Complexation effect of copper(II) with HEDP supported by activated carbon and influence on acetylene hydration,New Journal of Chemistry

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Complexation effect of copper(II) with HEDP supported by activated carbon and influence on acetylene hydration
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2020-12-18 , DOI: 10.1039/d0nj04928j
Qiang Zhang _{1,

2,

3,

4,

5} , Xiaohong Liu _{1,

2,

3,

4,

5} , Jiannan Luo _{1,

2,

3,

4,

5} , Cunhua Ma _{1,

2,

3,

4,

5} , Caixia Xu _{1,

2,

3,

4,

5}

Affiliation

Heterogeneous catalysts based on Hg are found to be highly active for the acetylene hydration reaction with a very high yield of acetaldehyde, but severe toxicity limits its application. Herein, HEDP was selected as a polydentate phosphonate ligand to synthesize novel green Cu-based catalysts by a simple impregnation method. The prepared catalyst with the best ratio of Cu/ligand of 1 : 1 and 4 wt% Cu loading can achieve >82.9% selectivity of the aldehyde with 99% conversion of acetylene after 8 h compared to the ligand-free catalyst. The effect of the ligand and the active component on the catalytic performance was evaluated in detail by several characterization methods. XRD, TPR, and HRTEM coupled with EDS analysis revealed that the introduction of HEDP could enhance the dispersion of Cu species and decrease the particle sizes of Cu. XPS indicated strong interaction of the coordination compound formed by the coordination of Cu²⁺ with HEDP molecules, which effectively inhibited the reduction of Cu ions during the reaction process. TGA revealed that this complex could inhibit the coking deposition produced during the reaction. The novel perspective will provide the potential of using HEDP as a metal chelating agent to stabilize the active components and increase the dispersion for the heterogeneous catalyst.

中文翻译：

活性炭负载下铜（II）与HEDP的络合作用及其对乙炔水合的影响

发现基于Hg的多相催化剂对乙炔水合反应具有很高的活性，并且乙醛的收率很高，但是严重的毒性限制了其应用。在此，选择HEDP作为多齿膦酸酯配体，以通过简单的浸渍方法合成新颖的基于绿色Cu的催化剂。与不含配体的催化剂相比，具有最佳的Cu /配体比例为1：1和4 wt％的Cu负载量的制得的催化剂可在8小时后实现乙醛的> 82.9％的选择性和乙炔的99％的转化率。通过几种表征方法详细评估了配体和活性成分对催化性能的影响。XRD，TPR和HRTEM结合EDS分析表明，引入HEDP可以增强Cu种类的分散性并减小Cu的粒径。HEDP分子具有²⁺，可有效抑制反应过程中Cu离子的还原。TGA显示该络合物可以抑制反应期间产生的焦化沉积。该新颖的观点将提供使用HEDP作为金属螯合剂来稳定活性组分并增加非均相催化剂的分散性的潜力。

更新日期：2021-01-11

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