Guo Xueli, Tan Yiwei
State Key Laboratory of Materials-Oriented Chemical Engineering, School of Chemistry and Chemical Engineering, Nanjing Tech University, Nanjing 210009, China.
Phys Chem Chem Phys. 2015 Dec 21;17(47):31956-65. doi: 10.1039/c5cp05531h.
Branched Pd nanocrystals (NCs) with tunable architectures are synthesized in high yields (>95%) by simply adjusting the concentration of H2PdCl4 in the presence of fixed amounts of cetyltrimethylammonium bromide (CTAB), L-ascorbic acid (L-AA), and CuBr2(-) that is produced by reducing CuBr2 with L-AA. The as-synthesized branched Pd NCs have long, straight branches with thin diameters. At the same time, the growth process of the branched Pd NCs is monitored, which provides mechanistic insights for the branching growth of Pd NCs. It is identified that a high concentration of CTAB combined with an appropriate amount of CuBr2(-) species, acting as an in situ cooperatively organized template, is a decisive factor for the anisotropic growth of the branched Pd nanostructures during aqueous-phase reduction of the Pd precursor, using L-AA as a reducing agent. The electrocatalytic activities of the branched Pd NCs were tested. The branched Pd NCs are found to be an excellent electrocatalyst for the methanol oxidation reaction (MOR) largely due to the size and morphological effects of the branched structures.
通过在固定量的十六烷基三甲基溴化铵(CTAB)、L-抗坏血酸(L-AA)以及由L-AA还原CuBr₂产生的CuBr₂⁻存在下简单地调节H₂PdCl₄的浓度,可高产率(>95%)合成具有可调结构的分支状钯纳米晶体(NCs)。所合成的分支状钯NCs具有长的、直径较细的直分支。同时,对分支状钯NCs的生长过程进行了监测,这为钯NCs的分支生长提供了机理见解。已确定,高浓度的CTAB与适量的CuBr₂⁻物种相结合,作为一种原位协同组装模板,是在以L-AA作为还原剂对钯前驱体进行水相还原过程中,分支状钯纳米结构各向异性生长的决定性因素。测试了分支状钯NCs的电催化活性。发现分支状钯NCs是甲醇氧化反应(MOR)的优良电催化剂,这主要归因于分支结构的尺寸和形态效应。