In catalysis,tuning the structural composition of the metal alloy is known as an efficient way to optimize the catalytic activity.This work presents the synthesis of compositional segregated six-armed PtCu nanostars v...In catalysis,tuning the structural composition of the metal alloy is known as an efficient way to optimize the catalytic activity.This work presents the synthesis of compositional segregated six-armed PtCu nanostars via a facile solvothermal method and their distinct composition-structure-dependent performances in electrooxidation processes.The alloy is shown to have a unique six arms with a Cu-rich dodecahedral core,mainly composed of {110} facets and exhibit superior catalytic activity toward alcohols electrooxidation compared to the hollow counterpart where Cu was selectively etched.Density functional theory (DFT) calculations suggest that the formation of hydroxyl intermediate (OH^*) is crucial to detoxify CO poisoning during the electrooxidation processes.The addition of Cu is found to effectively adjust the d band location of the alloy catalyst and thus enhance the formation of ^*OH intermediate from water splitting,which decreases the coverage of ^*CO intermediate.Our work demonstrates that the unique compositional anisotropy in alloy catalyst may boost their applications in electrocatalysis and provides a methodology for the design of this type catalyst.展开更多
The activity and stability of Cu nanostructures strongly depend on their sizes,morphology and structures.Here we report the preparation of two-dimensional(2 D)Cu@Cu-BTC core-shell nanosheets(NSs).The thickness of the ...The activity and stability of Cu nanostructures strongly depend on their sizes,morphology and structures.Here we report the preparation of two-dimensional(2 D)Cu@Cu-BTC core-shell nanosheets(NSs).The thickness of the Cu NSs could be tuned to sub-10 nm through a mild etching process,in which the Cu-BTC in situ grow along with the oxidation on the surface of the Cu NSs.This unique strategy can also be extended to synthesize one-dimensional(1 D)Cu@Cu-BTC nanowires(NWs).Furthermore,the obtained Cu@Cu-BTC NSs could be applied as an effective material to the memory device with the write-onceread-many times(WORM)behavior and the high ION/I(OFF)ratio(>2.7×103).展开更多
基金the support from National Natural Science Foundation of China (Nos.21571001,21372006,21631001,and U1532141)the Ministry of Education, the Education Department of Anhui Province211 Project of Anhui University.Y G.W gratefully acknowledges the financial support from Southern University of Science and Technolgoy (SUSTech). The calculations were performed by using the Taiyi high-performance supercomputer cluster located at SUSTech.
文摘In catalysis,tuning the structural composition of the metal alloy is known as an efficient way to optimize the catalytic activity.This work presents the synthesis of compositional segregated six-armed PtCu nanostars via a facile solvothermal method and their distinct composition-structure-dependent performances in electrooxidation processes.The alloy is shown to have a unique six arms with a Cu-rich dodecahedral core,mainly composed of {110} facets and exhibit superior catalytic activity toward alcohols electrooxidation compared to the hollow counterpart where Cu was selectively etched.Density functional theory (DFT) calculations suggest that the formation of hydroxyl intermediate (OH^*) is crucial to detoxify CO poisoning during the electrooxidation processes.The addition of Cu is found to effectively adjust the d band location of the alloy catalyst and thus enhance the formation of ^*OH intermediate from water splitting,which decreases the coverage of ^*CO intermediate.Our work demonstrates that the unique compositional anisotropy in alloy catalyst may boost their applications in electrocatalysis and provides a methodology for the design of this type catalyst.
基金supported by the National Key R&D Program of China(No.2017YFA0700104)National Natural Science Foundation of China(Nos.21571169,21871238)+2 种基金Fundamental Research Funds for the Central Universities(No.WK2060190081)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2018494)Young Elite Scientists Sponsorship Program by CAST(No.2016QNRC001)
文摘The activity and stability of Cu nanostructures strongly depend on their sizes,morphology and structures.Here we report the preparation of two-dimensional(2 D)Cu@Cu-BTC core-shell nanosheets(NSs).The thickness of the Cu NSs could be tuned to sub-10 nm through a mild etching process,in which the Cu-BTC in situ grow along with the oxidation on the surface of the Cu NSs.This unique strategy can also be extended to synthesize one-dimensional(1 D)Cu@Cu-BTC nanowires(NWs).Furthermore,the obtained Cu@Cu-BTC NSs could be applied as an effective material to the memory device with the write-onceread-many times(WORM)behavior and the high ION/I(OFF)ratio(>2.7×103).
