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异双金属单源前驱体:二元金属间化合物合成的跳板。

Heterobimetallic Single-Source Precursors: A Springboard to the Synthesis of Binary Intermetallics.

作者信息

Daniels Carena L, Mendivelso-Perez Deyny L, Rosales Bryan A, You Di, Sahu Sumit, Jones J Stuart, Smith Emily A, Gabbaï François P, Vela Javier

机构信息

Department of Chemistry, Iowa State University, Ames, Iowa 50011, United States.

Ames Laboratory, Ames, Iowa 50011, United States.

出版信息

ACS Omega. 2019 Mar 12;4(3):5197-5203. doi: 10.1021/acsomega.9b00088. eCollection 2019 Mar 31.

Abstract

Intermetallics are atomically ordered crystalline compounds containing two or more main group and transition metals. In addition to their rich crystal chemistry, intermetallics display unique properties of interest for a variety of applications, including superconductivity, hydrogen storage, and catalysis. Because of the presence of metals with a wide range of reduction potentials, the controlled synthesis of intermetallics can be difficult. Recently, soft chemical syntheses such as the modified polyol and ship-in-a-bottle methods have helped advance the preparation of these materials. However, phase-segregated products and complex multistep syntheses remain common. Here, we demonstrate the use of heterobimetallic single-source precursors for the synthesis of 10-15 and 11-15 binary intermetallics. The coordination environment of the precursor, as well as the exact temperature used play a critical role in determining the crystalline intermetallic phase that is produced, highlighting the potential versatility of this approach in the synthesis of a variety of compounds. Furthermore, we show that a recently developed novel plasma-processing technique is successful in removing the surface graphitic carbon observed in some of the prepared compounds. This new single-source precursor approach is a powerful addition to the synthesis of atomically ordered intermetallic compounds and will help facilitate their further study and development for future applications.

摘要

金属间化合物是包含两种或更多主族金属和过渡金属的原子有序晶体化合物。除了丰富的晶体化学性质外,金属间化合物还展现出对多种应用具有吸引力的独特性质,包括超导性、储氢和催化作用。由于存在具有广泛还原电位的金属,金属间化合物的可控合成可能具有挑战性。近来,诸如改进的多元醇法和瓶中造船法等软化学合成方法有助于推进这些材料的制备。然而,相分离产物和复杂的多步合成仍然很常见。在此,我们展示了使用异双金属单源前驱体来合成10-15和11-15二元金属间化合物。前驱体的配位环境以及所使用的精确温度在决定生成的晶体金属间相方面起着关键作用,突出了这种方法在合成各种化合物方面的潜在通用性。此外,我们表明,一种最近开发的新型等离子体处理技术成功地去除了在一些制备的化合物中观察到的表面石墨碳。这种新的单源前驱体方法是对原子有序金属间化合物合成的有力补充,并将有助于促进其在未来应用中的进一步研究和开发。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c7af/6648806/ed201daf6549/ao-2019-00088e_0006.jpg

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