Photon-induced dissociation pathways of thymine are investigated with vacuum ultraviolet photoionization mass spectrometry and theoretical calculations. The photoionization mass spectra of thymine at different photon ...Photon-induced dissociation pathways of thymine are investigated with vacuum ultraviolet photoionization mass spectrometry and theoretical calculations. The photoionization mass spectra of thymine at different photon energy are measured and presented. By selecting suitable photon energy, exclusively molecular ion m/z=126 is obtained. At photon energy of 12.0 eV, the major ionic fragments at m/z=98, 97, 84, 83, 70, and 55 are obtained, which are assigned to C4H6N2O＋, C4H5N2O＋, C3H4N2O＋ （or C4H6NO＋）, C4H5NO＋, C2NO2＋, and C3H5N＋, respectively. With help of theoretical calculations, the detailed dissociation pathways of thymine at low energy are well established.展开更多
Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only...Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only molecular ions are measured by virtue of nearthreshold photoionization. While increasing photon energy to 11.7 eV or more, four distinct fragment ions are obtained for tyramine and dopamine, respectively. Besides, the ionization energies of tyramine and dopamine are determined to be 7.984-0.05 and 7.674-0.05 eV by measuring the photoionization efficiency curves of corresponding molecular ions. With help of density function theory calculations, the detailed fragmentation pathways are established as well. These two molecular cations have similar aminoethyl group elimination pathways, CTHsO2＋ （m/z=124） and C7H8O＋ （m/z=108） are supposed to be generated by the McLafferty rearrangement via γ-hydrogen （7-H） shift inducing β-fission. And CH2NH2＋ is proposed to derive from the direct fission of C7-C8 bond. Besides, the McLafferty rearrangement and the C7-C8 bond fission are validated to be dominant dissociation pathways for tyramine and dopamine cations.展开更多
Ceramic electrolytes are important in ceramic-liquid hybrid electrolytes(CLHEs),which can effectively solve the interfacial issues between the electrolyte and electrodes in solid-state batteries and provide a highly e...Ceramic electrolytes are important in ceramic-liquid hybrid electrolytes(CLHEs),which can effectively solve the interfacial issues between the electrolyte and electrodes in solid-state batteries and provide a highly efficient Li-ion transfer for solid–liquid Li metal batteries.Understanding the ionic transport mechanisms in CLHEs and the corresponding role of ceramic electrolytes is crucial for a rational design strategy.Herein,the Li-ion transfer in the ceramic electrolytes of CLHEs was confirmed by tracking the 6Li and 7Li substitution behavior through solid-state nuclear magnetic resonance spectroscopy.The ceramic and liquid electrolytes simultaneously participate in Li-ion transport to achieve highly efficient Li-ion transfer in CLHEs.A spontaneous Li-ion exchange was also observed between ceramic and liquid electrolytes,which serves as a bridge that connects the ceramic and liquid electrolytes,thereby greatly strengthening the continuity of Li-ion pathways in CLHEs and improving the kinetics of Li-ion transfer.The importance of an abundant solid–liquid interface for CLHEs was further verified by the enhanced electrochemical performance in LiFePO4/Li and LiNi0.8Co0.1Mn0.1O2/Li batteries from the generated interface.This work provides a clear understanding of the Li-ion transport pathway in CLHEs that serves as a basis to build a universal Li-ion transport model of CLHEs.展开更多
基金This work was supported by the Chinese Academy of Sciences and the National Natural Science Foundation of China （No.10805047）. Authors appreciate the kind help from Dr. Yang Pan in experiments.
文摘Photon-induced dissociation pathways of thymine are investigated with vacuum ultraviolet photoionization mass spectrometry and theoretical calculations. The photoionization mass spectra of thymine at different photon energy are measured and presented. By selecting suitable photon energy, exclusively molecular ion m/z=126 is obtained. At photon energy of 12.0 eV, the major ionic fragments at m/z=98, 97, 84, 83, 70, and 55 are obtained, which are assigned to C4H6N2O＋, C4H5N2O＋, C3H4N2O＋ （or C4H6NO＋）, C4H5NO＋, C2NO2＋, and C3H5N＋, respectively. With help of theoretical calculations, the detailed dissociation pathways of thymine at low energy are well established.
基金Authors thank Dr. Yang Pan for useful discussions This work was supported by the National Natural Science Foundation of China （No.10805047）.
文摘Photon induced dissociation investigations of neutral tyramine and dopamine are carried out with synchrotron vacuum uRraviolet photoionization mass spectrometry and theoretical calculations. At low photon energy, only molecular ions are measured by virtue of nearthreshold photoionization. While increasing photon energy to 11.7 eV or more, four distinct fragment ions are obtained for tyramine and dopamine, respectively. Besides, the ionization energies of tyramine and dopamine are determined to be 7.984-0.05 and 7.674-0.05 eV by measuring the photoionization efficiency curves of corresponding molecular ions. With help of density function theory calculations, the detailed fragmentation pathways are established as well. These two molecular cations have similar aminoethyl group elimination pathways, CTHsO2＋ （m/z=124） and C7H8O＋ （m/z=108） are supposed to be generated by the McLafferty rearrangement via γ-hydrogen （7-H） shift inducing β-fission. And CH2NH2＋ is proposed to derive from the direct fission of C7-C8 bond. Besides, the McLafferty rearrangement and the C7-C8 bond fission are validated to be dominant dissociation pathways for tyramine and dopamine cations.
基金supported by the National Natural Science Foundation of China(U2001220)Key-Area Research and Development Program of Guangdong Province(2020B090919001)+2 种基金Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center(XMHT20200203006)Shenzhen Technical Plan Project(RCJC20200714114436091,JCYJ20180508152210821JCYJ20180508152135822)。
文摘Ceramic electrolytes are important in ceramic-liquid hybrid electrolytes(CLHEs),which can effectively solve the interfacial issues between the electrolyte and electrodes in solid-state batteries and provide a highly efficient Li-ion transfer for solid–liquid Li metal batteries.Understanding the ionic transport mechanisms in CLHEs and the corresponding role of ceramic electrolytes is crucial for a rational design strategy.Herein,the Li-ion transfer in the ceramic electrolytes of CLHEs was confirmed by tracking the 6Li and 7Li substitution behavior through solid-state nuclear magnetic resonance spectroscopy.The ceramic and liquid electrolytes simultaneously participate in Li-ion transport to achieve highly efficient Li-ion transfer in CLHEs.A spontaneous Li-ion exchange was also observed between ceramic and liquid electrolytes,which serves as a bridge that connects the ceramic and liquid electrolytes,thereby greatly strengthening the continuity of Li-ion pathways in CLHEs and improving the kinetics of Li-ion transfer.The importance of an abundant solid–liquid interface for CLHEs was further verified by the enhanced electrochemical performance in LiFePO4/Li and LiNi0.8Co0.1Mn0.1O2/Li batteries from the generated interface.This work provides a clear understanding of the Li-ion transport pathway in CLHEs that serves as a basis to build a universal Li-ion transport model of CLHEs.
