摘要
尽管扭曲的晶体在自然界中无处不在,但由于理想纳米晶体的形成需要极其严格的条件,因此人工制造具有定制形态和扭曲结构的纳米晶体具有极大的挑战性.本研究通过改变生长温度实现了动力学诱导的扭曲Pd_(20)Sb_(7)菱面体纳米晶体的定向形貌演变.详细的表征和实验表明,缓慢的动力学导致Pd_(20)Sb_(7)从正菱面体到扭曲菱面体的形态演变,而在此演变过程中纳米晶体的结构保持相同,均暴露6个{211}晶面.此外,不同形貌的Pd_(20)Sb_(7)纳米晶体表现出相似的甲酸氧化反应活性(基于表面钯原子的归一化活性),进一步验证了该动力学诱导形貌演变过程不改变Pd_(20)Sb_(7)纳米晶体的结构.本研究拓展了具有特定形貌的钯基纳米晶体的精确控制合成,并有望推动其在化学、材料科学、催化等相关领域的实际应用.
Although distorted crystals are ubiquitous in nature,the artificial creation of distorted nanoscale crystals with tailored morphology and structure are greatly challenging,since the formation of ideal nanocrystals requires extremely rigorous condition.We herein demonstrate a kineticsinduced orientational morphological evolution of distorted Pd_(20)Sb_(7) rhombohedral nanocrystals(RNCs)by altering the temperature for growth.Detailed characterizations and experiments show that the retarded kinetics leads to the morphological evolution from regular rhombohedron to distorted rhombohedron,while the crystalline structure is kept identical by exposing six{211}facets.Moreover,the morphological evolution of distorted Pd_(20)Sb_(7) RNCs is further validated by the similar normalized activity towards formic oxidation reaction based on the surface Pd atoms.This work advances the precisely controlled synthesis of Pd-based nanocrystals with tailored morphologies,which may attract great interests in various fields including chemistry,materials science,catalysis and beyond.
作者
王梦君
吕林喆
蒋巧荣
李广
洪麒明
王明敏
徐勇
黄小青
Mengjun Wang;Linzhe Lü;Qiaorong Jiang;Guang Li;Qiming Hong;Mingmin Wang;Yong Xu;Xiaoqing Huang(State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China;Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices,Collaborative Innovation Center of Advanced Energy Materials,School of Materials and Energy,Guangdong University of Technology,Guangzhou 510006,China;Testing and Analysis Center,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China)
基金
supported by the National Key R&D Program of China(2020YFB1505802)
the Ministry of Science and Technology(2017YFA0208200)
the National Natural Science Foundation of China(22025108,U21A20327,and 22121001)
Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(2021B1515020081)
the start-up support from Xiamen University and Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices(20195010002)。