Pyrite-type ruthenium disulfide with tunable disorder and defects enables ultra-efficient overall water splitting

Yinlong Zhu, Hassan A. Tahini, Yang Wang, Qian Lin, Yan Liang, Cara M. Doherty, Yue Liu, Xingya Li, Jun Lu, Sean Smith, Cordelia Selomulya, Xiwang Zhang, Zongping Shao, Huanting Wang

Research output: Contribution to journalArticleResearchpeer-review

Abstract

The exploration of efficient electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is significant for water splitting associated with the storage of clean and renewable energy. Here, we report a simple and scalable low-temperature sulfuration method to achieve simultaneous modulation of disorder and defects in pyrite-type RuS2 nanoparticles to dramatically enhance the HER and OER catalytic activity. The disordered structure can increase the electrochemically active surface area, while defect engineering can effectively regulate the electronic structure and thus improve the intrinsic activity, as revealed by combined experimental and theoretical density functional theory (DFT) investigations. Through controllable disorder and defect engineering, the optimized RuS2-500 catalyst (with a sulfuration temperature of 500 °C) supported on a glassy carbon electrode exhibits ultra-efficient bifunctional electrocatalytic activity with η-10 = 78 mV for the HER and η10 = 282 mV for the OER, superior to various Ru-based and pyrite-type catalysts. Remarkably, when used as both the anode and the cathode in an alkaline water electrolyzer, RuS2-500 delivers 10 mA cm-2 at an ultralow cell voltage of 1.527 V with long-term stability, outperforming the benchmark Pt/C//RuO2 couple and most state-of-the-art overall-water-splitting electrocatalysts ever reported. This work thus provides a new and facile way for improving the catalytic activity through a synergistic modulation strategy.

Original languageEnglish
Pages (from-to)14222-14232
Number of pages11
JournalJournal of Materials Chemistry A
Volume7
Issue number23
DOIs
Publication statusPublished - 17 May 2019

Cite this

Zhu, Yinlong ; Tahini, Hassan A. ; Wang, Yang ; Lin, Qian ; Liang, Yan ; Doherty, Cara M. ; Liu, Yue ; Li, Xingya ; Lu, Jun ; Smith, Sean ; Selomulya, Cordelia ; Zhang, Xiwang ; Shao, Zongping ; Wang, Huanting. / Pyrite-type ruthenium disulfide with tunable disorder and defects enables ultra-efficient overall water splitting. In: Journal of Materials Chemistry A. 2019 ; Vol. 7, No. 23. pp. 14222-14232.
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abstract = "The exploration of efficient electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is significant for water splitting associated with the storage of clean and renewable energy. Here, we report a simple and scalable low-temperature sulfuration method to achieve simultaneous modulation of disorder and defects in pyrite-type RuS2 nanoparticles to dramatically enhance the HER and OER catalytic activity. The disordered structure can increase the electrochemically active surface area, while defect engineering can effectively regulate the electronic structure and thus improve the intrinsic activity, as revealed by combined experimental and theoretical density functional theory (DFT) investigations. Through controllable disorder and defect engineering, the optimized RuS2-500 catalyst (with a sulfuration temperature of 500 °C) supported on a glassy carbon electrode exhibits ultra-efficient bifunctional electrocatalytic activity with η-10 = 78 mV for the HER and η10 = 282 mV for the OER, superior to various Ru-based and pyrite-type catalysts. Remarkably, when used as both the anode and the cathode in an alkaline water electrolyzer, RuS2-500 delivers 10 mA cm-2 at an ultralow cell voltage of 1.527 V with long-term stability, outperforming the benchmark Pt/C//RuO2 couple and most state-of-the-art overall-water-splitting electrocatalysts ever reported. This work thus provides a new and facile way for improving the catalytic activity through a synergistic modulation strategy.",
author = "Yinlong Zhu and Tahini, {Hassan A.} and Yang Wang and Qian Lin and Yan Liang and Doherty, {Cara M.} and Yue Liu and Xingya Li and Jun Lu and Sean Smith and Cordelia Selomulya and Xiwang Zhang and Zongping Shao and Huanting Wang",
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Pyrite-type ruthenium disulfide with tunable disorder and defects enables ultra-efficient overall water splitting. / Zhu, Yinlong; Tahini, Hassan A.; Wang, Yang; Lin, Qian; Liang, Yan; Doherty, Cara M.; Liu, Yue; Li, Xingya; Lu, Jun; Smith, Sean ; Selomulya, Cordelia; Zhang, Xiwang; Shao, Zongping; Wang, Huanting.

In: Journal of Materials Chemistry A, Vol. 7, No. 23, 17.05.2019, p. 14222-14232.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Zhu, Yinlong

AU - Tahini, Hassan A.

AU - Wang, Yang

AU - Lin, Qian

AU - Liang, Yan

AU - Doherty, Cara M.

AU - Liu, Yue

AU - Li, Xingya

AU - Lu, Jun

AU - Smith, Sean

AU - Selomulya, Cordelia

AU - Zhang, Xiwang

AU - Shao, Zongping

AU - Wang, Huanting

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N2 - The exploration of efficient electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is significant for water splitting associated with the storage of clean and renewable energy. Here, we report a simple and scalable low-temperature sulfuration method to achieve simultaneous modulation of disorder and defects in pyrite-type RuS2 nanoparticles to dramatically enhance the HER and OER catalytic activity. The disordered structure can increase the electrochemically active surface area, while defect engineering can effectively regulate the electronic structure and thus improve the intrinsic activity, as revealed by combined experimental and theoretical density functional theory (DFT) investigations. Through controllable disorder and defect engineering, the optimized RuS2-500 catalyst (with a sulfuration temperature of 500 °C) supported on a glassy carbon electrode exhibits ultra-efficient bifunctional electrocatalytic activity with η-10 = 78 mV for the HER and η10 = 282 mV for the OER, superior to various Ru-based and pyrite-type catalysts. Remarkably, when used as both the anode and the cathode in an alkaline water electrolyzer, RuS2-500 delivers 10 mA cm-2 at an ultralow cell voltage of 1.527 V with long-term stability, outperforming the benchmark Pt/C//RuO2 couple and most state-of-the-art overall-water-splitting electrocatalysts ever reported. This work thus provides a new and facile way for improving the catalytic activity through a synergistic modulation strategy.

AB - The exploration of efficient electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is significant for water splitting associated with the storage of clean and renewable energy. Here, we report a simple and scalable low-temperature sulfuration method to achieve simultaneous modulation of disorder and defects in pyrite-type RuS2 nanoparticles to dramatically enhance the HER and OER catalytic activity. The disordered structure can increase the electrochemically active surface area, while defect engineering can effectively regulate the electronic structure and thus improve the intrinsic activity, as revealed by combined experimental and theoretical density functional theory (DFT) investigations. Through controllable disorder and defect engineering, the optimized RuS2-500 catalyst (with a sulfuration temperature of 500 °C) supported on a glassy carbon electrode exhibits ultra-efficient bifunctional electrocatalytic activity with η-10 = 78 mV for the HER and η10 = 282 mV for the OER, superior to various Ru-based and pyrite-type catalysts. Remarkably, when used as both the anode and the cathode in an alkaline water electrolyzer, RuS2-500 delivers 10 mA cm-2 at an ultralow cell voltage of 1.527 V with long-term stability, outperforming the benchmark Pt/C//RuO2 couple and most state-of-the-art overall-water-splitting electrocatalysts ever reported. This work thus provides a new and facile way for improving the catalytic activity through a synergistic modulation strategy.

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SN - 2050-7488

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