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High Performance of Supported Cu-based Catalysts Modulated via Phosphamide Coordination in Acetylene Hydrochlorination
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-01-02 , DOI: 10.1016/j.apcata.2020.117408
Yubing Hu , Yan Wang , Yulian Wang , Wei Li , Jinli Zhang , You Han

In order to develop a cut-price, high-efficiency non-mercuric catalyst for acetylene hydrochlorination reaction, several kinds of supported Cu-based catalysts containing phosphoramide ligands have been synthesized by wet impregnation method. The outstanding catalytic activity was obtained over 15%Cu10%HMPA/SAC catalyst with acetylene conversion of 87.25% in the test conditions of T =180 °C, GHSV(C2H2) =180 h-1 and V(HCl): V(C2H2) = 1.2. The catalyst with optimal HMPA ligand also exhibited splendid stability in 100 h lifetime test. The analysis for XRD, TEM, TGA, ICP, H2-TPR and XPS indicated that HMPA ligand can improve Cu species dispersion, restrain coke deposition, suppress loss of loading Cu, and stabilize valence state of active Cu species. Due to electron transfer mechanism, steady coordination structure between Cu and HMPA led to favorable properties of Cu-based catalyst, which was further proved by FT-IR, Raman spectra, O 1s XPS spectra integrated with DFT calculations.



中文翻译:

乙炔盐酸盐中磷酰胺配位调控的负载型铜基催化剂的高性能

为了开发用于乙炔盐酸盐化反应的廉价,高效的非汞催化剂,已经通过湿浸渍法合成了几种包含磷酰胺配体的负载型Cu基催化剂。在T = 180°C,GHSV(C 2 H 2)= 180 h -1V(HCl)的测试条件下,在15%Cu10%HMPA / SAC催化剂上乙炔转化率为87.25%的情况下获得了出色的催化活性:V(C 2 H 2)= 1.2。具有最佳HMPA配体的催化剂在100小时寿命测试中也表现出出色的稳定性。XRD,TEM,TGA,ICP,H 2的分析-TPR和XPS表明HMPA配体可改善Cu物种的分散性,抑制焦炭沉积,抑制负载Cu的损失并稳定活性Cu物种的化合价态。由于电子转移机理,Cu与HMPA之间稳定的配位结构导致了铜基催化剂的良好性能,并通过FT-IR,拉曼光谱,O 1s XPS光谱以及DFT计算得到了进一步的证明。

更新日期:2020-01-02
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