Method and system for preparing hydrocarbon-rich carbon-based fuel gas by driving carbon dioxide/water synergistic conversion through molten salt electrochemical method

A carbon dioxide, hydrocarbon-rich carbon-based technology, applied in electrodes, electrolysis process, electrolysis components, etc., can solve the problems of system short circuit, experiment failure, carbon powder falling off, etc., to improve corrosion resistance, avoid oxidation and corrosion, and prolong life. effect of time

Inactive Publication Date: 2021-02-23
NORTHEAST GASOLINEEUM UNIV
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Problems solved by technology

[0003] Chinese patent application CN104562073A provides a high temperature electrolytic CO 2 / H 2 O to produce hydrocarbon systems that can achieve CO at relatively low temperatures at low electrolysis voltages 2 / H 2 The co-electrolysis of O, conversion to hydrocarbons, and the electrolysis reaction is relatively simple, and the selectivity of the electrolysis reaction is good in a short time; this patent application has already covered CO 2 The transformation mechanism in the molten salt system and the key control factors of the electrolysis process have been clearly explored, but the electrode problem has not been well resolved; this is because traditional metal anodes cannot remain stable in the molten salt system for a long time The main reason is the electrochemical oxidation of the anode and the physical dissolution of the surface oxide film
For example, in the Chinese patent application CN104562073A, when metallic nickel is selected as the molten salt electrochemical method to drive CO 2 / H 2 When O synergistic conversion is used to prepare the anode of the hydrocarbon-rich carbon-based fuel gas system, a certain corrosion resistance can be maintained in a short period of time, but with the prolongation of the reaction time, the nickel anode is gradually oxidized to nickel oxide, and severe corrosion will occur Phenomena, resulting in the decrease of current efficiency and energy loss of gas products, and even electrode breakage, which cannot guarantee the continuity of electrochemical reactions for a long time
In addition, Chinese patent application CN104562073A in CO 2 The electrolysis experiment was carried out in a gas atmosphere, but the CO 2 The high partial pressure leads to a strong tendency of carbon generation in the system. During the electrolysis process, a large amount of solid elemental carbon is deposited on the cathode, resulting in a low conversion rate of gas products, and some carbon powder falls off in the molten salt system. The salt system causes pollution, and even causes a short circuit in the system, resulting in the failure of the experiment

Method used

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  • Method and system for preparing hydrocarbon-rich carbon-based fuel gas by driving carbon dioxide/water synergistic conversion through molten salt electrochemical method
  • Method and system for preparing hydrocarbon-rich carbon-based fuel gas by driving carbon dioxide/water synergistic conversion through molten salt electrochemical method
  • Method and system for preparing hydrocarbon-rich carbon-based fuel gas by driving carbon dioxide/water synergistic conversion through molten salt electrochemical method

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0061] Embodiment 1: the corrosion resistance (durability) experiment of preoxidation film-forming nickel electrode

[0062] ① Na 2 CO 3 -K 2 CO 3 A total of 50g of mixed molten salt +0.2LiOH is put into an alumina crucible, the operating temperature is 700°C, and the surface area is 20cm 2 The nickel anode and nickel cathode were inserted into the molten salt medium; in an argon atmosphere, a 3h pre-oxidation film-forming treatment was performed at a constant voltage of 1.0V to obtain a molten salt in-situ pre-oxidation film-forming nickel anode.

[0063] ②Set the surface area to 20cm 2 The nickel electrode was heated in air at 800°C for 2 hours to prepare an air-heated pre-oxidized film-forming nickel anode.

[0064] The pre-oxidized film-forming nickel electrode prepared by the above two methods was used as the anode, and the iron with the same surface area was used as the cathode. 0.85 Na0.61 K 0.54 CO 3 +0.2LiOH mixed molten salt is used as the electrolyte, and th...

Embodiment 2

[0069] Example 2: H 2 Effect of O flow rate on gas product formation rate experiment

[0070] The surface area is 20cm 2 The pre-oxidized film-forming nickel anode and iron cathode obtained by the method of air heating film-forming in Example 1, at 575 ° C, the amount of electrolyte with a 2.0V constant voltage is 100g of Li 0.85 Na 0.61 K 0.54 CO 3 +0.2LiOH+0.05CaO molten salt system, the CO 2 The flow rate is controlled at 180mL / h, the Ar flow rate is controlled at 600mL / h, and the H 2 When the O flow rate is 0.10, 0.15, 0.20, 0.25g / h, the CH 4 and H 2 output rate, the result is as follows Figure 7 And as shown in Table 2: when H in the feed gas 2 When O flow rate is 0.10g / h, methane (CH 4 ) formation rate is 31.21mL / h, H 2 The formation rate reached 38.72mL / h, and the CH in the gas product 4 The content is low, and the economic value is not high; with the H in raw materials 2 Gradual increase of O flow rate, CH 4 The generation rate increases accordingly, whe...

Embodiment 3

[0072] Example 3: CO 2 Effect of flow rate on gas product generation rate experiment

[0073] The surface area is 20cm 2 The pre-oxidized film-forming nickel anode and iron cathode obtained by the method of air heating film-forming in Example 1, at 575 ° C, the amount of electrolyte with a 2.0V constant voltage is 100g of Li 0.85 Na 0.61 K 0.54 CO 3 +0.2LiOH+0.05CaO molten salt system, H 2 The flow rate of O is controlled at 0.15g / h, and the flow rate of Ar is controlled at 600mL / h. 2 When the flow rate is 180, 300, 600, 900mL / h, the CH in the gas product 4 and H 2 output rate, the result is as follows Figure 9 and Table 2: When CO 2 When the flow rate is 180mL / h, CH 4 The production rate was the highest, reaching 34.66mL / h. But with CO 2 As the flow rate increases, the CO inside the reactor 2 As the partial pressure increases, the whole system tends to undergo elemental carbon deposition reaction, making CH in the product 4 Spawn rate decreased. Due to the ele...

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Abstract

The invention relates to a method and system for preparing hydrocarbon-rich carbon-based fuel gas by driving carbon dioxide/water synergistic conversion through a molten salt electrochemical method, and the method comprises the following steps: carrying out pre-oxidation film-forming treatment on a nickel electrode to obtain a modified nickel electrode; taking mixed molten salt formed by carbonateand hydroxide as a molten salt medium, taking the modified nickel electrode as an anode, and taking nickel, platinum, titanium, iridium, ruthenium, palladium, iron, tungsten, chromium, copper, gold,graphite or stainless steel materials as a cathode to form a molten salt electrochemical reactor; and carrying water vapor by using a mixed gas of carbon dioxide and argon, and introducing the water vapor into the molten salt electrochemical reactor to carry out electrochemical reduction reaction so as to drive CO2/H2O to synergistically convert and prepare the hydrocarbon-rich carbon-based fuel gas. The method can continuously drive CO2/H2O to synergistically convert and prepare the hydrocarbon-rich carbon-based fuel gas for a long time, has the advantages of high gas product conversion rate,high gas product current efficiency and the like, and opens up a new green, environment-friendly and efficient CO2 resource utilization way.

Description

technical field [0001] The invention belongs to high temperature molten salt driving CO 2 / H 2 The technical field of O hydrocarbon production system, especially relates to a molten salt electrochemical method to drive CO 2 / H 2 A method and system for preparing hydrocarbon-rich carbon-based fuel gas by synergistic conversion of O. Background technique [0002] In view of the serious situation of global carbon dioxide emissions and forest area sharp decline, the problem of climate warming caused by the greenhouse effect has attracted the attention of many scientific research institutions. How to achieve carbon dioxide emission reduction and resource utilization on the premise of ensuring rapid economic development has become a worldwide problem. Develop green, efficient and environmentally friendly CO 2 The capture and conversion method is an important way to alleviate the greenhouse effect and realize the recycling of resources. In recent years, breakthroughs have bee...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B3/03C25B3/26C25B9/17C25B11/042C25B15/08C25B15/02C25B15/021C25B15/023C25B1/02
CPCC25B1/02C25B11/04C25B15/02C25B15/08
Inventor 纪德强吴红军纪德彬朱凌岳苑丹丹王鹏
Owner NORTHEAST GASOLINEEUM UNIV
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