为了对多酸化合物合成过程的反应机理研究提供更多的基础信息,同时扩充同多酸盐的结构指纹图谱。以合成多钼酸盐化合物的两种常见反应物TBA_(2)[Mo_(6)O_(19)]与TBA_(4)[α-Mo_(8)O_(26)]为研究对象,以Na_(2)MoO_(4)为基础原料合成两种...为了对多酸化合物合成过程的反应机理研究提供更多的基础信息,同时扩充同多酸盐的结构指纹图谱。以合成多钼酸盐化合物的两种常见反应物TBA_(2)[Mo_(6)O_(19)]与TBA_(4)[α-Mo_(8)O_(26)]为研究对象,以Na_(2)MoO_(4)为基础原料合成两种化合物,用红外光谱(IR)对其固体结构进行了表征,用电喷雾质谱法(Electrospray Ionization Mass Spectrometry,ESI-MS)对二者的溶液行为进行了研究。结果表明,TBA_(2)[Mo_(6)O_(19)]在溶液中的存在形式为裸多阴离子,TBA_(4)[α-Mo_(8)O_(26)]在溶液中主要以降解后形成的低核钼簇的形式存在,其中{Mo_(4)}含量最高。对两种化合物相互转化关系的研究表明,TBA_(4)[α-Mo_(8)O_(26)]溶液加酸可成功转化为TBA_(2)[Mo_(6)O_(19)],温度对该转化过程无明显影响。TBA_(2)[Mo_(6)O_(19)]溶液加碱未能成功实现其转化为TBA_(4)[α-Mo_(8)O_(26)]的逆反应过程。对两种多钼酸盐的ESI-MS、IR表征,得到了两种化合物的结构指纹图谱。对两种多钼酸盐转化的研究为多酸化合物之间的相互转化补充了一条可行方案,为多酸化合物合成过程的反应机理研究提供了更丰富的基础信息。展开更多
Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with ...Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.展开更多
文摘为了对多酸化合物合成过程的反应机理研究提供更多的基础信息,同时扩充同多酸盐的结构指纹图谱。以合成多钼酸盐化合物的两种常见反应物TBA_(2)[Mo_(6)O_(19)]与TBA_(4)[α-Mo_(8)O_(26)]为研究对象,以Na_(2)MoO_(4)为基础原料合成两种化合物,用红外光谱(IR)对其固体结构进行了表征,用电喷雾质谱法(Electrospray Ionization Mass Spectrometry,ESI-MS)对二者的溶液行为进行了研究。结果表明,TBA_(2)[Mo_(6)O_(19)]在溶液中的存在形式为裸多阴离子,TBA_(4)[α-Mo_(8)O_(26)]在溶液中主要以降解后形成的低核钼簇的形式存在,其中{Mo_(4)}含量最高。对两种化合物相互转化关系的研究表明,TBA_(4)[α-Mo_(8)O_(26)]溶液加酸可成功转化为TBA_(2)[Mo_(6)O_(19)],温度对该转化过程无明显影响。TBA_(2)[Mo_(6)O_(19)]溶液加碱未能成功实现其转化为TBA_(4)[α-Mo_(8)O_(26)]的逆反应过程。对两种多钼酸盐的ESI-MS、IR表征,得到了两种化合物的结构指纹图谱。对两种多钼酸盐转化的研究为多酸化合物之间的相互转化补充了一条可行方案,为多酸化合物合成过程的反应机理研究提供了更丰富的基础信息。
基金supported by National Natural Science Foundation of China(52208272,41706080 and 51702328)the Basic Scientific Fund for National Public Research Institutes of China(2020S02 and 2019Y03)+3 种基金the Basic Frontier Science Research Program of Chinese Academy of Sciences(ZDBS-LY-DQC025)the Young Elite Scientists Sponsorship Program by CAST(No.YESS20210201)the Strategic Leading Science&Technology Program of the Chinese Academy of Sciences(XDA13040403)the Key Research and Development Program of Shandong Province(Major Scientific and Technological Innovation Project)(2019JZZY020711).
文摘Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.
