Complexes of As4S4 interacting with H+and OH by computational quantum chemistry
Objective To determine the possible arsenic species of realgar in acidic and alkaline media,by studying the complexes of As4S4 interacting with H+and OH-with computational quantum chemistry method.Methods Firstly,the Gaussian View software was used to design the possible complexes formed by interaction between As4S4 isomers with H+and OH-;subsequently,Gaussian 09 software was used to perform geometric optimization and thermodynamic calculations on the possible formation of[As4S4-H]+complexes at the HF/STO-3G,B3LYP/6-31G*and B3LYP/6-311+G*theory levels;for the possible formation of[As4S4-OH]-complexes,geometric optimization and thermodynamic calculations were conducted at the HF/STO-3G,B3LYP/6-31+G*,and B3LYP/6-311+G*theory levels.Then,natural bond orbital analysis was performed on[As4S4-H]+and[As4S4-OH]-complexes at the B3LYP/6-31G*and B3LYP/6-31+G*levels.Results Two isomers of As4S4 could both form complexes with H+and OH-ions at a 1∶1 ratio,and 21 complexes found were thermodynamically stable.The frontier orbital energy level and bond level analysis showed that the stability of[As4S4-H]+and[As4S4-OH]-complexes were relatively poor.Conclusion The complexes generated by realgar in acidic and alkaline media may exist as short-lived species,which may be the reactive intermediates in acidic and alkaline media.
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