Anisotropic 2D Cu(2-x) Se Nanocrystals from Dodecaneselenol and Their Conversion to CdSe and CuInSe(2) Nanoparticles.
Anisotropic 2D Cu(2-x) Se Nanocrystals from Dodecaneselenol and Their Conversion to CdSe and CuInSe(2) Nanoparticles.
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DOI：
10.1021/acs.chemmater.8b01143
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发表时间：
2018-06-12
期刊：
影响因子：
--
通讯作者：
de Mello Donega C
中科院分区：
文献类型：
--
作者：
Berends AC;van der Stam W;Akkerman QA;Meeldijk JD;van der Lit J;de Mello Donega C
以未开发的无膦硒前驱体1-十二烷硒醇(DDSe)为原料，合成了尺寸和形状可控的胶体各向异性Cu2-xSe纳米晶(NCS)。这种前驱体与铜(I)形成层状络合物，使NC形态从0D多面体裁剪为高度各向异性的2D形状。随后，Cu2-xSe纳米碳管被用作后合成阳离子交换反应的模板，通过这些反应，它们成功地转化为CdSe和CuInSe量子点、纳米小片和超薄纳米片。在阳离子交换反应中，模板六方纳米片的形状保持不变，尽管阴离子亚晶格发生了实质性的重组，导致母体Cu2-xSe NCS的四方锰矿晶体结构转变为六方纤锌矿CdSe和CuInSe2，并伴随着纳米片的厚度和横向尺寸的变化。产物NCS的晶型转变和重构归因于母相和产物晶相的晶胞尺寸和内部熟化过程的结合。这项工作为合理设计形状可控的胶体各向异性Cu2-xSe纳米碳管提供了新的工具，除了具有良好的光电性能外，还构成了一类新的阳离子交换模板，用于合成纤锌矿、CdSe、CuInSe等金属硒化合物的形状可控纳米碳管，这是直接合成方法无法获得的。此外，由于DDSe可能能够与其他几种金属形成层状络合物，因此本文提供的见解可能也适用于其他金属硒化合物的形状控制NCS的直接合成。
We present the synthesis of colloidal anisotropic Cu2–xSe nanocrystals (NCs) with excellent size and shape control, using the unexplored phosphine-free selenium precursor 1-dodecaneselenol (DDSe). This precursor forms lamellar complexes with Cu(I) that enable tailoring the NC morphology from 0D polyhedral to highly anisotropic 2D shapes. The Cu2–xSe NCs are subsequently used as templates in postsynthetic cation exchange reactions, through which they are successfully converted to CdSe and CuInSe2 quantum dots, nanoplatelets, and ultrathin nanosheets. The shape of the template hexagonal nanoplatelets is preserved during the cation exchange reaction, despite a substantial reorganization of the anionic sublattice, which leads to conversion of the tetragonal umangite crystal structure of the parent Cu2–xSe NCs into hexagonal wurtzite CdSe and CuInSe2, accompanied by a change of both the thickness and the lateral dimensions of the nanoplatelets. The crystallographic transformation and reconstruction of the product NCs are attributed to a combination of the unit cell dimensionalities of the parent and product crystal phases and an internal ripening process. This work provides novel tools for the rational design of shape-controlled colloidal anisotropic Cu2–xSe NCs, which, besides their promising optoelectronic properties, also constitute a new family of cation exchange templates for the synthesis of shape-controlled NCs of wurtzite CdSe, CuInSe2, and other metal selenides that cannot be attained through direct synthesis approaches. Moreover, the insights provided here are likely applicable also to the direct synthesis of shape-controlled NCs of other metal selenides, since DDSe may be able to form lamellar complexes with several other metals.
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DOI：
10.1021/acs.chemmater.7b04925
发表时间：
2017-12-26
期刊：
Chemistry of materials : a publication of the American Chemical Society
影响因子：
--
作者：
Berends AC;Meeldijk JD;van Huis MA;de Mello Donega C
通讯作者：
de Mello Donega C
影响因子：
17.1
作者：
Cunningham, Patrick D.;Souza, Joao B., Jr.;Talapin, Dmitri V.
通讯作者：
Talapin, Dmitri V.
影响因子：
10.8
作者：
Groeneveld, Esther;van Berkum, Susanne;Donega, Celso de Mello
通讯作者：
Donega, Celso de Mello
影响因子：
5.7
作者：
Berends, Anne C.;Rabouw, Freddy T.;Donega, Celso de Mello
通讯作者：
Donega, Celso de Mello
影响因子：
17.1
作者：
Groeneveld, Esther;Witteman, Leon;Donega, Celso de Mello
通讯作者：
Donega, Celso de Mello