contaminants in wastewater treatment. However, precisely identifying and quantifying transient atomic H* presents a significant challenge due to its limited lifespan and its existence solely within the boundary layer at the electrode/solution interface. Herein, we developed the electrodeposition of palladium nanoparticles onto carbon cloth and assessed its effectiveness as a cathode for generating and stabilizing atomic H*. The environmental application of atomic H* was validated through the dechlorination of 2, 4-dichlorophenol wastewater and the reduction of antimonite wastewater. Additionally, the identification of atomic H* was verified by electrochemical measurements, high-resolution mass spectra, and density functional theory. Moreover, introducing an excess of a spin trapping agent (5,5-dimethyl-1-pyrroline-N-oxide) and fast in-situ spin trapping facilitated creating favorable conditions for efficient trapping of atomic H* and subsequent electron spin resonance (ESR) spectroscopy quantification analysis. Subsequently, the quantification of atomic H* was achieved by double integration of the ESR signal of spin adduct and comparison with the external standard agent (4-hydroxy-2,2,6,6-tetramethyl-1-piperidine 1-oxyl). This study introduces a novel method for in-situ spin trapping and quantification of atomic H*, facilitating the advancement of electrochemical reduction technology and its application in wastewater treatment.

KW - Atomic hydrogen

KW - Electrochemical reduction

KW - Electron spin resonance

KW - Environmental applications

KW - Identification and quantification

UR - http://www.scopus.com/inward/record.url?scp=85184778812&partnerID=8YFLogxK

U2 - 10.1016/j.cej.2024.149226

DO - 10.1016/j.cej.2024.149226

M3 - Journal article

AN - SCOPUS:85184778812

SN - 1385-8947

VL - 483

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 149226

ER -

Identification and quantification of electron-generated atomic hydrogen through in-situ electron spin resonance and density functional theory

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