The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
基于重庆市气象局业务运行的风暴尺度快速同化和预报系统(Storm-Scale Rapid Assimilation and Forecast System,SSRAFS)、气象信息综合分析处理系统(Meteorological Information Comprehensive Analysis And Process System,MICAPS)地...基于重庆市气象局业务运行的风暴尺度快速同化和预报系统(Storm-Scale Rapid Assimilation and Forecast System,SSRAFS)、气象信息综合分析处理系统(Meteorological Information Comprehensive Analysis And Process System,MICAPS)地面观测和高空观测资料,进行模式输出统计(Model Output Statistics,MOS)方法和纳入超前实况因子的MOS(MOS with Prior Observation Predictors,OMOS)方法对重庆地区地面气温96 h内逐小时预报试验,并以SSRAFS地面气温预报结果作为参考进行对比分析。结果表明:MOS方法在1~96 h预报时效内的预报技巧高于SSRAFS,气温预报均方根误差(Root Mean Square Error,RMSE)平均减小1.22℃,CC和HR2分别平均增大0.006和20.4%;在1~7 h预报时效,RMSE平均减小1.70℃,CC和HR2分别平均增大0.07和34.5%;且MOS方法在重庆东北部及中南部地区改进效果较为明显。OMOS方法在气温短期预报中表现优于MOS方法,尤其在1~7 h预报时效,比MOS方法RMSE平均减小0.43℃,CC和HR2分别平均增大0.008和8.3%;其在1~4 h预报时效时表现更加优异,与MOS方法相比,RMSE平均减小0.66℃,CC和HR2分别平均增大0.13和12.3%。因此,在MOS的基础上,OMOS能够进一步提升地面气温的预报技巧,且在重庆东北部及中南部地区的预报效果有明显改进。展开更多
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
文摘基于重庆市气象局业务运行的风暴尺度快速同化和预报系统(Storm-Scale Rapid Assimilation and Forecast System,SSRAFS)、气象信息综合分析处理系统(Meteorological Information Comprehensive Analysis And Process System,MICAPS)地面观测和高空观测资料,进行模式输出统计(Model Output Statistics,MOS)方法和纳入超前实况因子的MOS(MOS with Prior Observation Predictors,OMOS)方法对重庆地区地面气温96 h内逐小时预报试验,并以SSRAFS地面气温预报结果作为参考进行对比分析。结果表明:MOS方法在1~96 h预报时效内的预报技巧高于SSRAFS,气温预报均方根误差(Root Mean Square Error,RMSE)平均减小1.22℃,CC和HR2分别平均增大0.006和20.4%;在1~7 h预报时效,RMSE平均减小1.70℃,CC和HR2分别平均增大0.07和34.5%;且MOS方法在重庆东北部及中南部地区改进效果较为明显。OMOS方法在气温短期预报中表现优于MOS方法,尤其在1~7 h预报时效,比MOS方法RMSE平均减小0.43℃,CC和HR2分别平均增大0.008和8.3%;其在1~4 h预报时效时表现更加优异,与MOS方法相比,RMSE平均减小0.66℃,CC和HR2分别平均增大0.13和12.3%。因此,在MOS的基础上,OMOS能够进一步提升地面气温的预报技巧,且在重庆东北部及中南部地区的预报效果有明显改进。
