Robotic Lepidoptery: Structural Characterization of (mostly) Unexpected Palladium Complexes Obtained from High-Throughput Catalyst Screening
Robotic Lepidoptery: Structural Characterization of (mostly) Unexpected Palladium Complexes Obtained from High-Throughput Catalyst Screening
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DOI：
10.1021/om900240a
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发表时间：
2009-09-14
期刊：
影响因子：
2.8
通讯作者：
Virgil, Scott
中科院分区：
文献类型：
--
作者：
Bercaw, John E.;Day, Michael W.;Virgil, Scott
在高通量搜索双齿配体与Pd（II）羧酸酯的最佳组合以生成氧化催化剂的过程中，我们获得了许多结晶产物并对其进行了晶体学表征。而有些组合得到了预期的（L-L）Pd(OC(O)R)(2)结构（L-L =联吡啶，tmeda; R = CH3, CF3）。许多化合物通过C-H活化（L-L = sparteine）、P-C键裂解（L-L = 1,2-二苯基膦乙烷）和溶剂（丙酮）与配体（L-L = 1,4-二（2,6-二异丙基苯基）-1,4-重氮-1,3-丁二烯）之间的C-C键形成等反应生成了不寻常的低金属配合物。这些发现说明了基于假设均匀的原位催化剂自组装的筛选程序的潜在缺陷。
In the course of a high-throughput search for optimal combinations of bidentate ligands with Pd(II) carboxylates to generate oxidation catalysts, we obtained and crystallographically characterized a number of crystalline products. While some combinations afforded the anticipated (L-L)Pd(OC(O)R)(2) structures (L-L = bipyridine, tmeda; R = CH3, CF3). many gave unusual oligometallic complexes resulting from reactions such as C-H activation (L-L = sparteine), P-C bond cleavage (L-L = 1,2-bis(diphenylphosphino)ethane, and C-C bond formation between solvent (acetone) and ligand (L-L = 1,4-bis(2,6-diisopropylphenyl)-1,4-diaza-1,3-butadiene). These findings illustrate potential pitfalls of screening procedures based on assuming uniform, in situ catalyst self-assembly.