Plasma Discharge Reactor Flowing Liquid Gas C-H Bond Activation

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Solution Overview

Problem

The challenge in chemical synthesis is to control plasma-induced radical reactions and promote reaction selectivity, particularly in the oxidation of C—H bonds in alkanes at low temperature and pressure, where over-oxidation and selectivity issues are prevalent, and there is a need for efficient conversion of methane to methanol using plasma reactors.

Innovation Solution

A pulsed plasma reactor with a flowing liquid water film and carrier gas is used to convert alkanes into oxygenated products such as alcohols, ketones, and aldehydes by hydroxyl radical attack, while also generating hydrogen peroxide, employing a reactor design with a cylindrical body and conductive capillaries to propagate plasma along the liquid-gas interface.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Productivity

If plasma discharge is used to activate C-H bonds in alkanes, then chemical conversion is achieved, but selectivity is poor and over-oxidation occurs

Engineering Contradiction:
Improvechemical conversionVSAvoidreaction selectivity
Core Design Contradiction:
ProductivityVSManufacturing precision

Solution Approach 1:

The plasma reactor operates in periodic cycles alternating between plasma discharge phase and dark phase. During the plasma phase, radicals are generated to activate C-H bonds. During the dark phase, radical reactions are suppressed, allowing selective oxidation products to form without further degradation. This periodic operation prevents over-oxidation while maintaining conversion efficiency.

Inventive Principle:
Principle #19Periodic action

Solution Approach 2:

A liquid stream (water or organic liquid) is introduced as an intermediary medium between the plasma phase and the substrate. The liquid absorbs excess radicals during the plasma phase and releases them during the dark phase, mediating the oxidation process to improve selectivity. The liquid phase also serves as a heat sink to control reaction temperature and prevent runaway oxidation.

Inventive Principle:
Principle #24Intermediary (Mediator)

2Productivity

If high plasma power is applied to increase conversion rate, then productivity improves, but energy efficiency decreases

Engineering Contradiction:
Improveconversion rateVSAvoidenergy efficiency
Core Design Contradiction:
ProductivityVSLoss of energy

Solution Approach 1:

By operating in periodic cycles rather than continuous high-power mode, the reactor achieves high conversion during plasma phases while allowing energy recovery and thermal management during dark phases. This reduces overall energy consumption compared to continuous high-power operation while maintaining productivity.

Inventive Principle:
Principle #19Periodic action

Solution Approach 2:

The reactor optimizes plasma power parameters by using moderate power levels in periodic cycles rather than high continuous power. The duty cycle, pulse width, and inter-pulse intervals are adjusted to achieve maximum conversion efficiency at minimum energy input, improving energy efficiency while maintaining productivity.

Inventive Principle:
Principle #35Parameter changes

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

This approach effectively activates C—H bonds, producing valuable functionalized organic products with enhanced selectivity and energy efficiency, as demonstrated by GC-MS and NMR spectroscopy, where 3-hexanol, 2-hexanol, 3-hexanone, and hexanal are formed, and hydrogen peroxide is produced, indicating successful transformation of hydrocarbons into higher value compounds.

Implementation Method 1

a plasma discharge is propagated along a liquid-gas interface

Methodology Applied
Scientific EffectPlasma discharge: Plasma

Implementation Method 2

convert alkanes into oxygenated products such as alcohols, ketones, and aldehydes by hydroxyl radical attack

Methodology Applied
Scientific EffectHydroxyl radical attack: Oxidation

Implementation Method 3

dissociating the liquid water in the plasma discharge to form a plurality of dissociation products; producing hydrogen peroxide from the plurality of dissociation products

Methodology Applied
Scientific EffectDissociation: Photodissociation

Data Source

PatentUS10610850B2Plasma discharge reactor with flowing liquid and gas
Publication Date: 2020.04.07 FLORIDA STATE UNIV RES FOUND INC
  • US10610850B2 patent drawing
  • US10610850B2 patent drawing
  • US10610850B2 patent drawing

AI summary

The activation of the C—H bond using low temperature plasma with an inlet liquid stream such that value added products are formed effectively. An organic liquid (e.g., hexane which is immiscible with liquid water) is injected into a flowing gas (argon) stream followed by mixing with a liquid water stream. Thereafter, the mixture contacts a plasma region formed by a pulsed electric discharge. The plasma formed with the flowing liquid and gas between the two electrodes causes chemical reactions that generate various compounds.