钯三角双锥单孪晶的合成

doi:10.7503/cjcu20170337

高等学校化学学报 ›› 2017, Vol. 38 ›› Issue (12): 2149.doi: 10.7503/cjcu20170337

• 研究论文: 无机化学 • 上一篇下一篇

钯三角双锥单孪晶的合成

孙长勇, 林亮标, 解晓伟()

广东工业大学轻工化工学院清洁化学技术重点实验室, 广州 510006

收稿日期:2017-05-31 出版日期:2017-12-10 发布日期:2017-11-21
作者简介:联系人简介: 解晓伟, 女, 博士, 教授, 主要从事纳米材料和多相催化研究. E-mail: xwxie@gdut.edu.cn
基金资助:
国家自然科学基金(批准号: 21103182, 21273049)、广东省自然科学基金(批准号: S2013050014127)和广东省教育厅项目(批准号: CGZHZD1104, 2013CXZDA016)资助

Synthesis of Palladium Right Bipyramids with a Singly Twinned Structure^†

SUN Changyong, LIN Liangbiao, XIE Xiaowei^*()

Key Laboratory of Clean Chemical Technology, School of Chemical Engineering and Light Industry,Guangdong University of Technology, Guangzhou 510006, China

Received:2017-05-31 Online:2017-12-10 Published:2017-11-21
Contact: XIE Xiaowei E-mail:xwxie@gdut.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China(Nos.21103182, 21273049), the Natural Science Foundation of Guangdong Province, China(No.S2013050014127) and the Education Department Funding of Guangdong Province, China(Nos CGZHZD1104, 2013CXZDA016)

摘要/Abstract

摘要：

采用液相还原法, 以Na₂PdCl₄为钯源, PVP为还原剂和分散剂, 碘离子作为晶面选择吸附剂和配位剂, 硝酸根离子作为氧化蚀刻剂, 水为溶剂, 在n(Na₂PdCl₄)∶n(PVP)∶n(KI)∶n(NaNO₃)=1∶35∶10∶9和pH=11条件下, 合成了形貌规整的纯度大于99%的钯三角双锥单孪晶. 碘离子在合成体系中主要通过改变钯前驱体还原速率来影响钯晶种的生长转化和产物的形貌, 对氧化蚀刻作用的影响在较高pH值下并不明显. 钾离子和钠离子比例的变化显著影响了产物的形貌组成, 此阳离子效应可归因于反应体系在钠离子存在时较钾离子存在时表现出更快的钯前驱体还原速率.

关键词: 三角双锥, 钯单孪晶, 氧化蚀刻, 还原速率, 阳离子效应

Abstract:

Through solution phase reduction route, palladium right bipyramid nanocrystals with a singly twinned structure were synthesized with Na₂PdCl₄ as a precursor, PVP as a stabilizer and reductant, I^- as a plane-selective capping agent and coordination reagent, and N $O 3 -$ as an etching agent in a hydrophilic system. When n(Na₂PdCl₄)∶n(PVP)∶n(KI)∶n(NaNO₃)=1∶35∶10∶9 and pH=11, well-defined palladium right bipyramid nanocrystals with purity higher than 99% could be achieved. I^- in the present reaction system affected the growth and transformation of crystal seed and the morphology of final product by changing reduction rate of Pd precursor, whereas the effect of I^- on oxidative etching was not obvious at high pH value. The ratio of K⁺/Na⁺ considerably influenced the morphology of product, showing a cation effect, which was possibly attributed to higher reduction rate in the presence of Na⁺ than that in the presence of K⁺.

Key words: Right triangular bipyramid, Singly twinned Pd nanocrystal, Oxidative etching, Reduction rate, Cation effect

中图分类号:

O614
O641

TrendMD:

孙长勇, 林亮标, 解晓伟. 钯三角双锥单孪晶的合成. 高等学校化学学报, 2017, 38(12): 2149.

SUN Changyong, LIN Liangbiao, XIE Xiaowei. Synthesis of Palladium Right Bipyramids with a Singly Twinned Structure^†. Chem. J. Chinese Universities, 2017, 38(12): 2149.

图/表 8

Fig.1 TEM images of as-synthesized sample at low and high magnificationsn(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶20∶8, initial pH=11. The inset of (C) shows 3D models of individual Pd right bipyramids in three common orientations that correspond to the different projected shapes, yellow denotes {111} twin plane inside the crystal, all exposed facets are {100} without coloring.

Fig.2 HRTEM images of Pd right bipyramid(A) and 5-fold twinned wire(B) with 3D models showing e-beam orientations and the corresponding FT pictures(insets)

Fig.3 TEM images of the as-synthesized samples at initial pH of 9(A, B) and 7(C, D)n(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶20∶8.

Fig.4 TEM images of the as-synthesized samples under different NaNO3 dosagesn(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶20∶X. (A), (B) X=0; (C), (D) X=4; (E), (F) X=10.

Fig.5 TEM images of the as-synthesized samples under different KI dosagesn(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶X∶8. (A), (B) X=10; (C), (D) X=30.

Fig.6 TEM images of the as-synthesized sample under optimal conditionsn(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶10∶9.

Fig.7 TEM images of the as-synthesized sample using NaI instead of KIn(Na2PdCl4)∶n(PVP)∶n(NaI)∶n(NaNO3)=1∶35∶20∶0.

Fig.8 UV-Vis spectra at different reaction stages(A) n(Na2PdCl4)∶n(PVP)∶n(KI)∶n(NaNO3)=1∶35∶20∶0; (B) n(Na2PdCl4)∶n(PVP)∶n(NaI)∶n(NaNO3)=1∶35∶20∶0. The inset depicts the time dependence of the absorbance around 343 nm, which is directly proportional to the concentration of the [PdI4]2- species.

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钯三角双锥单孪晶的合成

Synthesis of Palladium Right Bipyramids with a Singly Twinned Structure^†

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钯三角双锥单孪晶的合成

Synthesis of Palladium Right Bipyramids with a Singly Twinned Structure†

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Synthesis of Palladium Right Bipyramids with a Singly Twinned Structure^†