From recovered metal waste to high-performance palladium catalysts,Green Chemistry

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From recovered metal waste to high-performance palladium catalysts
Green Chemistry ( IF 9.3 ) Pub Date : 2017-11-20 00:00:00 , DOI: 10.1039/c7gc02678a
Khairil A. Jantan _{1,

2,

3,

4,

5} , Chuek Yee Kwok _{1,

2,

3,

4} , Kuang Wen Chan _{1,

2,

3,

4} , Luciano Marchiò _{6,

7,

8,

9,

10} , Andrew J. P. White _{1,

2,

3,

4} , Paola Deplano _{10,

11,

12,

13} , Angela Serpe _{1,

2,

3,

4,

14} , James D. E. T. Wilton-Ely _{1,

2,

3,

4}

Affiliation

The catalytic activity of a series of neutral and cationic, homo- and heteroleptic, mono- and bimetallic palladium(II) compounds based on dithiocarbamate and dithiooxamide S,S-donor ligands is described. High activity was observed in the regio- and chemo-selective C–H functionalization of benzo[h]quinoline to 10-alkoxybenzo[h]quinoline and 8-methylquinoline to 8-(methoxymethyl)quinoline in the presence of the oxidant PhI(OAc)₂. The best performance was found for [Pd(Me₂dazdt)₂]I₆ (Me₂dazdt = N,N′-dimethyl-perhydrodiazepine-2,3-dithione), [PdI₂(Me₂dazdt)] and [Pd(Cy₂DTO)₂]I₈ (Cy₂DTO = N,N′-dicyclohexyl-dithiooxamide) which are all obtained directly as products of sustainable Pd-metal leaching processes used to recover palladium from scrap metal. These compounds provided almost quantitative yields under milder conditions (50 °C, 1–3 mol% Pd loading) and much shorter reaction times (1–3 h) than reported previously. These results illustrate how the complexes obtained from the selective and sustainable recovery of Pd from automotive heterogeneous Three Way Catalysts (TWC) can be employed directly in homogeneous catalysis, avoiding further metal recovery steps and valorising the metal complex itself in a ‘circular economy’ model.

中文翻译：

从回收的金属废料到高性能的钯催化剂

描述了基于二硫代氨基甲酸酯和二硫代草酰胺S，S-给体配体的一系列中性和阳离子，均配和杂配，单金属和双金属钯（II）化合物的催化活性。在苯并[的区域选择性和化学选择性的C-H官能化，观察到高活性ħ ]喹啉〜10 alkoxybenzo [ ħ ]喹啉和8-甲基喹啉以8-（甲氧基甲基）在氧化剂是Phl的存在喹啉（OAC ）₂。发现[Pd（Me ₂ dazdt）₂ ] I ₆（Me ₂ dazdt = N，N'-二甲基-过氢二氮杂-2,3-二硫酮），[PdI ₂（Me₂ dazdt）]和[Pd（Cy₂ DTO）₂ ] I₈（Cy₂ DTO = N， N'-（二环己基-二硫代草酰胺），都是作为可持续Pd-金属浸出过程的产品直接获得的，该浸出过程用于从废金属中回收钯。这些化合物在较温和的条件（50°C，1-3 mol％Pd负载）下提供了几乎定量的产率，并且反应时间（1-3 h）比以前报道的要短得多。这些结果说明了从汽车多相三效催化剂（TWC）中选择性和可持续地回收Pd所获得的络合物如何直接用于均相催化中，从而避免了进一步的金属回收步骤，并在“循环经济”模型中使金属络合物本身处于增值状态。

更新日期：2017-11-22

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