Ru/NC heterointerfaces boost energy-efficient production of green H2 over a wide pH range
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Green hydrogen (H2) is an import energy carrier due to the zero-carbon emission in the energy cycle. Nevertheless, green H2 production based on electrolyzer and photovoltaics (EZ/PV) remains limited due to the highly pH-dependant and energy exhausting overall water splitting. Herein, we report a series of Ru-nanocluster-modified mesoporous nanospheres (Rux@mONC) as pH-universal electrocatalysts towards both hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR). The optimal catalyst Ru20@mONC realizes remarkable catalytic activity and stability towards both HER and HzOR regardless of electrolytes. As a result, the electrode pair of Ru20@mONC//Ru20@mONC requires low cell-potentials of 39/429, 405/926, and 164/1,141 mV to achieve the current density of 10/100 mA·cm−2, as well as the long-term stability for HzOR assisted electrochemical water splitting in alkaline, acidic, and neutral media, respectively. Those performances are more promising compared to the state-of-the-art electrocatalysts so far reported. A proof-of-concept test demonstrates an efficient production of green H2 powered by a single-junction silicon solar cell, which may inspire the use of a cost-effective EZ/PV system. Furthermore, a combined spectroscopic and theoretical study verifies the formation of abundant Ru/NC heterointerfaces in Ru20@mONC, which not only contributes to the balancing of H* adsorption/desorption in HER but also facilitates the *N2H2 dehydrogenation in HzOR.
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Ru/NC heterointerfaces boost energy-efficient production of green H2 over a wide pH range
Abstract
Green hydrogen (H2) is an import energy carrier due to the zero-carbon emission in the energy cycle. Nevertheless, green H2 production based on electrolyzer and photovoltaics (EZ/PV) remains limited due to the highly pH-dependant and energy exhausting overall water splitting. Herein, we report a series of Ru-nanocluster-modified mesoporous nanospheres (Rux@mONC) as pH-universal electrocatalysts towards both hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR). The optimal catalyst Ru20@mONC realizes remarkable catalytic activity and stability towards both HER and HzOR regardless of electrolytes. As a result, the electrode pair of Ru20@mONC//Ru20@mONC requires low cell-potentials of 39/429, 405/926, and 164/1,141 mV to achieve the current density of 10/100 mA·cm−2, as well as the long-term stability for HzOR assisted electrochemical water splitting in alkaline, acidic, and neutral media, respectively. Those performances are more promising compared to the state-of-the-art electrocatalysts so far reported. A proof-of-concept test demonstrates an efficient production of green H2 powered by a single-junction silicon solar cell, which may inspire the use of a cost-effective EZ/PV system. Furthermore, a combined spectroscopic and theoretical study verifies the formation of abundant Ru/NC heterointerfaces in Ru20@mONC, which not only contributes to the balancing of H* adsorption/desorption in HER but also facilitates the *N2H2 dehydrogenation in HzOR.
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Acknowledgements
This work is supported in part by the Natural Science Foundation of China (No. 52172050), Natural Science Research Project of Jiangsu Higher Education Institutions (No. 21KJA480002), six talent peaks project in Jiangsu province (No. XCL-078), the National Key Research, and Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies. L. F. also thanks Beijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics of the Chinese Academy of Sciences, for XANES measurements.
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