The geometry, electronic structure, polarizability and hyperpolarizability of dye sensitizer 3,4-bis[1-（carboxymethyl）-3-indolyl]-1H-pyrrole-2,5-dione （BIMCOOH） were studied using density functional theory （DFT）...The geometry, electronic structure, polarizability and hyperpolarizability of dye sensitizer 3,4-bis[1-（carboxymethyl）-3-indolyl]-1H-pyrrole-2,5-dione （BIMCOOH） were studied using density functional theory （DFT） with hybrid functional B3LYP, and the electronic absorption spectra were investigated using semi-empirical quantum chemical method ZINDO-1 and time-dependent DFT （TDDFT）. The results of natural bond orbital suggest that the natural charges of the dione, indole, and acetic groups are about 0.15e, -0.29e, and 0.44e, respectively. The calculated isotropic polarizability, polarizability anisotropy invariant and hyperpolarizability are 305.4, 188.3, and 1155.4 a.u., respectively. The electronic absorption spectral features in visible and near-UV region were assigned to the π→π^＊ transition due to the qualitative agreement between the experiment and the TDDFT calculations, and the transitions of the excited states 9-11 related to photoinduced intramolecular charge transfer processes. The analysis of electronic structure and UV-Vis absorption indicates that the indole groups primarily contributed sensitization of photo-to-currency conversion processes, and the interracial electron transfer between semiconductor TiO2 electrode and dye sensitizer BIMCOOH are electron injection processes from excited states of the dyes to the semiconductor conduction band.展开更多
Metal nitride is one of the best anode materials of the energy storage device;however,the low stability of the pure metal nitride limits its wide applications.In this work,a new method of bioabsorbable fabrication was...Metal nitride is one of the best anode materials of the energy storage device;however,the low stability of the pure metal nitride limits its wide applications.In this work,a new method of bioabsorbable fabrication was developed for preparing molybdenum nitride that corporates into the porous carbon materials.The molybdenum ions in pollutions could be easily absorbed by Ligustrum quihoui,and the transportation,accumulation,and circulation of molybdenum ions in Ligustrum quihoui were studied.The obtained composite material of biochar and molybdenum nitride is employed as anode material of supercapacitors and batteries which exhibits good electrochemical performance,especially the rate and long lifespan aspects.Typically,it is found that the specific capacity is344 F·g^(-1)at current density of 0.5 A·g^(-1)in 2 mol·L^(-1)KOH,and the capacitance retention and coulomb efficiency are above 90%after 10,000 cycles.It should be noted that the novel approach combines fabricating anode materials with advanced nanostructure and suppressing the environmental problems with metal pollution at the same time.展开更多
基金This work was supported by the National Natural Science Foundation of China(No.11964016)the HongLiu First-class Disciplines Development Program of Lanzhou University of Technology.The authors were grateful to the National Supercomputing Center in Shenzhen.
基金ACKNOWLEDGMENTS This work was supported by the NationM NaturM Science Foundation of China （No. 10647006）, the Prominent Youth Foundation （No.Q200704） and the Scientific Developmental Foundation of Lanzhou University of Technology. Cai-rong Zhang would like to thank Professor Wan-zhen Liang （USTC）, and the Gansu Supercomputer Center is also appreciated.
文摘The geometry, electronic structure, polarizability and hyperpolarizability of dye sensitizer 3,4-bis[1-（carboxymethyl）-3-indolyl]-1H-pyrrole-2,5-dione （BIMCOOH） were studied using density functional theory （DFT） with hybrid functional B3LYP, and the electronic absorption spectra were investigated using semi-empirical quantum chemical method ZINDO-1 and time-dependent DFT （TDDFT）. The results of natural bond orbital suggest that the natural charges of the dione, indole, and acetic groups are about 0.15e, -0.29e, and 0.44e, respectively. The calculated isotropic polarizability, polarizability anisotropy invariant and hyperpolarizability are 305.4, 188.3, and 1155.4 a.u., respectively. The electronic absorption spectral features in visible and near-UV region were assigned to the π→π^＊ transition due to the qualitative agreement between the experiment and the TDDFT calculations, and the transitions of the excited states 9-11 related to photoinduced intramolecular charge transfer processes. The analysis of electronic structure and UV-Vis absorption indicates that the indole groups primarily contributed sensitization of photo-to-currency conversion processes, and the interracial electron transfer between semiconductor TiO2 electrode and dye sensitizer BIMCOOH are electron injection processes from excited states of the dyes to the semiconductor conduction band.
基金financially supported by the National Natural Science Foundation of China (Nos.51763014 and52073133)the Key Talent Project Foundation of Gansu Province+1 种基金Joint Fund between Shenyang National Laboratory for Materials Science and State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals (No.18LHPY002)the Program for Hongliu Distinguished Young Scholars in Lanzhou University of Technology。
文摘Metal nitride is one of the best anode materials of the energy storage device;however,the low stability of the pure metal nitride limits its wide applications.In this work,a new method of bioabsorbable fabrication was developed for preparing molybdenum nitride that corporates into the porous carbon materials.The molybdenum ions in pollutions could be easily absorbed by Ligustrum quihoui,and the transportation,accumulation,and circulation of molybdenum ions in Ligustrum quihoui were studied.The obtained composite material of biochar and molybdenum nitride is employed as anode material of supercapacitors and batteries which exhibits good electrochemical performance,especially the rate and long lifespan aspects.Typically,it is found that the specific capacity is344 F·g^(-1)at current density of 0.5 A·g^(-1)in 2 mol·L^(-1)KOH,and the capacitance retention and coulomb efficiency are above 90%after 10,000 cycles.It should be noted that the novel approach combines fabricating anode materials with advanced nanostructure and suppressing the environmental problems with metal pollution at the same time.
