物理化学学报2021，Vol.37Issue(7)：154-161,8.DOI:10.3866/PKU.WHXB202009082
碳点增强的Ru纳米颗粒复合材料用于碱性条件下高效电解水析氢
Carbon Dots Enhance Ruthenium Nanoparticles for Efficient Hydrogen Production in Alkaline
摘要
Abstract
In the 21 st century,hydrogen energy is a novel energy source.Its use is expected to mitigate the problems of environmental pollution and global warming caused by the excessive use of conventional fossil fuels.The hydrogen evolution reaction(HER)for water splitting has attracted considerable attention because of its environmental friendliness.To improve electrocatalyst performance and reduce operation cost,carbon-based metal hybrid materials exhibiting high efficiency and catalytic activity have been developed.Among them,carbon dots(CDs)have garnered significant research attention and have been widely applied in biosensing,bioimaging,and energy conversion/storage because of their facile synthesis,biocompatibility,tunable photoluminescence,excellent stability,and good electronic properties.CDs are widely used as carriers in the construction of electrocatalysts prepared from carbon-based metal hybrid materials.At present,it is believed that CDs exhibit excellent confinement effects,which can effectively inhibit the growth and agglomeration of metal nanoparticles,thereby preparing well-distributed carbon-based metal hybrid materials with a uniform and controllable size.However,the formation process of the small-molecule raw materials of CDs has not been elucidated.In this study,CDs and small-molecule raw materials from synthetic CDs were used as precursors to prepare nitrogen-doped CD-supported ruthenium nanoparticle(Ru@CDs)and small-molecule-supported ruthenium nanoparticle(Ru@Molecule)hybrid materials,respectively.The interaction between the small molecules and Ru in the process of CD formation and the effect on HER performance were explored.Moreover,we prepared different carriers such as metal organic frameworks(MOF),carbon nanotubes(CNTs),and graphene(GO)-supported ruthenium nanoparticle hybrid materials.Among them,Ru@CDs exhibited controllable size and excellent dispersibility and exhibited outstanding HER activity and good stability.Ru@CDs were found to require a low overpotential of 22 mV to reach a current density of 10 mA·cm-2.Moreover,we observed the presence of an intermediate state between the molecules and CDs and demonstrated that the intermediate state exhibits no confinement effect.Furthermore,we found that with increasing calcination temperature,the intermediate state gradually changes to CDs.The unique spatial confinement between CDs and metal ions is key to the formation of monodisperse Ru nanoparticles.Our results confirmed that Ru@CDs serve as excellent HER catalyst supports.This work not only reveals the effect of the unique spatial confinement of CDs on the supported metals and their promoting effect on electrocatalytic activity but also provides guides the future development of CD-based metal hybrid electrocatalysts.关键词
碳点/碳基载体/杂化材料/电解水产氢Key words
Carbon dots/Carbon-base carriers/Hybrid materials/Hydrogen evolution reaction分类
化学化工引用本文复制引用
刘源,李卫东,吴捍,卢思宇..碳点增强的Ru纳米颗粒复合材料用于碱性条件下高效电解水析氢[J].物理化学学报,2021,37(7):154-161,8.基金项目
This work was supported by the National Natural Science Foundation of China(51973200,21905253)and the China Postdoctoral Science Foundation(2018M640681,2019T120632).国家自然科学基金(51973200,21905253)与中国博士后科学基金(2018M640681,2019T120632)资助 （51973200,21905253）
