Fast and Stable Electrochemical Production of H2O2by Electrode Architecture Engineering

Wenwen Xu; Zheng Liang; Shun Gong; Baoshan Zhang; Hui Wang; Linfeng Su; Xu Chen; Nana Han; Ziqi Tian; Tanja Kallio; Liang Chen; Zhiyi Lu; Xiaoming Sun

doi:10.1021/acssuschemeng.1c01468

Fast and Stable Electrochemical Production of H₂O₂by Electrode Architecture Engineering

Wenwen Xu
, Zheng Liang
, Shun Gong
, Baoshan Zhang
, Hui Wang
, Linfeng Su
, Xu Chen
, Nana Han
, Ziqi Tian
, Tanja Kallio
, Liang Chen^*
, Zhiyi Lu
, Xiaoming Sun

^*Corresponding author for this work

CAS - Ningbo Institute of Material Technology and Engineering
Shanghai Jiao Tong University
University of Chinese Academy of Sciences
Beijing University of Chemical Technology

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

48 Citations (Scopus)

195 Downloads (Pure)

Abstract

Fast and stable production of hydrogen peroxide (H2O2) through electrochemical pathways is crucial for wastewater treatment applications. With this objective, herein, we report an integrated and superaerophilic electrode composed of atomically dispersed Ni-O-C site-enriched carbon nanosheets (IS-NiOC electrode) for electrochemical oxygen reduction to produce H2O2. Both experimental and theoretical results have proven that atomically dispersed Ni-O-C sites enable a low overpotential (260 mV at 0.1 mA cm-2) and high selectivity (>90% at 0.0-0.5 V vs reversible hydrogen electrode (RHE)) in a neutral electrolyte. Compared with a commercial gas-diffusion electrode, the IS-NiOC electrode offers stronger affinity to oxygen bubbles and more robust three-phase contact points, resulting in high current density (∼106 mA cm-2 at 0.25 V vs RHE) and superior stability (∼200 h). These merits allow the application of the IS-NiOC electrode in an electro-Fenton-like process, which enables fast degradation of representative organic pollutants in both a steady state and a flow state.

Original language	English
Pages (from-to)	7120-7129
Number of pages	10
Journal	ACS Sustainable Chemistry & Engineering
Volume	9
Issue number	20
Early online date	11 May 2021
DOIs	https://doi.org/10.1021/acssuschemeng.1c01468
Publication status	Published - 24 May 2021
MoE publication type	A1 Journal article-refereed

Funding

This work was supported by the Ningbo S&T Innovation 2025 Major Special Program (2020Z059 and 2020Z107), the BoXin project (BX20190339), the Natural Science Foundation of Ningbo (Nos. 2019A610442 and 202003N4351), the China Postdoctoral Science Foundation (Nos. 2019M662127and 2019M662124), and the Hundred Talents Programs in Chinese Academy of Science. The DFT calculation was supported by the High-Performance Computing Center of Collaborative Innovation Center of Advanced Microstructures, Nanjing University.

UN SDGs

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

SDG 6 Clean Water and Sanitation

Keywords

electrocataysis
Fenton-like process
hydrogen peroxide
oxygen reduction reaction
superaerophilic electrode

Access to Document

10.1021/acssuschemeng.1c01468

CHEM_Xu_et_al_Fast_and_Stable_Electrochemical_Production_2021_ACS_Sustainable_Chemistry_and_EngineeringAccepted author manuscript, 1.94 MBLicence: Unspecified

Cite this

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title = "Fast and Stable Electrochemical Production of H2O2by Electrode Architecture Engineering",

abstract = "Fast and stable production of hydrogen peroxide (H2O2) through electrochemical pathways is crucial for wastewater treatment applications. With this objective, herein, we report an integrated and superaerophilic electrode composed of atomically dispersed Ni-O-C site-enriched carbon nanosheets (IS-NiOC electrode) for electrochemical oxygen reduction to produce H2O2. Both experimental and theoretical results have proven that atomically dispersed Ni-O-C sites enable a low overpotential (260 mV at 0.1 mA cm-2) and high selectivity (>90\% at 0.0-0.5 V vs reversible hydrogen electrode (RHE)) in a neutral electrolyte. Compared with a commercial gas-diffusion electrode, the IS-NiOC electrode offers stronger affinity to oxygen bubbles and more robust three-phase contact points, resulting in high current density (∼106 mA cm-2 at 0.25 V vs RHE) and superior stability (∼200 h). These merits allow the application of the IS-NiOC electrode in an electro-Fenton-like process, which enables fast degradation of representative organic pollutants in both a steady state and a flow state. ",

keywords = "electrocataysis, Fenton-like process, hydrogen peroxide, oxygen reduction reaction, superaerophilic electrode",

author = "Wenwen Xu and Zheng Liang and Shun Gong and Baoshan Zhang and Hui Wang and Linfeng Su and Xu Chen and Nana Han and Ziqi Tian and Tanja Kallio and Liang Chen and Zhiyi Lu and Xiaoming Sun",

note = "Funding Information: This work was supported by the Ningbo S\&T Innovation 2025 Major Special Program (2020Z059 and 2020Z107), the BoXin project (BX20190339), the Natural Science Foundation of Ningbo (Nos. 2019A610442 and 202003N4351), the China Postdoctoral Science Foundation (Nos. 2019M662127and 2019M662124), and the Hundred Talents Programs in Chinese Academy of Science. The DFT calculation was supported by the High-Performance Computing Center of Collaborative Innovation Center of Advanced Microstructures, Nanjing University. Publisher Copyright: {\textcopyright} ",

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language = "English",

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T1 - Fast and Stable Electrochemical Production of H2O2by Electrode Architecture Engineering

AU - Xu, Wenwen

AU - Liang, Zheng

AU - Gong, Shun

AU - Zhang, Baoshan

AU - Wang, Hui

AU - Su, Linfeng

AU - Chen, Xu

AU - Han, Nana

AU - Tian, Ziqi

AU - Kallio, Tanja

AU - Chen, Liang

AU - Lu, Zhiyi

AU - Sun, Xiaoming

N1 - Funding Information: This work was supported by the Ningbo S&T Innovation 2025 Major Special Program (2020Z059 and 2020Z107), the BoXin project (BX20190339), the Natural Science Foundation of Ningbo (Nos. 2019A610442 and 202003N4351), the China Postdoctoral Science Foundation (Nos. 2019M662127and 2019M662124), and the Hundred Talents Programs in Chinese Academy of Science. The DFT calculation was supported by the High-Performance Computing Center of Collaborative Innovation Center of Advanced Microstructures, Nanjing University. Publisher Copyright: ©

PY - 2021/5/24

Y1 - 2021/5/24

N2 - Fast and stable production of hydrogen peroxide (H2O2) through electrochemical pathways is crucial for wastewater treatment applications. With this objective, herein, we report an integrated and superaerophilic electrode composed of atomically dispersed Ni-O-C site-enriched carbon nanosheets (IS-NiOC electrode) for electrochemical oxygen reduction to produce H2O2. Both experimental and theoretical results have proven that atomically dispersed Ni-O-C sites enable a low overpotential (260 mV at 0.1 mA cm-2) and high selectivity (>90% at 0.0-0.5 V vs reversible hydrogen electrode (RHE)) in a neutral electrolyte. Compared with a commercial gas-diffusion electrode, the IS-NiOC electrode offers stronger affinity to oxygen bubbles and more robust three-phase contact points, resulting in high current density (∼106 mA cm-2 at 0.25 V vs RHE) and superior stability (∼200 h). These merits allow the application of the IS-NiOC electrode in an electro-Fenton-like process, which enables fast degradation of representative organic pollutants in both a steady state and a flow state.

AB - Fast and stable production of hydrogen peroxide (H2O2) through electrochemical pathways is crucial for wastewater treatment applications. With this objective, herein, we report an integrated and superaerophilic electrode composed of atomically dispersed Ni-O-C site-enriched carbon nanosheets (IS-NiOC electrode) for electrochemical oxygen reduction to produce H2O2. Both experimental and theoretical results have proven that atomically dispersed Ni-O-C sites enable a low overpotential (260 mV at 0.1 mA cm-2) and high selectivity (>90% at 0.0-0.5 V vs reversible hydrogen electrode (RHE)) in a neutral electrolyte. Compared with a commercial gas-diffusion electrode, the IS-NiOC electrode offers stronger affinity to oxygen bubbles and more robust three-phase contact points, resulting in high current density (∼106 mA cm-2 at 0.25 V vs RHE) and superior stability (∼200 h). These merits allow the application of the IS-NiOC electrode in an electro-Fenton-like process, which enables fast degradation of representative organic pollutants in both a steady state and a flow state.

KW - electrocataysis

KW - Fenton-like process

KW - hydrogen peroxide

KW - oxygen reduction reaction

KW - superaerophilic electrode

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