季铵盐阳离子的Waugh型化合物的合成与表征

doi:10.3969/j.issn.1000-1565.2022.03.007

摘要/Abstract

摘要： 以(NH₄)₆［MnMo₉O₃₂］为前体原料,采用常规的水溶液法与四甲(乙)氯化铵反应制备了2种含有混合阳离子的Waugh型钼酸盐(NH₄)₄［N(CH₃)₄］₂［MnMo₉O₃₂］·9H₂O(化合物1)和(NH₄)₄［N(CH₂CH₃)₄］₂［MnMo₉O₃₂］·7H₂O(化合物2),用元素分析、红外光谱、热重分析对其进行了表征,并对化合物1进行了单晶结构测定,化合物1属于单斜晶系,C2/c空间群,a=2.379(11)nm,b=1.186(5)nm,c=1.600(7)nm,β=102.308(4)°,V=4.413(3)nm³,Z=4,Dc=2.460 g/cm³,R₁=0.041 8,wR₂=0.117 5(I>2σ),GOF=1.058.对化合物的形成规律探索发现:季铵盐与(NH₄)₆MnMo₉O₃₂的物质的量之比为3∶1,易形成单晶.对化合物1和2光催化降解亚甲基蓝模拟废水进行了探索,光催化90 min和180 min时脱色率分别达到95.96%和85.64%,表明化合物1和2对亚甲基蓝染料废水均具有良好的光催化活性.

关键词: Waugh结构, 季铵盐, 晶体结构, 表征, 光催化

Abstract: The new Waugh compounds(NH₄)₄［N(CH₃)₄］₂［MnMo₉O₃₂］·9H₂O(1)and(NH₄)₄［N(CH₂CH₃)₄］₂［MnMo₉O₃₂］·7H₂O(2)containing quaternary ammonium cations were obtained by reacting of(NH₄)₆MnMo₉O₃₂ and tetramethyl ammonium chloride or tetraethyl ammonium chloride in aqueous solution, and properties were characterized by elemental analysis, IR and TG. The structure of the compound 1 was determined by single crystal X-ray diffraction. The chemical formula of the compound 1 belongs to monoclinic system with space group C2/c, a=2.379(11)nm,b=1.186(5)nm,c=1.600(7)nm,β=102.308(4)°,V=4.413(3)nm³, Z=4, Dc=2.460 g/cm³, R₁=0.041 8, wR₂=0.117 5(I>2σ), GOF=1.058. Exploring the formation rules of the compounds 1 and 2 revealed that the optimal ratio of the amount of［N(CH₃)₄］Cl or［N(C₂H₅)₄］Cl to(NH₄)₆MnMo₉O₃₂·9H₂O is equal to 3∶1, and that single crystals of title compounds were easily formed. Methylene blue simulated dye wastewater for photocatalytic degradation by compounds 1 and 2 was explored, the decolorization of methylene blue solutions at 90 min and 180 min reached 95.96% and 85.64%, respectively. The photocatalytic results show- DOI:10.3969/j.issn.1000-1565.2022.03.007季铵盐阳离子的Waugh型化合物的合成与表征刘雪梅,郭珂欣,李金环,李慧敏,胡若晖( 西安石油大学化学化工学院,陕西西安 710065)摘要:以(NH₄)₆［MnMo₉O₃₂］为前体原料,采用常规的水溶液法与四甲(乙)氯化铵反应制备了2种含有混合阳离子的Waugh型钼酸盐(NH₄)₄［N(CH₃)₄］₂［MnMo₉O₃₂］·9H₂O(化合物1)和(NH₄)₄［N(CH₂CH₃)₄］₂［MnMo₉O₃₂］·7H₂O(化合物2),用元素分析、红外光谱、热重分析对其进行了表征,并对化合物1进行了单晶结构测定,化合物1属于单斜晶系,C2/c空间群,a=2.379(11)nm,b=1.186(5)nm,c=1.600(7)nm,β=102.308(4)°,V=4.413(3)nm³,Z=4,Dc=2.460 g/cm³,R₁=0.041 8,wR₂=0.117 5(I>2σ),GOF=1.058.对化合物的形成规律探索发现:季铵盐与(NH₄)₆MnMo₉O₃₂的物质的量之比为3∶1,易形成单晶.对化合物1和2光催化降解亚甲基蓝模拟废水进行了探索,光催化90 min和180 min时脱色率分别达到95.96%和85.64%,表明化合物1和2对亚甲基蓝染料废水均具有良好的光催化活性.关键词:Waugh结构;季铵盐;晶体结构;表征;光催化中图分类号:O611.2 文献标志码:A 文章编号:1000-1565(2022)03-0265-08Synthesis and characterization of Waugh-type compounds containing quaternary ammonium cationsLIU Xuemei, GUO Kexin, LI Jinhuan, LI Huimin, HU Ruohui( College of Chemistry and Chemical Engineering, Xian Shiyou University, Xian 710065, China )Abstract: The new Waugh compounds(NH₄)₄［N(CH₃)₄］₂［MnMo₉O₃₂］·9H₂O(1)and(NH₄)₄［N(CH₂CH₃)₄］₂［MnMo₉O₃₂］·7H₂O(2)containing quaternary ammonium cations were obtained by reacting of(NH₄)₆MnMo₉O₃₂ and tetramethyl ammonium chloride or tetraethyl ammonium chloride in aqueous solution, and properties were characterized by elemental analysis, IR and TG. The structure of the compound 1 was determined by single crystal X-ray diffraction. The chemical formula of the compound 1 belongs to monoclinic system with space group C2/c, a=2.379(11)nm,b=1.186(5)nm,c=1.600(7)nm,β=102.308(4)°,V=4.413(3)nm³, Z=4, Dc=2.460 g/cm³, R₁=0.041 8, wR₂=0.117 5(I>2σ), GOF=1.058. Exploring the formation rules of the compounds 1 and 2 revealed that the optimal ratio of the amount of［N(CH₃)₄］Cl or［N(C₂H₅)₄］Cl to(NH₄)₆MnMo₉O₃₂·9H₂O is equal to 3∶1, and that single crystals of title compounds were easily formed. Methylene blue simulated dye wastewater for photocatalytic degradation by compounds 1 and 2 was explored, the decolorization of methylene blue solutions at 90 min and 180 min reached 95.96% and 85.64%, respectively. The photocatalytic results show- 收稿日期:2021-09-21 基金项目:陕西省自然科学基础研究计划项目(2016JQ2037);国家级大学生创新创业训练计划项目(S202010705018);西安石油大学研究生创新与实践能力培养项目(YCS20211018) 第一作者:刘雪梅(1976—),女,陕西西安人,西安石油大学副教授,博士.主要从事杂多化合物方向的研究.E-mail: lxm2503@163.com第3期刘雪梅等:季铵盐阳离子的Waugh型化合物的合成与表征that both compounds 1 and 2 have good photocatalytic activity against methylene blue simulated dye wastewater.

Key words: Waugh structure, quaternary ammonium, crystal structure, characterization, photocatalysis

中图分类号:

O611.2

刘雪梅,郭珂欣,李金环,李慧敏,胡若晖. 季铵盐阳离子的Waugh型化合物的合成与表征[J]. 河北大学学报(自然科学版), 2022, 42(3): 265-272.

LIU Xuemei, GUO Kexin, LI Jinhuan, LI Huimin, HU Ruohui. Synthesis and characterization of Waugh-type compounds containing quaternary ammonium cations[J]. Journal of Hebei University(Natural Science Edition), 2022, 42(3): 265-272.

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