摘要
Based on the density functional theory(DFT) calculations,we showed that the interactions between different valence anions(PO_(4)^(3-),CH_(3)PO_(4)^(2-),(CH_(3))_(2)PO_(4)^(-)) and graphene significantly increased as the valence of anion increased from negative monovalence to negative trivalence.The adsorption energy of(CH_(3))_(2)PO_(4)^(-)on the electron-rich graphene flake(C84H24)is-8.3 kcal/mol.The adsorption energy of CH_(3)PO_(4)^(2-) on the electron-rich graphene flake(C_(84)H_(24)) is-48.0 kcal/mol,which is about six times that of(CH_(3))_(2)PO_(4) adsorption on electron-rich graphene flake(C_(84)H_(24)) and is even much larger than that of CO_(3)^(2-) adsorption on electron-deficient aromatic ring C_(6)F_(6)(-28.4 kcal/mol).The adsorption energy of PO_(4)^(3-)on the electron-rich graphene flake(C_(84)H_(24)) is-159.2 kcal/mol,which is about 20 times that of(CH_(3))_(2)PO_(4) adsorption on the graphene flake(C_(84)H_(24)).The super-strong adsorption energy is mainly attributed to the orbital interactions between multivalent anions and graphene.This work provides new insights for understanding the interaction between multivalent anions and π-electron-rich carbon-based nanomaterials and is helpful for the design of graphene-based DNA biosensor.
作者
Xing Liu
Guosheng Shi
刘星;石国升(Shanghai Applied Radiation Institute,State Key Laboratory Advanced Special Steel,Shanghai University,Shanghai 200444,China;Division of Interfacial Water and Key Laboratory of Interfacial Physics and Technology,Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201800,China)
基金
Project supported by the National Natural Science Foundation of China for Outstanding Young Scholars(Grant No.11722548)
the China Postdoctoral Science Foundation(Grant No.2019M651462)
the National Natural Science Foundation of China(Grant No.U1932123)
the Innovative Research Team of High-Level Local Universities in Shanghai
the Open Project of State Key Laboratory of Advanced Special Steel,Shanghai Key Laboratory of Advanced Ferrometallurgy and the Science and Technology Commission of Shanghai Municipality(Gant No.19DZ2270200)
the Deepcomp7000 and Sc Grid of Supercomputing Center,Computer Network Information Center of the Chinese Academy of Sciences,the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund(second phase)
the Shanghai Supercomputer Center of China,the High Performance Computing Platform of Shanghai University。
