Looking for breakthrough ideas for innovation challenges? Try Patsnap Eureka!

Quantum chemistry method capable of calculating gas-phase hydroxyl radical reaction rate constants of various perfluoroalkyl/polyfluoroalkyl compounds

A reaction rate constant, polyfluoroalkyl technology, applied in computational theoretical chemistry, chemical structure search, chemical process analysis/design, etc., can solve the problems of unknown quantum chemical methods, different quantum chemical methods, etc., and achieve low cost , Wide range of application, fast effect

Pending Publication Date: 2022-07-12
DALIAN UNIV OF TECH
View PDF0 Cites 0 Cited by
  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] Existing studies have focused on exploring the atmospheric transformation mechanism of PFASs, and calculated their k OH is only one step in the atmospheric transformation process, therefore, whether the quantum chemical method used is suitable for calculating the k of PFASs OH still in doubt
Secondly, the research goal is usually only for a single PFASs, and whether the quantum chemical method used is applicable to other types of PFASs is still unknown
Finally, the quantum chemical methods used in previous studies are different, and the choice of the method is only based on the calculation effect of this method on other compounds

Method used

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
View more

Image

Smart Image Click on the blue labels to locate them in the text.
Viewing Examples
Smart Image
  • Quantum chemistry method capable of calculating gas-phase hydroxyl radical reaction rate constants of various perfluoroalkyl/polyfluoroalkyl compounds
  • Quantum chemistry method capable of calculating gas-phase hydroxyl radical reaction rate constants of various perfluoroalkyl/polyfluoroalkyl compounds
  • Quantum chemistry method capable of calculating gas-phase hydroxyl radical reaction rate constants of various perfluoroalkyl/polyfluoroalkyl compounds

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0048] Select 15 known k OH The PFASs of the PFASs were firstly downloaded for their 3D configuration, and the CP2K software was used to perform BOMD simulation. The CP2K output file had typical representative configurations, and the M06-2X / cc-pVDZ method was used to optimize the structure and obtain its most stable configuration according to the energy. Using this method, the transition states of each channel for the reaction of ·OH with 15 PFASs were also searched.

[0049]

[0050] Refer to the structure and logk of PFASs OH (k OH :cm 3 molecule -1 ·s -1 )

[0051]

[0052] CF 3 CFH 2 (a), CF 3 CH 2 CF 3 (b), C 2 F 5 (CHF) 2 CF 3 (c) Reaction channel for reaction with OH

[0053]

[0054] CH 3 OC 2 F 5 (d), CF 3 OCF 2 H(e), CF 3 CHCl 2 (f) Reaction channel for reaction with OH

[0055]

[0056]

[0057] CF 2 =CH 2 (g), CF 3 OCF=CF 2 (h), CF 3 CF=CF 2 (i), 8:2FTO(j), 4:2FTA(k) reaction channel with OH

[0058]

[0059]

[0...

Embodiment 2

[0084] Given a PFASs: 1,1,1,2,3,3,3-heptafluoropropane, k OH is 1.622×10 -15 cm 3 molecule -1 ·s -1 . First download its 3D configuration, use CP2K software to perform BOMD simulation, and use the M06-2X / cc-pVDZ method to optimize the structure, calculate the energy, and obtain the 3D configuration of its most stable configuration. coordinate. Similarly, the M06-2X / cc-pVDZ method was used to find the transition states of each channel of the reaction between OH and 1,1,1,2,3,3,3-heptafluoropropane. The structure is optimized with the transition state and the thermodynamic parameters are extracted, and the single-point energy is obtained by the addition of M06-2X-D3 / jun-pVTZ:ωb97x-D / jul-pVTZ=0.5:0.5. The single point energy and thermodynamic parameters are added together, as the final thermodynamic parameter ΔG is 50.945kJ mol -1 ;E a is 14.754kJ mol -1 ; For: 1566.752cm -1 ; V is 0.000kJ mol -1 . and apply it to the TST method to calculate k TST , and multiply b...

Embodiment 3

[0086] Given a PFASs: 1,1,2,2,3-pentafluoropropane, k OH is 1.089×10 -14 cm 3 molecule -1 ·s -1 . First download its 3D configuration from PubChem, use CP2K software to perform BOMD simulation, and use the M06-2X / cc-pVDZ method to optimize the structure, calculate the energy, and obtain the most stable structure. 3D coordinates of the type. Similarly, the M06-2X / cc-pVDZ method was used to find the transition states of each channel in the reaction between OH and 1,1,2,2,3-pentafluoropropane. Structural optimization was carried out and thermodynamic parameters were extracted, and the single-point energy was obtained by the summation of M06-2X-D3 / jun-pVTZ:ωb97x-D / jul-pVTZ=0.5:0.5. The single point energy and thermodynamic parameters are added together as the final thermodynamic parameter ΔG for channel 1: 43.2kJ mol -1 , channel 2: 49.3 kJ mol -1 , channel 3: 48.1 kJ mol -1 ;Channel 1:E a 5.634kJ mol -1 , channel 2: E a is 13.126kJ mol -1 , channel 3: E a 9.720kJmo...

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
Login to View More

PUM

No PUM Login to View More

Abstract

The invention discloses a quantum chemistry method capable of calculating gas-phase hydroxyl radical reaction rate constants of various perfluoroalkyl / polyfluoroalkyl compounds. The gas phase kOH value of the PFASs can be directly obtained by utilizing the most stable configuration of the known PFASs and applying the constructed quantum chemical calculation method. The construction process of the quantum chemistry method comprises the following steps: collecting 15 PFASs stable configurations of known kOH, searching a reaction path of PFASs and. OH by using a density functional theory, carrying out subsequent structure optimization, calculating single-point energy by using different DFT methods, and calculating thermodynamic parameters and kOH. And performing linear fitting on results of different calculation methods and experimental values, and screening an optimal method. The quantum chemical calculation method developed by the invention can accurately and efficiently calculate the kOH of the unknown PFASs, provides a necessary tool for evaluating the atmospheric durability of the PFASs, and has very important significance.

Description

technical field [0001] The invention belongs to the field of atmospheric persistence screening for per / polyfluoroalkyl compounds (PFASs), and a method capable of calculating reaction rate constants (k) of various types of PFASs and gas phase ·OH OH ) of the quantum chemical method. Background technique [0002] Per / polyfluoroalkyl compounds (PFASs) are widely added to products due to their excellent surface activity, stability and other properties. Currently, more than 1,400 PFASs are used as chemicals in more than 200 fields. The specific structures are known. There are more than 8,000 PFASs. However, more and more studies have demonstrated that some commonly used PFASs have ultra-long persistence, bioaccumulation and toxicity. Among them, the environmental persistence assessment of PFASs is one of the core contents of PFASs risk management. Environmental persistence refers to the ability of chemicals to be difficult to degrade and transform in the environment and remain...

Claims

the structure of the environmentally friendly knitted fabric provided by the present invention; figure 2 Flow chart of the yarn wrapping machine for environmentally friendly knitted fabrics and storage devices; image 3 Is the parameter map of the yarn covering machine
Login to View More

Application Information

Patent Timeline
no application Login to View More
Patent Type & Authority Applications(China)
IPC IPC(8): G16C10/00G16C20/10G16C20/40
CPCG16C10/00G16C20/10G16C20/40
Inventor 丁保君姜琦陈景文
Owner DALIAN UNIV OF TECH
Who we serve
  • R&D Engineer
  • R&D Manager
  • IP Professional
Why Patsnap Eureka
  • Industry Leading Data Capabilities
  • Powerful AI technology
  • Patent DNA Extraction
Social media
Patsnap Eureka Blog
Learn More
PatSnap group products

Browse by: Latest US Patents, China's latest patents, Technical Efficacy Thesaurus, Application Domain, Technology Topic, Popular Technical Reports.

© 2024 PatSnap. All rights reserved.Legal|Privacy policy|Modern Slavery Act Transparency Statement|Sitemap|About US| Contact US: help@patsnap.com