以丙酸和硝基苯为混合溶剂,苯甲醛、对羟基苯甲醛和吡咯为原料合成了5-对羟基苯基-10,15,20-三苯基卟啉(HPTPP).然后以HPTPP和环氧氯丙烷为原料,在NaOH催化条件下合成了5-[4-(2,3-环氧丙氧基)苯基]-10,15,20-三苯基卟啉(EPPTPP).利用傅...以丙酸和硝基苯为混合溶剂,苯甲醛、对羟基苯甲醛和吡咯为原料合成了5-对羟基苯基-10,15,20-三苯基卟啉(HPTPP).然后以HPTPP和环氧氯丙烷为原料,在NaOH催化条件下合成了5-[4-(2,3-环氧丙氧基)苯基]-10,15,20-三苯基卟啉(EPPTPP).利用傅里叶变换红外光谱仪(FTIR)、核磁共振波谱仪(NMR)、紫外可见分光光度计(UV-Vis)和荧光分光光度计分别对HPTPP和EPPTPP的化学结构和光学性质进行了表征与测试.结果表明:FTIR谱图中,1 347cm-1和917cm-1处为EPPTPP卟啉环中C N键伸缩振动吸收峰和环氧化物环的(C—OC键)不对称伸缩振动吸收峰.EPPTPP的1 H NMR谱图中,在δ2.94～4.56内5个位移峰峰面积比为1∶1∶1∶1∶1,与EPPTPP中环氧基团的不同氢原子数比完全一致.UV-Vis谱图中,具有与卟啉结构相符合的吸收峰,表明成功合成了EPPTPP.通过荧光光谱分析了HPTPP和EPPTPP的荧光性质,并计算得到了二者的荧光量子产率分别为0.140和0.143.展开更多
The development of novel and effective methods for the activation of methane is fascinating,which offers a promising potential for the sustainable development of chemical industry and the mitigation of greenhouse effe...The development of novel and effective methods for the activation of methane is fascinating,which offers a promising potential for the sustainable development of chemical industry and the mitigation of greenhouse effect.Here we successfully synthesize two-dimensional(2D)Zr/5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin(TCPP)ultrathin nanobelts(UNBs)as a high efficiency catalyst for methane(CH_(4))oxidation to carbon monoxide(CO).The Co-UNBs show well photo-coupled electrocatalytic performances for CH4 activation(CO production rates are 0.171 and 8.416 mmol·g−1·h−1 under dark/visible light,respectively).Density functional theory(DFT)calculations were performed to illustrate the mechanism of photoelectrocatalytic process and the high efficiency oxidation of CH4 to CO.Based on the ultrathin structure and highly efficient catalytic properties,this work provides a prospecting avenue for the design and synthesis of methane oxidation catalyst.展开更多
文摘以丙酸和硝基苯为混合溶剂,苯甲醛、对羟基苯甲醛和吡咯为原料合成了5-对羟基苯基-10,15,20-三苯基卟啉(HPTPP).然后以HPTPP和环氧氯丙烷为原料,在NaOH催化条件下合成了5-[4-(2,3-环氧丙氧基)苯基]-10,15,20-三苯基卟啉(EPPTPP).利用傅里叶变换红外光谱仪(FTIR)、核磁共振波谱仪(NMR)、紫外可见分光光度计(UV-Vis)和荧光分光光度计分别对HPTPP和EPPTPP的化学结构和光学性质进行了表征与测试.结果表明:FTIR谱图中,1 347cm-1和917cm-1处为EPPTPP卟啉环中C N键伸缩振动吸收峰和环氧化物环的(C—OC键)不对称伸缩振动吸收峰.EPPTPP的1 H NMR谱图中,在δ2.94～4.56内5个位移峰峰面积比为1∶1∶1∶1∶1,与EPPTPP中环氧基团的不同氢原子数比完全一致.UV-Vis谱图中,具有与卟啉结构相符合的吸收峰,表明成功合成了EPPTPP.通过荧光光谱分析了HPTPP和EPPTPP的荧光性质,并计算得到了二者的荧光量子产率分别为0.140和0.143.
基金supported by the National Key R&D Program of China(Nos.2017YFA0700101 and 2016YFA0202801)the National Natural Science Foundation of China(Nos.22035004 and 22205061)the XPLORER PRIZE and the China Postdoctoral Science Foundation(No.2019M660608)。
文摘The development of novel and effective methods for the activation of methane is fascinating,which offers a promising potential for the sustainable development of chemical industry and the mitigation of greenhouse effect.Here we successfully synthesize two-dimensional(2D)Zr/5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin(TCPP)ultrathin nanobelts(UNBs)as a high efficiency catalyst for methane(CH_(4))oxidation to carbon monoxide(CO).The Co-UNBs show well photo-coupled electrocatalytic performances for CH4 activation(CO production rates are 0.171 and 8.416 mmol·g−1·h−1 under dark/visible light,respectively).Density functional theory(DFT)calculations were performed to illustrate the mechanism of photoelectrocatalytic process and the high efficiency oxidation of CH4 to CO.Based on the ultrathin structure and highly efficient catalytic properties,this work provides a prospecting avenue for the design and synthesis of methane oxidation catalyst.
