Synthesis of the novel layered amorphous and crystalline zirconium phosphate–phosphonates Zr(HPO₄)[O₃PCH₂N(CH₂CH₂)₂O]·nH₂O, Zr(HPO₄)[O₃PCH₂

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• 作者：Xuebing ; Ma ; Xiangkai ; Fu
• 关键词：Zirconium [N-(phosphonomethyl)morpholine-phosphate] ; Zirconium [N-(phosphonomethyl)iminodiacetic acid-phosphate] ; Zirconium [N ; N-di(phosphonomethyl) acetic acid] ; Palladium ; Hydrogenation
• 刊名：Journal of Molecular Catalysis A: Chemical
• 出版年：2004
• 出版时间：February 2, 2004
• 年：2004
• 卷：208
• 期：1-2
• 页码：129-133
• 全文大小：104 K

文摘

The layered amorphous and crystalline samples of zirconium [N-(phosphonomethyl)morpholine-phosphate] Zr(HPO₄)[O₃PCH₂N(CH₂CH₂)₂O]·nH₂O (1a, 2a), zirconium [N-(phosphonomethyl)iminodiacetic acid-phosphate] Zr(HPO₄)[O₃PCH₂N(CH₂CO₂H)₂]·nH₂O (1b, 2b) and zirconium [N,N-di(phosphonomethyl) acetic acid] Zr[(O₃PCH₂)₂NCH₂CO₂H]·nH₂O (1c, 2c) were synthesized for the first time with zirconium oxychloride, sodium dihydrogen phosphate and H₂O₃PCH₂N(CH₂CH₂)₂O, H₂O₃PCH₂N(CH₂CO₂H)₂ or (H₂O₃PCH₂)₂NCH₂CO₂H in the absence and presence of hydrofluoric acid. The samples were comparatively characterized by XRD, IR, TG and elemental analysis. XRD data showed that the crystalline samples 2a, 2b and 2c are highly crystalline with interlayer spacings of 1.606, 1.538 and 1.239nm, respectively. The amorphous and crystalline samples lost nearly the weight calculated for their organic component over the same broad temperature range of 172–664, 184–680 and 176–668°C, respectively. XPS data indicated that the coordination bonds formed between nitrogen and palladium in the palladium complexes. Their palladium complexes possessed good activities for the hydrogenation of the carbon–carbon double bond. The catalytic activities of the palladium complexes of amorphous 1a, 1b and 1c is 1.5–3.1 times as high as that of the palladium complexes of crystalline 2a, 2b and 2c.