Mg-Al水滑石负载纳米钯催化剂的超声原位还原制备及其催化十二氢-N-乙基咔唑释氢  

Ultrasonic In-situ Reduction Preparation of Mg-Al Hydrotalcite Supported Nano-palladium Catalyst and Its Catalytic Dehydrogenation of Dodecahydro-N-ethylcarbazole

作　　者：韩玉水 张琳昱 白雪峰[1] HAN Yushui;ZHANG Linyu;BAI Xuefeng(Institute of Petrochemistry,Heilongjiang Academy of Sciences,Harbin 150040,China)

机构地区：[1]黑龙江省科学院石油化学研究院,黑龙江哈尔滨150040

出　　处：《化学与粘合》2024年第4期323-327,349,共6页Chemistry and Adhesion

基　　金：黑龙江省科学院科研基金项目(编号:STZY2022SH01)。

摘　　要：在超声的空化作用下,镁铝水滑石(LDHs)的表面羟基解离成具有强还原性的氢自由基,解离出的氢自由基能够把吸附于LDHs表面的Pd2+进一步原位还原为Pd,从而成功制备出Pd NPs负载的LDHs催化剂(Pd/LDHs)。采用X-ray diffraction(XRD),Transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),和N2物理吸附等手段对Pd/LDHs催化剂进行表征,结果表明Pd纳米粒子(Pd NPs)均匀分散在LDHs表面,平均粒径为1.8 nm。在180℃下,Pd/LDHs催化十二氢-N-乙基咔唑(12H-NEC)的脱氢反应实验结果表明,反应6 h时12H-NEC脱氢效率为93.6%,TOF值可达2.88 g H_(2)/g Pd·min。经过4次循环,Pd/LDHs依然能保持其稳定性。By the action of cavitation effect of ultrasound,the hydroxyl groups on the surface of magnesium-aluminum hydrotalcites(LDHs)dissociate into hydrogen radicals with strong reducing properties,which further reduces Pd2+adsorbed on the surface of LDHs to Pd in situ,and the LDHs-loaded nano-palladium catalysts(Pd/LDHs)are successfully prepared.The Pd/LDHs catalysts are thoroughly investigated by means of XRD,TEM,XPS and N2 physisorption.The results show that the Pd nanoparticles(PdNPs)evenly distribute on the LDHs surface with an average diameter of 1.8 nm.It is shown from the results of dehydrogenation reaction of dodecahydro-N-ethylcarbazole(12H-NEC)over Pd/LDHs at 180℃ that the dehydrogenation efficiency of 12H-NEC in 6 h is 93.6%,and the TOF value reaches up to 2.88 gH_(2)/gPd·min.After four cycles,the Pd/LDHs still maintain their stability.

关 键 词：镁铝水滑石 十二氢-N-乙基咔唑脱氢 纳米钯催化剂 超声原位还原 

分 类 号：TQ426.8[化学工程] O643.38[理学—物理化学]