Chemical doping is verified to be a promising strategy to regulate local electron distribution and further promote the poor intrinsic catalytic activity of graphdiyne.However,the current doping approach still faces pr...Chemical doping is verified to be a promising strategy to regulate local electron distribution and further promote the poor intrinsic catalytic activity of graphdiyne.However,the current doping approach still faces problems such as precise doping for creating active sites and the destruction of graphdiyne skeleton calling for high temperature.Here,we achieved charge redistribution on graphdiyne surface through molecule functionalization.A p-type molecule–F4 TCNQ(2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodime thane)was introduced and the site-defined functionalization was accomplished.Theoretical calculations showed that the charge transfer ability is improved and graphdiyne becomes positively charged.The oxygen reduction electrocatalysis was conducted as a proof of principle,where the electronic states of sp hybridized C active site was tuned toward favorable reaction intermediates’adsorption.Such work from both theoretical prediction and experimental validation,found that molecule functionalization is effective to promote the electrocatalytic oxygen reduction,which creates new possibilities for graphdiyne’s applications in different electrochemical reactions.展开更多
In the present article,coarse grained Dissipative Particle Dynamics simulation with implementation of electrostatic interactions is developed in constant pressure and surface tension ensemble to elucidate how the anti...In the present article,coarse grained Dissipative Particle Dynamics simulation with implementation of electrostatic interactions is developed in constant pressure and surface tension ensemble to elucidate how the antimicrobial peptidemolecules affect bilayer cellmembrane structure and kill bacteria.We find that peptideswith different chemical-physical properties exhibit differentmembrane obstructing mechanisms.Peptide molecules can destroy vital functions of the affected bacteria by translocating across their membranes via worm-holes,or by associating with membrane lipids to form hydrophilic cores trapped inside the hydrophobic domain of the membranes.In the latter model,the affected membranes are strongly buckled,in accord with very recent experimental observations[G.E.Fantner et al.,Nat.Nanotech.,5(2010),pp.280-285].展开更多
基金supported by the National Natural Science Foundation of China(21773016,21971244,51932001)the National Key R&D Program of China(2018YFA0703504)。
文摘Chemical doping is verified to be a promising strategy to regulate local electron distribution and further promote the poor intrinsic catalytic activity of graphdiyne.However,the current doping approach still faces problems such as precise doping for creating active sites and the destruction of graphdiyne skeleton calling for high temperature.Here,we achieved charge redistribution on graphdiyne surface through molecule functionalization.A p-type molecule–F4 TCNQ(2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodime thane)was introduced and the site-defined functionalization was accomplished.Theoretical calculations showed that the charge transfer ability is improved and graphdiyne becomes positively charged.The oxygen reduction electrocatalysis was conducted as a proof of principle,where the electronic states of sp hybridized C active site was tuned toward favorable reaction intermediates’adsorption.Such work from both theoretical prediction and experimental validation,found that molecule functionalization is effective to promote the electrocatalytic oxygen reduction,which creates new possibilities for graphdiyne’s applications in different electrochemical reactions.
基金This work is supported by National Science Foundation of China(Grant No.20873007).We are thankful to the referee for very useful comments.
文摘In the present article,coarse grained Dissipative Particle Dynamics simulation with implementation of electrostatic interactions is developed in constant pressure and surface tension ensemble to elucidate how the antimicrobial peptidemolecules affect bilayer cellmembrane structure and kill bacteria.We find that peptideswith different chemical-physical properties exhibit differentmembrane obstructing mechanisms.Peptide molecules can destroy vital functions of the affected bacteria by translocating across their membranes via worm-holes,or by associating with membrane lipids to form hydrophilic cores trapped inside the hydrophobic domain of the membranes.In the latter model,the affected membranes are strongly buckled,in accord with very recent experimental observations[G.E.Fantner et al.,Nat.Nanotech.,5(2010),pp.280-285].
