Trifunctional Single-Atomic Ru Sites Enable Efficient Overall Water Splitting and Oxygen Reduction in Acidic Media

Xianyun Peng; Shunzheng Zhao; Yuying Mi; Lili Han; Xijun Liu; Defeng Qi; Jiaqiang Sun; Yifan Liu; Haihong Bao; Longchao Zhuo; Huolin L. Xin; Jun Luo; Xiaoming Sun

doi:10.1002/smll.202002888

Trifunctional Single-Atomic Ru Sites Enable Efficient Overall Water Splitting and Oxygen Reduction in Acidic Media

Xianyun Peng, Shunzheng Zhao, Yuying Mi, Lili Han, Xijun Liu, Defeng Qi, Jiaqiang Sun, Yifan Liu, Haihong Bao, Longchao Zhuo, Huolin L. Xin, Jun Luo, Xiaoming Sun

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

170 Scopus citations

Abstract

Development of cost-effective, active trifunctional catalysts for acidic oxygen reduction (ORR) as well as hydrogen and oxygen evolution reactions (HER and OER, respectively) is highly desirable, albeit challenging. Herein, single-atomic Ru sites anchored onto Ti₃C₂T_x MXene nanosheets are first reported to serve as trifunctional electrocatalysts for simultaneously catalyzing acidic HER, OER, and ORR. A half-wave potential of 0.80 V for ORR and small overpotentials of 290 and 70 mV for OER and HER, respectively, at 10 mA cm⁻² are achieved. Hence, a low cell voltage of 1.56 V is required for the acidic overall water splitting. The maximum power density of an H₂–O₂ fuel cell using the as-prepared catalyst can reach as high as 941 mW cm⁻². Theoretical calculations reveal that isolated Ru–O₂ sites can effectively optimize the adsorption of reactants/intermediates and lower the energy barriers for the potential-determining steps, thereby accelerating the HER, ORR, and OER kinetics.

Original language	English
Article number	2002888
Journal	Small
Volume	16
Issue number	33
DOIs	https://doi.org/10.1002/smll.202002888
State	Published - Aug 1 2020
Externally published	Yes

Funding

This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (51971157, 21601136, 51808037, and 51761165012), and Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800). This work made use of the resources of the Wuxi Research Institute of Applied Technologies of Tsinghua University. The authors also acknowledged Beijing Super Cloud Computing Center for providing the computational resources and materials studio. This research used the 7-BM beamline of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (51971157, 21601136, 51808037, and 51761165012), and Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800). This work made use of the resources of the Wuxi Research Institute of Applied Technologies of Tsinghua University. The authors also acknowledged Beijing Super Cloud Computing Center for providing the computational resources and materials studio. This research used the 7‐BM beamline of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704.

Keywords

acidic environment
overall water splitting
oxygen reduction
single-atomic Ru sites
trifunctional catalysts

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10.1002/smll.202002888

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title = "Trifunctional Single-Atomic Ru Sites Enable Efficient Overall Water Splitting and Oxygen Reduction in Acidic Media",

abstract = "Development of cost-effective, active trifunctional catalysts for acidic oxygen reduction (ORR) as well as hydrogen and oxygen evolution reactions (HER and OER, respectively) is highly desirable, albeit challenging. Herein, single-atomic Ru sites anchored onto Ti3C2Tx MXene nanosheets are first reported to serve as trifunctional electrocatalysts for simultaneously catalyzing acidic HER, OER, and ORR. A half-wave potential of 0.80 V for ORR and small overpotentials of 290 and 70 mV for OER and HER, respectively, at 10 mA cm−2 are achieved. Hence, a low cell voltage of 1.56 V is required for the acidic overall water splitting. The maximum power density of an H2–O2 fuel cell using the as-prepared catalyst can reach as high as 941 mW cm−2. Theoretical calculations reveal that isolated Ru–O2 sites can effectively optimize the adsorption of reactants/intermediates and lower the energy barriers for the potential-determining steps, thereby accelerating the HER, ORR, and OER kinetics.",

keywords = "acidic environment, overall water splitting, oxygen reduction, single-atomic Ru sites, trifunctional catalysts",

author = "Xianyun Peng and Shunzheng Zhao and Yuying Mi and Lili Han and Xijun Liu and Defeng Qi and Jiaqiang Sun and Yifan Liu and Haihong Bao and Longchao Zhuo and Xin, {Huolin L.} and Jun Luo and Xiaoming Sun",

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year = "2020",

month = aug,

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doi = "10.1002/smll.202002888",

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T1 - Trifunctional Single-Atomic Ru Sites Enable Efficient Overall Water Splitting and Oxygen Reduction in Acidic Media

AU - Peng, Xianyun

AU - Zhao, Shunzheng

AU - Mi, Yuying

AU - Han, Lili

AU - Liu, Xijun

AU - Qi, Defeng

AU - Sun, Jiaqiang

AU - Liu, Yifan

AU - Bao, Haihong

AU - Zhuo, Longchao

AU - Xin, Huolin L.

AU - Luo, Jun

AU - Sun, Xiaoming

PY - 2020/8/1

Y1 - 2020/8/1

N2 - Development of cost-effective, active trifunctional catalysts for acidic oxygen reduction (ORR) as well as hydrogen and oxygen evolution reactions (HER and OER, respectively) is highly desirable, albeit challenging. Herein, single-atomic Ru sites anchored onto Ti3C2Tx MXene nanosheets are first reported to serve as trifunctional electrocatalysts for simultaneously catalyzing acidic HER, OER, and ORR. A half-wave potential of 0.80 V for ORR and small overpotentials of 290 and 70 mV for OER and HER, respectively, at 10 mA cm−2 are achieved. Hence, a low cell voltage of 1.56 V is required for the acidic overall water splitting. The maximum power density of an H2–O2 fuel cell using the as-prepared catalyst can reach as high as 941 mW cm−2. Theoretical calculations reveal that isolated Ru–O2 sites can effectively optimize the adsorption of reactants/intermediates and lower the energy barriers for the potential-determining steps, thereby accelerating the HER, ORR, and OER kinetics.

AB - Development of cost-effective, active trifunctional catalysts for acidic oxygen reduction (ORR) as well as hydrogen and oxygen evolution reactions (HER and OER, respectively) is highly desirable, albeit challenging. Herein, single-atomic Ru sites anchored onto Ti3C2Tx MXene nanosheets are first reported to serve as trifunctional electrocatalysts for simultaneously catalyzing acidic HER, OER, and ORR. A half-wave potential of 0.80 V for ORR and small overpotentials of 290 and 70 mV for OER and HER, respectively, at 10 mA cm−2 are achieved. Hence, a low cell voltage of 1.56 V is required for the acidic overall water splitting. The maximum power density of an H2–O2 fuel cell using the as-prepared catalyst can reach as high as 941 mW cm−2. Theoretical calculations reveal that isolated Ru–O2 sites can effectively optimize the adsorption of reactants/intermediates and lower the energy barriers for the potential-determining steps, thereby accelerating the HER, ORR, and OER kinetics.

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Trifunctional Single-Atomic Ru Sites Enable Efficient Overall Water Splitting and Oxygen Reduction in Acidic Media

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