| Urease can catalyze the hydrolysis of urea into carbon dioxide and ammonia.It is a key nickel-containing oligomerase involved in the nitrogen cycle.Urease is widely found in various bacteria,fungi,and plants.It can provide the nitrogen source needed by the organism through the action of urea,and participate in the process of transferring nitrogen.Because of the special properties and wide applications of urease,it has attracted considerable attention from researchers.The derivatives obtained after the coordination of hydrazide derivatives possess strong biological activity and have attracted people's attention.In this thesis,four functional groups of salicylhydrazide derivatives were synthesized by introducing functional groups2-furanoyl,benzoyl and o-carboxybenzoyl to modify the terminal N of salicylhydrazide derivatives,and then the ligand Coordinate with metal nickel ions,obtain the corresponding nickel metal complex through self-assembly reaction,and analyze its crystal structure.Finally,using(2-hydroxypropyl)-(p-nitrophenyl)phosphate(HPNPP)to study the hydrolysis activity of nickel complexes.The main research work of this paper is as follows:(1)Preparation of 2-furancarboxylic acid chloride by reacting 2-furancarboxylic acid with dichlorosulfoxide,and then reacted with 5-chlorosalicylic hydrazide to synthesize the ligand N-(2-furanformyl)-5-chlorosalicylic hydrazide,and IR,1HNMR,13CNMR and elements Analysis etc.performed structural characterization.The corresponding nickel metal complex was obtained by reacting the synthesized ligand with Ni2+ions through self-assembly.The crystal structure of the complex was analyzed by X-Ray single crystal diffraction.The results show that the nickel metal complex is a trinuclear nickel cluster with the structural formula[Ni3(C12H6Cl N2O4)2(C5H5N)2(C3H7NO)2]·2CH3OH.The crystal system is monoclinic crystal,space group P2(1)/n,Cell parameter:a=15.581(3)?,b=9.5517(19)?,c=16.123(3)?,?=90 o,?=103.344(4)o,?=90 o,Z=2,Calculated density=1.565 mg/m3,V=2334.7(8)A3,R1=0.0578,w R2=0.1197,GOF=1.121.Taking(2-hydroxypropyl)-(p-nitrophenyl)phosphate(HPNPP)as the hydrolysis substrate,it was found that it has a relatively good catalytic ability for the hydrolysis of HPNPP under alkaline pH conditions.(2)Preparation of 2-furancarboxylic acid chloride by reacting2-furancarboxylic acid with dichlorosulfoxide,and then reacted with5-bromosalicylhydrazide to synthesize the ligand N-(2-furanformyl)-5-bromosalicylhydrazide,and IR,1HNMR,13CNMR and Elemental analysis was performed to characterize the structure.The synthesized ligand was reacted with Ni2+ions by self-assembly to obtain the corresponding nickel metal complex,and the crystal structure of the complex was analyzed by X-Ray single crystal diffractometer.The results show that the nickel metal complex is a trinuclear nickel cluster with the structural formula[Ni3(C12H6Br N2O4)2(C5H5N)2(C3H7NO)2]·2CH3OH.The crystal system is monoclinic crystal,space group P2(1)/n,Cell parameter:a=15.6139(16)?,b=9.5546(10)?,c=16.3312(16)?,?=90 o,?=104.311(2)o,?=90 o,Z=2,Calculated density=1.672 mg/m3,V=2360.8(4)A3,R1=0.0530,w R2=0.1030,GOF=1.006.Taking(2-hydroxypropyl)-(p-nitrophenyl)phosphate(HPNPP)as the hydrolysis substrate,it was found that it has a relatively good catalytic ability for the hydrolysis of HPNPP under alkaline pH conditions.(3)Preparation of benzoyl chloride by reacting benzoic acid with dichlorosulfoxide,and then reacted with salicyl hydrazide to synthesize the ligand N-benzoyl salicyl hydrazide,and IR,1HNMR,13CNMR and Elemental analysis was performed to characterize the structure.The synthesized ligand was reacted with Ni2+ions by self-assembly to obtain the corresponding nickel metal complex,and the crystal structure of the complex was analyzed by X-Ray single crystal diffractometer.The results show that the nickel metal complex is a trinuclear nickel clusterwiththestructuralformula[Ni3(C14H9N2O3)2(C5H5N)4][Ni3(C14H9N2O3)2(C5H5N)4]·2CH3OH.The crystal system is monoclinic crystal,space group P2(1)/n,Cell parameter:a=15.9549(18)?,b=14.5648(17)?,c=19.503(2)?,?=90 o,?=95.280(2)o,?=90 o,Z=2,Calculated density=1.518mg/m3,V=4512.8(9)A3,R1=0.0644,w R2=0.1999,GOF=1.059.Taking(2-hydroxypropyl)-(p-nitrophenyl)phosphate(HPNPP)as the hydrolysis substrate,it was found that it has a relatively good catalytic ability for the hydrolysis of HPNPP under alkaline pH conditions.(4)Ligand 2-(N-salicyloylformyl)benzoic acid was synthesized by the reaction of phthalic anhydride and salicylhydrazide,and IR,1HNMR,13CNMR and Elemental analysis was performed to characterize the structure.The synthesized ligand was reacted with Ni2+ions by self-assembly to obtain the corresponding nickel metal complex,and the crystal structure of the complex was analyzed by X-Ray single crystal diffractometer.The results show that the nickel metal complex is a trinuclear nickel cluster with a structure formula[Ni3(C16H11N2O5)2(C5H5N)4].The crystal system is orthorhombic crystal,space group Aba2,Cell parameters:a=20.3351(19)?,b=19.6905(16)?,c=12.4770(16)?,?=90 o,?=90 o,?=90 o,Z=4,Calculated density=1.483 mg/m3,V=4995.9(9)A3,R1=0.0687,w R2=0.1600,GOF=1.183.Taking(2-hydroxypropyl)-(p-nitrophenyl)phosphate(HPNPP)as the hydrolysis substrate,it was found that it has a relatively good catalytic ability for the hydrolysis of HPNPP under alkaline pH conditions. |
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