A method for coupling adsorption-enhanced plasma-induced low-temperature reforming of methanol to produce hydrogen

Abstract

This invention discloses a plasma-induced low-temperature reforming method for hydrogen production from methanol using coupled adsorption enhancement. This method suppresses CO formation through adsorption enhancement and induces low-temperature activation of methanol through plasma discharge. In this invention, a reduced catalytic adsorbent sample is placed in a plasma reactor, nitrogen gas is introduced, and all gas in the device is purged and leaks are checked. Subsequently, the heating element is turned on to preheat the device to 120°C. A prepared methanol-water solution is vaporized in the heating zone using a constant flow pump, and then introduced into the plasma reactor for discharge experiments. The outlet is connected to a gas chromatograph (GC) to detect the gaseous components in the product. This invention utilizes high-energy electron collisions generated at low temperatures by dielectric barrier discharge to induce methanol activation. At temperatures below 160°C, the H2 concentration can reach over 95%, and the methanol conversion rate can reach 80%.

Description

Technical Field

[0001] This invention relates to a plasma-induced low-temperature reforming method for producing hydrogen from methanol with enhanced coupling adsorption, belonging to the field of combustion chemistry and materials technology. Background Technology

[0002] With global warming, air pollution, and energy shortages becoming increasingly prominent, the large-scale development and utilization of clean, low-carbon emerging energy sources is urgently needed. Hydrogen energy, with its advantages of wide availability, renewability, high energy density, and pollution-free byproducts, is hailed as the "ultimate energy" of the 21st century. The end-use applications of hydrogen energy are very extensive, covering multiple fields such as power, transportation, aerospace, and chemicals. Among these, fuel cells are one of the important new technologies for the efficient and clean utilization of hydrogen energy. Hydrogen fuel cell vehicles, which directly convert hydrogen into electricity for power, can achieve truly low pollution or even zero emissions, providing a feasible technological path for the electrification of transportation.

[0003] Traditional hydrogen production processes mainly include coal-to-hydrogen, natural gas-to-hydrogen, and water electrolysis. Coal-to-hydrogen, due to its high investment cost, is typically only used for large-scale production; natural gas, as an important clean energy source, faces strict limitations in its application; and water electrolysis, due to its high power consumption, is currently only suitable for small-scale applications. Methanol is an ideal liquid hydrogen storage carrier and in-situ hydrogen supply carrier, possessing significant advantages such as high hydrogen storage capacity, wide availability, convenient transportation, and low price. Under different process conditions, methanol can be converted into hydrogen through various pathways, among which steam reforming is one of the most promising methods. However, the reforming process is often accompanied by methanol cracking and reverse water-gas shift reactions, leading to problems such as high CO selectivity, low methanol conversion rate, and low energy utilization efficiency.

[0004] Although adsorption enhancement technology can promote the forward shift of the CO-water-gas shift reaction and remove CO2 in situ, the high CO2 desorption temperature easily leads to deactivation of the catalytic adsorbent. Based on the above research, a novel plasma-induced low-temperature reforming method for methanol to produce hydrogen, coupled with adsorption enhancement, is proposed. This method effectively suppresses CO formation through adsorption enhancement, while employing plasma discharge to induce methanol reaction activation at low temperatures. The aim is to achieve high-yield, high-quality, and high-efficiency methanol-water-gas reforming for hydrogen production, and to promote the application of research results on real-time methanol hydrogen supply technology. Summary of the Invention

[0005] To address the problems of high CO selectivity, low methanol conversion rate, and low energy utilization efficiency in existing methanol steam reforming technologies, this invention proposes a plasma-induced low-temperature methanol reforming method with coupled adsorption enhancement, aiming to improve hydrogen purity, reduce carbon monoxide concentration, and achieve efficient methanol-to-hydrogen conversion.

[0006] A plasma-induced low-temperature reforming method for hydrogen production from methanol with coupled adsorption enhancement includes the following steps:

[0007] Step 1): Mix the methanol reforming catalyst with the CO2 adsorbent to obtain a catalyst adsorbent sample. Weigh the reduced catalyst adsorbent sample and place it in the plasma reactor. Introduce nitrogen gas to purge all the gas in the device and check the airtightness.

[0008] Step 2): Prepare a methanol-water solution and introduce it into the preheating device at a flow rate of 0.004–0.01 ml / min using a constant flow pump for vaporization;

[0009] Step 3): The generated methanol vapor is fed into the plasma reactor for discharge experiment. The reactor outlet is connected to a gas chromatograph to detect H2, CO2, CO, N2, CH4 and unreacted methanol CH3OH products. When stopping the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0010] Step 4): The reacted catalytic adsorbent is purged with nitrogen at 250-450℃ for desorption and regeneration. The regenerated catalytic adsorbent is then recycled according to steps 1) to 3).

[0011] This invention is the first to apply adsorption enhancement and plasma coupling to methanol reforming for hydrogen production. Based on effectively suppressing CO formation by utilizing adsorption enhancement, plasma discharge is used to induce methanol to achieve reaction activation at low temperature, thereby realizing efficient hydrogen production from methanol at low temperature.

[0012] In this invention, the reaction apparatus includes a gas cylinder, valves, a mass flow meter, a constant flow pump, a heating belt, a plasma reactor, and a gas chromatograph. The plasma reactor consists of a plasma generator, a transformer, an oscilloscope, and a power supply.

[0013] In step 1) of this invention, copper-based, palladium-based, platinum-based, and rhodium-based materials are used as catalysts for methanol steam reforming to provide active sites for the reaction, reduce the activation energy, and increase the reaction rate. Low-temperature potassium-based, sodium-based, and medium-temperature magnesium-based materials are used as CO2 adsorbents to promote the forward shift of the reaction and increase the hydrogen concentration. High-energy electron collisions generated at low temperatures by non-thermal barrier discharge induce methanol activation, thereby achieving high-conversion low-temperature reforming of methanol to produce hydrogen.

[0014] In this invention, in step 1), the reaction space velocity ranges from 1000 to 4000 h⁻¹. -1 .

[0015] In this invention, in step 1), the plasma reactor consists of a plasma generator, a transformer, an oscilloscope, and a power supply.

[0016] In this invention, in step 2), the water-to-alcohol ratio is 0.8 to 1.5:1.

[0017] In this invention, in step 3), the plasma discharge power is 30-70W and the discharge temperature is 120-200℃.

[0018] In this invention, in step 4), the desorption and regeneration temperature of the catalytic adsorbent is 250–450°C.

[0019] In this invention, the thermocatalytic methanol steam reforming experiment under the action of a single catalyst was carried out in a fixed-bed reactor as a control group. The experimental steps were the same as above, and the reaction temperature of the fixed-bed reactor was 160-220℃.

[0020] The beneficial effects of this invention are as follows:

[0021] 1) This invention reports for the first time the coupling of adsorption enhancement with plasma to achieve the preparation of high-purity hydrogen at low temperatures. Within the first 1.5 minutes of the reaction, the H2 concentration can reach 100%, meaning that the CO2 generated at the beginning of the reaction is completely adsorbed by the adsorbent. As time progresses, CO2 adsorption reaches saturation, and the H2 concentration stabilizes at around 75%. Furthermore, under adsorption enhancement conditions, the equilibrium of methanol cracking and reverse water-gas shift reaction is limited, effectively suppressing CO formation. Compared with single catalyst and single plasma discharge reactions, adsorption enhancement coupled with plasma significantly improves methanol conversion rate and hydrogen concentration at low temperatures.

[0022] 2) The high-energy electrons, ions, and free radicals generated during plasma discharge can collide and react with methanol molecules, effectively promoting the decomposition and conversion of methanol. These active substances can interact with the active sites on the catalyst surface, forming more active centers and significantly increasing the rate of methanol reforming. Plasma discharge can also maintain a high methanol conversion rate at low temperatures (<160℃), thus effectively inhibiting catalytic adsorbent deactivation and reducing the catalytic adsorbent desorption and regeneration temperature.

[0023] 3) Compared to conventional methanol steam reforming, the adsorption-enhanced coupled plasma reaction proceeds at lower temperatures and pressures, reducing the requirements for reaction equipment and decreasing energy consumption. The reaction yields higher-quality hydrogen, thereby improving energy density and power generation efficiency when used in conjunction with proton exchange membrane fuel cells, providing a new approach for achieving high-yield, high-quality, and high-efficiency methanol steam reforming for hydrogen production.

[0024] Based on the above analysis, it can be seen that the plasma-induced methanol low-temperature reforming method for hydrogen production by coupled adsorption enhancement has a low methanol conversion temperature, high hydrogen purity, simple and easy operation, and the produced hydrogen can be directly used in proton exchange membrane fuel cells with high energy efficiency and wide applicability. Attached Figure Description

[0025] Figure 1 Schematic diagram of an experimental setup for low-temperature reforming of methanol and water vapor to produce hydrogen via adsorption-enhanced coupled plasma activation.

[0026] Figure 2 Schematic diagram of an experimental setup for hydrogen production via methanol steam reforming enhanced by single adsorption.

[0027] Figure 3 This is a graph showing the changes in methanol conversion rate and product concentration over time in Example 1.

[0028] Figure 4 This is a graph showing the changes in methanol conversion rate and product concentration over time in Example 2.

[0029] Figure 5 This is a graph showing the changes in methanol conversion rate and product concentration over time in Example 3.

[0030] Figure 6 This is a graph showing the changes in methanol conversion rate and product concentration over time in Example 4.

[0031] Figure 7 This is a graph showing the changes in methanol conversion rate and product concentration over time in Example 5.

[0032] Figure 8 This is a graph showing the changes in methanol conversion rate and product concentration over time for Comparative Example 1.

[0033] Figure 9 This is a graph showing the changes in methanol conversion rate and product concentration over time for Comparative Example 2.

[0034] Figure 10 The image shows the Lissajous figure for Example 1 when the discharge power is 60W;

[0035] Figure 11 The Lissajous diagram is shown for Example 2 when the discharge power is 45W;

[0036] Figure 12 The Lissajous diagram is shown for Example 3 when the discharge power is 75W;

[0037] Figure 13 This is a graph showing the temperature variation inside the plasma reactor with discharge power. Detailed Implementation

[0038] The present invention will be further described below with reference to embodiments, comparative examples, and the accompanying drawings.

[0039] Example 1:

[0040] Through experimental testing

[0041] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it into the plasma reactor;

[0042] 2) Prepare 100 ml of methanol aqueous solution by mixing water and methanol at a molar ratio of 1.2:1;

[0043] 3) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 .

[0044] 4) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 60W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a mixture with a water-to-alcohol ratio of 1.2 is passed through a constant flow pump into the preheater (120℃) for vaporization, and then introduced into the plasma reactor.

[0045] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0046] Figure 3 The graph shows the changes in methanol conversion rate and product concentration over time. As can be seen from the graph, the hydrogen concentration is as high as 99.98% after 1.5 min of reaction. The concentration tends to stabilize after about 15 min, with a hydrogen concentration of 72% and a methanol conversion rate of 72%. No CO or methane is generated during the reaction. Figure 10 The Lissajous diagram corresponds to a discharge power of 60W.

[0047] Example 2:

[0048] The only difference from Example 1 is that the plasma discharge power is 45W.

[0049] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it into the plasma reactor;

[0050] 2) Prepare 100 ml of methanol aqueous solution by mixing water and methanol at a molar ratio of 1.2:1;

[0051] 3) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 .

[0052] 4) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 45W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a mixture with a water-to-alcohol ratio of 1.2 is vaporized by passing it through a constant flow pump at a specific flow rate into the preheater (120℃), and then into the plasma reactor.

[0053] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0054] Figure 4 The graph shows the changes in methanol conversion rate and product concentration over time in Example 2. As can be seen from the graph, the hydrogen concentration is as high as 99.95% after 1.5 min of reaction. The reaction tends to stabilize after about 15 min, at which point CO2 adsorption reaches saturation, the hydrogen concentration is 72%, the methanol conversion rate is 59%, and no CO or methane is generated during the reaction. Figure 11 The image shows a Lissajous plot corresponding to a discharge power of 45W. Compared to Example 1, the methanol conversion rate is lower, and the area of ​​the Lissajous plot is smaller.

[0055] Example 3:

[0056] The only difference from Example 1 is that the plasma discharge power is 75W.

[0057] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it into the plasma reactor;

[0058] 2) Prepare 100 ml of methanol aqueous solution by mixing water and methanol at a molar ratio of 1.2:1;

[0059] 3) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 .

[0060] 4) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 75W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a mixture with a water-to-alcohol ratio of 1.2 is vaporized by passing it through a constant flow pump at a specific flow rate into the preheater (120℃), and then into the plasma reactor.

[0061] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0062] Figure 5 The graph shows the changes in methanol conversion rate and product concentration over time in Example 3. As can be seen from the graph, the hydrogen concentration is as high as 99.99% after 1.5 min of reaction. The reaction tends to stabilize after about 15 min, at which point CO2 adsorption reaches saturation, the hydrogen concentration is 73%, the methanol conversion rate is 81%, and no CO or methane is generated during the reaction. Figure 12 The image shows a Lissajous plot corresponding to a discharge power of 75W. Compared to Example 1, the methanol conversion rate is increased, and the area of ​​the Lissajous plot is larger.

[0063] Figure 13 The graph shows the temperature variation with discharge power in the plasma reactors of Examples 1, 2, and 3. As can be seen from the graph, the reaction temperature increases with increasing discharge power.

[0064] Example 4:

[0065] The only difference from Example 1 is that the molar ratio of water to methanol is 1:1.

[0066] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it into the plasma reactor;

[0067] 2) Prepare 100 ml of methanol aqueous solution by mixing water and methanol in a molar ratio of 1:1;

[0068] 3) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 .

[0069] 4) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 45W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a 1:1 water-to-alcohol mixture is vaporized by passing it through a constant flow pump at a specific flow rate into the preheater (120℃), and then into the plasma reactor.

[0070] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0071] Figure 6 The graph shows the changes in methanol conversion rate and product concentration over time in Example 4. As can be seen from the graph, the hydrogen concentration reaches as high as 99.98% after 1.5 min of reaction, and stabilizes at 72% after about 15 min, with a methanol conversion rate of 62%. Compared to Example 1, the methanol conversion rate is lower.

[0072] Example 5:

[0073] Compared with Example 1, the only difference is that the nitrogen flow rate was changed, and the reaction space velocity was set to 3500 h⁻¹. -1 .

[0074] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it into the plasma reactor;

[0075] 2) Prepare 100 ml of methanol aqueous solution by mixing water and methanol at a molar ratio of 1.2:1;

[0076] 3) Introduce nitrogen gas into the reaction apparatus at a rate of 50 ml / min and check the airtightness of the apparatus. The reaction space velocity is 3500 h⁻¹. -1 .

[0077] 4) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 45W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a 1:1 water-to-alcohol mixture is vaporized by passing it through a constant flow pump at a specific flow rate into the preheater (120℃), and then into the plasma reactor.

[0078] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0079] Figure 7 The graph shows the changes in methanol conversion rate and product concentration over time in Example 5. As can be seen from the graph, the hydrogen concentration reaches as high as 99.96% after 1.5 min of reaction, and stabilizes at around 71% after about 15 min, with a methanol conversion rate of 51%. Compared to Example 1, the methanol conversion rate is lower.

[0080] Comparative Example 1:

[0081] Compared with Example 1, the only difference is that no catalytic adsorbent is added to the reactor, and only plasma discharge occurs.

[0082] 1) Prepare 100 ml of methanol aqueous solution by mixing water and methanol in a molar ratio of 1.2:1;

[0083] 2) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 ;

[0084] 3) After the airflow stabilizes, turn on the power switch of the plasma generator, adjust the discharge power to 45W using a transformer, and adjust the discharge frequency to about 9.5kHz to ensure stable discharge. Record the temperature inside the reactor at this time using an infrared thermometer. Subsequently, a mixture with a water-to-alcohol ratio of 1.2 is vaporized by passing it through a constant flow pump at a specific flow rate into the preheater (120℃), and then into the plasma reactor.

[0085] 4) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0.

[0086] Figure 8 The graph shows the changes in methanol conversion rate and product concentration over time in Comparative Example 1. As can be seen from the graph, the hydrogen concentration is approximately 60%, CH4 and CO are generated in the products, and the methanol conversion rate is approximately 40%. Compared to Example 1, both the hydrogen concentration and methanol conversion rate are reduced.

[0087] Comparative Example 2:

[0088] Compared to Example 1, the only difference is that there is only a single adsorption enhancement effect, and the reaction is carried out in a fixed-bed reactor.

[0089] 1) Weigh 0.3g of the mixture of copper-based catalyst and magnesium-based adsorbent and place it in a quartz tube (Φ=8mm), and support it in the constant temperature zone of the vertical furnace with quartz wool and a liner tube;

[0090] 2) Introduce nitrogen gas into the reaction apparatus at a rate of 40 ml / min and check the airtightness of the apparatus. The reaction space velocity is 2500 h⁻¹. -1 .

[0091] 3) Prepare 100 ml of methanol aqueous solution by mixing water and methanol in a molar ratio of 1.2:1;

[0092] 4) The mixture is vaporized by passing it through a constant flow pump into the heating zone (120°C) at a specific flow rate, and then into a fixed bed reactor at a reaction temperature of 180°C.

[0093] 5) Connect a gas chromatograph (GC) to the reactor outlet to detect products such as H2, CO2, CO, N2, CH4, and unreacted methanol (CH3OH). To stop the reaction, first turn off the constant flow pump to stop the feed, then turn off the furnace, and finally adjust the nitrogen pressure reducing valve to 0.

[0094] Figure 9 The graph shows the changes in methanol conversion rate and product concentration over time for Comparative Example 2. As can be seen from the graph, the hydrogen concentration is as high as 98.12% after 1.5 min of reaction. The hydrogen concentration tends to stabilize at 70% after about 15 min of reaction, and the methanol conversion rate is 71%. No CO or methane is generated during the reaction.

[0095] Table 1 summarizes the methanol conversion rate and product concentration results under the experimental conditions of the examples and comparative examples. As shown in the table, no CO or CH4 was generated in the products under either the plasma + adsorption enhancement or single adsorption enhancement conditions, indicating that adsorption enhancement inhibits the reaction byproduct CO. The hydrogen concentration and methanol conversion rate under the plasma + adsorption enhancement reaction conditions were significantly higher than those under single plasma and single adsorption enhancement conditions, indicating that the plasma-induced low-temperature reforming method for methanol to produce hydrogen using coupled adsorption enhancement can achieve a high methanol conversion rate at low temperatures, providing a new approach for achieving high-yield, high-quality, and high-efficiency methanol steam reforming to produce hydrogen.

[0096] Table 1

[0097]

[0098] The above embodiments are only used to illustrate the technical solutions of the present invention, and are not intended to limit it. Although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some of the technical features. Such modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A plasma-induced low-temperature reforming method for hydrogen production from methanol using coupled adsorption enhancement, comprising: Step 1): Mix the methanol reforming catalyst with the CO2 adsorbent to obtain a catalyst adsorbent sample. Weigh the reduced catalyst adsorbent sample and place it in the plasma reactor. Introduce nitrogen gas to purge all the gas in the device and check the airtightness. Step 2): Prepare a methanol-water solution and introduce it into the preheating device at a flow rate of 0.004~0.01 ml / min using a constant flow pump for vaporization; Step 3): The generated methanol vapor is fed into the plasma reactor for discharge experiments. The plasma discharge power is 30~70W and the discharge temperature is 120~200℃. The reactor outlet is connected to a gas chromatograph to detect H2, CO2, CO, N2, CH4 and unreacted methanol CH3OH products. When stopping the reaction, first turn off the constant flow pump to stop the feed, adjust the transformer input voltage to 0, turn off the plasma generator power switch, and finally adjust the nitrogen pressure reducing valve to 0. Step 4): The reacted catalytic adsorbent is purged with nitrogen at 250~450℃ for desorption and regeneration. The regenerated catalytic adsorbent is then recycled according to steps 1) to 3).

2. The plasma-induced low-temperature reforming method for hydrogen production from methanol with coupled adsorption enhancement according to claim 1, wherein: In step 1), copper-based, palladium-based, platinum-based, and rhodium-based materials are used as catalysts for methanol steam reforming, and low-temperature potassium-based, sodium-based, and medium-temperature magnesium-based materials are used as CO2 adsorbents.

3. The plasma-induced low-temperature reforming method for hydrogen production from methanol with coupled adsorption enhancement according to claim 1, wherein: In step 1), the nitrogen gas is introduced by introducing nitrogen gas into a reaction apparatus and checking the airtightness of the apparatus, and the reaction space velocity is 1000 to 4000 h -1 .

4. The plasma-induced low-temperature reforming method for hydrogen production from methanol with coupled adsorption enhancement according to claim 1, wherein: In step 2), the molar ratio of water to methanol is 0.8~1.5:

1.

5. The method for hydrogen production from methanol via coupled adsorption-enhanced plasma-induced low-temperature reforming according to claim 1, wherein: In step 3), the plasma discharge type is non-thermal barrier discharge.

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