摘要
Green hydrogen(H_(2))is an import energy carrier due to the zero-carbon emission in the energy cycle.Nevertheless,green H_(2)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 Ru_(2)0@mONC realizes remarkable catalytic activity and stability towards both HER and HzOR regardless of electrolytes.As a result,the electrode pair of Ru_(2)0@mONC//Ru_(2)0@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 H_(2)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 Ru_(2)0@mONC,which not only contributes to the balancing of H*adsorption/desorption in HER but also facilitates the*N_(2)H_(2)dehydrogenation in HzOR.
基金
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.