The synthesis of nanocrystals(NCs)with defined morphology and surface structure provides an effective way to investigate the structure-activity relationship of nanocatalytsts,and it will facilitate the design of nanoc...The synthesis of nanocrystals(NCs)with defined morphology and surface structure provides an effective way to investigate the structure-activity relationship of nanocatalytsts,and it will facilitate the design of nanocatalysts with excellent catalytic performance.In this paper,we developed a facile method to synthesize PdH0.43 NCs with the shape of cube,octahedron and rhombic dodecahedron(RD),whose surface facets are{100},{111}and{110},respectively.The asprepared PdH0.43 NCs are highly stable and exhibit enhanced catalytic activity and extremely low overpotential towards electro-oxidation of formic acid compared with the commercial Pd black and three types of Pd NCs.The specific activity of the cubic PdH0.43 NCs is more than five times that of the commercial Pd black and two times that of the cubic Pd NCs.Among the three types of PdH0.43 NCs with different surface structure,the activity order is followed by PdH0.43{100}>PdH0.43{111}>PdH0.43{110}.展开更多
The catalytic properties of noble metal nanocrystals can be tuned via engineering their structures. Nanocrystals with fractal structures are fascinating catalysts regarding their large surface area-to-volume ratios, l...The catalytic properties of noble metal nanocrystals can be tuned via engineering their structures. Nanocrystals with fractal structures are fascinating catalysts regarding their large surface area-to-volume ratios, large numbers of edges and corners, which can be tuned simultaneously by their hierarchical ordering. However, it is still a great challenge to control the hierarchical ordering of noble metal fractal nanocrystals and their formation mechanism is not fully understood. Herein, we report a facile solvothermal method for the direct preparation of a unique single-crystal Rh-hyperbranched structure, which consists of hierarchically ultrathin nanoplates with threefold symmetry, large surface area and high density of low-coordinated edge/corner sites.Importantly, the hierarchical ordering can be readily tuned by changing the composition of solvent. In addition, we found the as-prepared single-crystal hyperbranched Rh nanoplates possessed great structure stability, and exhibited better catalytic performance towards both ethanol electrooxidation and hydrogenation of styrene than the commercial Rh black, which can be attributed to the large surface area and high-dentisty of edge/corner sites.展开更多
基金supported by the National Key Research and Development Program of China (2020YFB1505802)the National Natural Science Foundation of China (21931009 and 21721001)+2 种基金the Fundamental Research Funds for the Central Universities (20720210016 and 20720210104)the China Postdoctoral Science Foundation (2020M671939)Additional support was provided by Feringa Nobel Prize Scientist Joint Research Center。
基金supported by the National Natural Science Foundation of China (21771153, 21721001, and 21773190)the Natural Science Foundation of Fujian Province (2018J01015)
文摘The synthesis of nanocrystals(NCs)with defined morphology and surface structure provides an effective way to investigate the structure-activity relationship of nanocatalytsts,and it will facilitate the design of nanocatalysts with excellent catalytic performance.In this paper,we developed a facile method to synthesize PdH0.43 NCs with the shape of cube,octahedron and rhombic dodecahedron(RD),whose surface facets are{100},{111}and{110},respectively.The asprepared PdH0.43 NCs are highly stable and exhibit enhanced catalytic activity and extremely low overpotential towards electro-oxidation of formic acid compared with the commercial Pd black and three types of Pd NCs.The specific activity of the cubic PdH0.43 NCs is more than five times that of the commercial Pd black and two times that of the cubic Pd NCs.Among the three types of PdH0.43 NCs with different surface structure,the activity order is followed by PdH0.43{100}>PdH0.43{111}>PdH0.43{110}.
基金supported by the National Basic Research Program of China (2015CB932301)the National Natural Science Foundation of China (21333008, 21671163, 21603178 and J1310024)China Postdoctoral Science Foundation (2016M602066 and 2017T100468)
文摘The catalytic properties of noble metal nanocrystals can be tuned via engineering their structures. Nanocrystals with fractal structures are fascinating catalysts regarding their large surface area-to-volume ratios, large numbers of edges and corners, which can be tuned simultaneously by their hierarchical ordering. However, it is still a great challenge to control the hierarchical ordering of noble metal fractal nanocrystals and their formation mechanism is not fully understood. Herein, we report a facile solvothermal method for the direct preparation of a unique single-crystal Rh-hyperbranched structure, which consists of hierarchically ultrathin nanoplates with threefold symmetry, large surface area and high density of low-coordinated edge/corner sites.Importantly, the hierarchical ordering can be readily tuned by changing the composition of solvent. In addition, we found the as-prepared single-crystal hyperbranched Rh nanoplates possessed great structure stability, and exhibited better catalytic performance towards both ethanol electrooxidation and hydrogenation of styrene than the commercial Rh black, which can be attributed to the large surface area and high-dentisty of edge/corner sites.
