Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H2O2

Yingjun Sun; Zhengyi Qian; Mingzi Sun; Yingjie Li; Qinghua Zhang; Yan Nie; Lin Gu; Mingchuan Luo; Jianguo Liu; Bolong Huang; Shaojun Guo

doi:10.1016/j.chempr.2024.102393

Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H₂O₂

Yingjun Sun, Zhengyi Qian, Mingzi Sun, Yingjie Li, Qinghua Zhang, Yan Nie, Lin Gu, Mingchuan Luo, Jianguo Liu, Bolong Huang^*, Shaojun Guo^*

^*Corresponding author for this work

Department of Chemistry

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

4 Citations (Scopus)

Abstract

Electrocatalytic hydrogen peroxide (H₂O₂) production from O₂ reduction is attractive because of its wide applications; however, the lack of efficient and selective electrocatalysts hinders its further development. Herein, we have created a class of electrocatalysts by anchoring osmium (Os) single atomic sites on ultrathin copper sulfide nanoplates (Os₁-CuS NPs) to greatly boost the electroreduction of O₂ into H₂O₂ via a two-electron pathway. The Os single-atomic-site catalyst with sulfur coordination achieved a record-high Os loading (25.9 wt %) and an exceptional H₂O₂ production rate (8.2 mol g_cat⁻¹ h⁻¹) with near-perfect selectivity (∼98%), making it a top performer among metal-based electrocatalysts. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations revealed that the introduced Os sites promote a selective 2e⁻ oxygen reduction pathway by strengthening OOH binding and thus suppressing the undesired 4e⁻ pathway. This study advances the design of high-performance single-atomic-site electrocatalysts for selective H₂O₂ generation. © 2024 Elsevier Inc.

Original language	English
Article number	102393
Journal	Chem
Online published	29 Jan 2025
DOIs	https://doi.org/10.1016/j.chempr.2024.102393
Publication status	Online published - 29 Jan 2025

Funding

This study was financially supported by the National Science Fund for Distinguished Young Scholars (no. 52025133), the Beijing Outstanding Young Scientist Program (JWZQ20240102004), the Tencent Foundation through the XPLORER PRIZE, the National Natural Science Foundation of China (no. 52103330), the National Natural Science Foundation of China/RGC Joint Research Scheme (no. N_PolyU502/21), and funding for Projects of Strategic Importance of the Hong Kong Polytechnic University (project code 1-ZE2V).

Research Keywords

electrocatalysis
electrosynthesis of H2O2
nanoplates
oxygen reduction reaction
SDG7: Affordable and clean energy
single-atomic-site catalysts

RGC Funding Information

RGC-funded

UN SDGs

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

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title = "Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H2O2",

abstract = "Electrocatalytic hydrogen peroxide (H2O2) production from O2 reduction is attractive because of its wide applications; however, the lack of efficient and selective electrocatalysts hinders its further development. Herein, we have created a class of electrocatalysts by anchoring osmium (Os) single atomic sites on ultrathin copper sulfide nanoplates (Os1-CuS NPs) to greatly boost the electroreduction of O2 into H2O2 via a two-electron pathway. The Os single-atomic-site catalyst with sulfur coordination achieved a record-high Os loading (25.9 wt %) and an exceptional H2O2 production rate (8.2 mol gcat−1 h−1) with near-perfect selectivity (∼98%), making it a top performer among metal-based electrocatalysts. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations revealed that the introduced Os sites promote a selective 2e− oxygen reduction pathway by strengthening OOH binding and thus suppressing the undesired 4e− pathway. This study advances the design of high-performance single-atomic-site electrocatalysts for selective H2O2 generation. {\textcopyright} 2024 Elsevier Inc.",

keywords = "electrocatalysis, electrosynthesis of H2O2, nanoplates, oxygen reduction reaction, SDG7: Affordable and clean energy, single-atomic-site catalysts",

author = "Yingjun Sun and Zhengyi Qian and Mingzi Sun and Yingjie Li and Qinghua Zhang and Yan Nie and Lin Gu and Mingchuan Luo and Jianguo Liu and Bolong Huang and Shaojun Guo",

year = "2025",

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TY - JOUR

T1 - Osmium atomic sites on CuS nanoplates for efficient two-electron oxygen reduction into H2O2

AU - Sun, Yingjun

AU - Qian, Zhengyi

AU - Sun, Mingzi

AU - Li, Yingjie

AU - Zhang, Qinghua

AU - Nie, Yan

AU - Gu, Lin

AU - Luo, Mingchuan

AU - Liu, Jianguo

AU - Huang, Bolong

AU - Guo, Shaojun

PY - 2025/1/29

Y1 - 2025/1/29

N2 - Electrocatalytic hydrogen peroxide (H2O2) production from O2 reduction is attractive because of its wide applications; however, the lack of efficient and selective electrocatalysts hinders its further development. Herein, we have created a class of electrocatalysts by anchoring osmium (Os) single atomic sites on ultrathin copper sulfide nanoplates (Os1-CuS NPs) to greatly boost the electroreduction of O2 into H2O2 via a two-electron pathway. The Os single-atomic-site catalyst with sulfur coordination achieved a record-high Os loading (25.9 wt %) and an exceptional H2O2 production rate (8.2 mol gcat−1 h−1) with near-perfect selectivity (∼98%), making it a top performer among metal-based electrocatalysts. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations revealed that the introduced Os sites promote a selective 2e− oxygen reduction pathway by strengthening OOH binding and thus suppressing the undesired 4e− pathway. This study advances the design of high-performance single-atomic-site electrocatalysts for selective H2O2 generation. © 2024 Elsevier Inc.

AB - Electrocatalytic hydrogen peroxide (H2O2) production from O2 reduction is attractive because of its wide applications; however, the lack of efficient and selective electrocatalysts hinders its further development. Herein, we have created a class of electrocatalysts by anchoring osmium (Os) single atomic sites on ultrathin copper sulfide nanoplates (Os1-CuS NPs) to greatly boost the electroreduction of O2 into H2O2 via a two-electron pathway. The Os single-atomic-site catalyst with sulfur coordination achieved a record-high Os loading (25.9 wt %) and an exceptional H2O2 production rate (8.2 mol gcat−1 h−1) with near-perfect selectivity (∼98%), making it a top performer among metal-based electrocatalysts. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations revealed that the introduced Os sites promote a selective 2e− oxygen reduction pathway by strengthening OOH binding and thus suppressing the undesired 4e− pathway. This study advances the design of high-performance single-atomic-site electrocatalysts for selective H2O2 generation. © 2024 Elsevier Inc.

KW - electrocatalysis

KW - electrosynthesis of H2O2

KW - nanoplates

KW - oxygen reduction reaction

KW - SDG7: Affordable and clean energy

KW - single-atomic-site catalysts

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