WO2022001985A1 - Natural gas desulfurization apparatus - Google Patents

Natural gas desulfurization apparatus Download PDF

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Publication number
WO2022001985A1
WO2022001985A1 PCT/CN2021/102847 CN2021102847W WO2022001985A1 WO 2022001985 A1 WO2022001985 A1 WO 2022001985A1 CN 2021102847 W CN2021102847 W CN 2021102847W WO 2022001985 A1 WO2022001985 A1 WO 2022001985A1
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WIPO (PCT)
Prior art keywords
desulfurization
natural gas
dry
gas
wet
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PCT/CN2021/102847
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French (fr)
Inventor
Songtao Chen
Original Assignee
Ceres Intellectual Property Company Limited
Weichai Power Co., Ltd.
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Application filed by Ceres Intellectual Property Company Limited, Weichai Power Co., Ltd. filed Critical Ceres Intellectual Property Company Limited
Publication of WO2022001985A1 publication Critical patent/WO2022001985A1/en

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/18—Absorbing units; Liquid distributors therefor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/26—Drying gases or vapours
    • B01D53/261—Drying gases or vapours by adsorption
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
    • B01D2252/30—Ionic liquids and zwitter-ions
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2256/00—Main component in the product gas stream after treatment
    • B01D2256/24—Hydrocarbons
    • B01D2256/245—Methane
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/30—Sulfur compounds
    • B01D2257/304—Hydrogen sulfide

Definitions

  • the present invention pertains to the field of desulfurization and particularly relates to a natural gas desulfurization apparatus for use with an SOFC system.
  • Natural gas typically contains acid gases such as inorganic sulfides (mainly H 2 S) and organic sulfides. Their presence will not only corrode the equipment, but also cause toxic damage to the SOFC stack, which will seriously affect the safety of the stack. Therefore, natural gas needs to be desulfurized and purified before entering the stack. Moreover, in order to achieve the desulfurization effect required by SOFC, a conventional desulfurization apparatus currently in use is relatively heavy and bulky and so is not convenient for installation and use on a vehicle.
  • acid gases such as inorganic sulfides (mainly H 2 S) and organic sulfides. Their presence will not only corrode the equipment, but also cause toxic damage to the SOFC stack, which will seriously affect the safety of the stack. Therefore, natural gas needs to be desulfurized and purified before entering the stack.
  • a conventional desulfurization apparatus currently in use is relatively heavy and bulky and so is not convenient for installation and use on a vehicle.
  • the present invention provides a natural gas desulfurization apparatus.
  • the natural gas desulfurization apparatus provided by the present invention comprises a wet desulfurization device and a dry desulfurization device and has an excellent desulfurization effect, and the two desulfurization devices can be arranged separately, so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle.
  • the present invention provides a natural gas desulfurization apparatus, comprising:
  • a wet desulfurization device which is provided with a natural gas inlet and a wet desulfurization gas outlet, and in which the desulfurizer is an alkali-functionalized protic ionic liquid;
  • a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying device.
  • the wet desulfurization device can comprise a wet desulfurization vessel for containing the alkaline-functionalized protic ionic liquid, a natural gas inlet arranged at the bottom of the wet desulfurization vessel, and a wet desulfurization gas outlet arranged at the top of the wet desulfurization vessel.
  • Several layers of orifice plates can be arranged in the wet desulfurization vessel, a certain predetermined distance being reserved between two adjacent layers of the orifice plates, and the orifices of two adjacent layers of the orifice plates are interlaced or offset.
  • the position of the bottommost layer of the orifice plates can be flush with the level of the ionic liquid contained in the wet desulfurization vessel.
  • a certain predetermined distance can be kept between the topmost layer of the orifice plates and the top of the wet desulfurization vessel.
  • the number of layers of the orifice plates can be 2 to 5.
  • the natural gas inlet can be provided with an inlet gas filter; and the wet desulfurization gas outlet can be provided with an outlet gas filter.
  • the wet desulfurization device can be further provided with an ionic liquid regeneration outlet.
  • the drying device can comprise a first drying unit and a second drying unit, the first drying unit can be a dryer filled with desiccant, and the second drying unit can be a dewatering filter;
  • a gas inlet of the dryer is connected to the wet desulfurization gas outlet
  • a dry gas outlet of the dryer is connected to a gas inlet of the dewatering filter
  • a dry gas outlet of the dewatering filter is connected to a gas inlet of the dry desulfurization device.
  • the dry desulfurization device can comprise a dry desulfurization vessel used for containing a dry desulfurizer, a gas inlet arranged at the bottom of the dry desulfurization vessel, and a dry desulfurization gas outlet arranged at the top of the dry desulfurization vessel.
  • the present invention provides a natural gas desulfurization apparatus.
  • the natural gas desulfurization apparatus provided by the present invention comprises a wet desulfurization device, which is provided with a natural gas inlet and a wet desulfurization gas outlet and in which the desulfurizer is an alkali-functionalized protic ionic liquid.
  • the present invention provides a composite desulfurization apparatus, which connects wet desulfurization and dry desulfurization in series.
  • the natural gas to be desulfurized is led into the wet desulfurization device using an alkali-functionalized protic ionic liquid (MLB-PILs) as a desulfurizer to remove inorganic sulfides represented by H 2 S.
  • MLB-PILs alkali-functionalized protic ionic liquid
  • H 2 S inorganic sulfides represented by H 2 S.
  • the natural gas from which inorganic sulfur has been removed enters the drying device for drying and dewatering.
  • the dewatered natural gas enters the dry desulfurization device to remove organic sulfides to obtain a desulfurized natural gas.
  • the desulfurization apparatus provided by the present invention uses the wet desulfurization device to remove inorganic sulfides in natural gas, uses the dry desulfurization device to remove organic sulfides in natural gas, and has an excellent desulfurization effect.
  • the two desulfurization devices in the desulfurization apparatus can be arranged separately so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle.
  • Fig. 1 is a structural schematic view of a natural gas desulfurization apparatus.
  • Fig. 2 is a structural schematic view of a wet desulfurization device.
  • Fig. 3 is a structural schematic view of an integrated adapter.
  • Fig. 4 is a structural schematic view of a natural gas desulfurization apparatus with two drying units.
  • the present invention provides a natural gas desulfurization apparatus, comprising:
  • a wet desulfurization device which is provided with a natural gas inlet and a wet desulfurization gas outlet and in which the desulfurizer is an alkali-functionalized protic ionic liquid;
  • a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying device.
  • Fig. 1 is a structural schematic view of a natural gas desulfurization apparatus provided in an embodiment of the present invention.
  • the apparatus of Fig. 1 includes a wet desulfurization device 1, a drying device 2, and a dry desulfurization device 3.
  • Fig. 2 is a structural schematic view of a wet desulfurization device provided in an embodiment of the present invention.
  • the device of Fig. 2 includes a natural gas inlet 11, a wet desulfurization vessel 12, an alkali-functionalized protic ionic liquid 13, an orifice plate 14, a wet desulfurization gas outlet 15, and an ionic liquid regeneration outlet 16.
  • the natural gas desulfurization apparatus comprises a wet desulfurization device 1, a drying device 2 and a dry desulfurization device 3.
  • the wet desulfurization device 1 is used for removing inorganic sulfides in natural gas (e.g., H 2 S) .
  • a natural gas inlet 11 and a wet desulfurization gas outlet 15 are arranged on the wet desulfurization device and the desulfurizer in the wet desulfurization device 1 is an alkali-functionalized protic ionic liquid 13, preferably a 3-diaminopropane acetic acid ( [TDMAPAH] [Ac] ) solution.
  • the concentration of the 3-diaminopropane acetic acid solution can be 40 to 50 wt%, such as 48 wt%.
  • the wet desulfurization device 1 comprises a wet desulfurization vessel used for containing the alkaline-functionalized protic ionic liquid 12.
  • a natural gas inlet 11 arranged at the bottom of the wet desulfurization vessel 12 and a wet desulfurization gas outlet 15 arranged at the top of the wet desulfurization vessel 12.
  • the included angle between the natural gas inlet 11 and the wet desulfurization gas outlet 15 is 90°.
  • the wet desulfurization vessel 12 In order to prevent the ionic liquid contained in the wet desulfurization vessel 12 from overflowing due to vibration of the vehicle, several layers of orifice plates 14 are arranged in the wet desulfurization vessel 12, with a predetermined distance maintained between two adjacent layers of the orifice plates. The orifices of two adjacent layers of the orifice plates are interlaced or offset. This can effectively block the ionic liquid from surging out and prevent the ionic liquid from entering the wet desulfurization gas outlet 15. The position of the bottommost layer of the orifice plates in the wet desulfurization vessel 12 is flush with the level of the ionic liquid 13 contained in the wet desulfurization vessel 12. This setting method can effectively prevent the ionic liquid from oscillating back and forth.
  • a certain distance is kept between the topmost layer of the orifice plates and the top of the wet desulfurization vessel 12.
  • the existence of this distance can reserve a certain space for the gathering of the gas separated from the liquid phase, thereby keeping the gas pressure relatively stable.
  • the number of layers of the orifice plates 14 in the wet desulfurization vessel 12 is 2 to 5, may be 2, 3, 4 or 5.
  • the natural gas inlet 11 is provided with an inlet gas filter.
  • the wet desulfurization gas outlet 15 is provided with an outlet gas filter.
  • the natural gas inlet 11 is equipped with a gas inlet adapter and the wet desulfurization gas outlet 15 is equipped with a gas outlet adapter.
  • One embodiment is equipped with an adapter and provided with a filter. The filter is not arranged separately but integrated on the adapter at the gas inlet/outlet, as shown in Fig. 3.
  • Fig. 3 is a structural schematic view of an integrated adapter provided in an embodiment of the present invention.
  • the filter element 112 is arranged at an internal step of the adapter body 111, and the filter 112 is a sintered filter element.
  • the size of the filtration pores is 0.1 to 1 ⁇ m, and may be 0.5 ⁇ m.
  • the wet desulfurization device 1 is further provided with an ionic liquid regeneration outlet 1-6.
  • the ionic liquid regeneration outlet 1-6 is arranged at the bottom of the wet desulfurization vessel 12 and a valve is arranged on the ionic liquid regeneration outlet.
  • the wet desulfurizer in a saturated absorption state can be discharged out of the wet desulfurization device 1, and then is desorbed and regenerated by such methods as heating and pressure reduction.
  • the regenerated wet desulfurizer can be reused in the wet desulfurization device 1.
  • the drying device 2 is used for dewatering and drying the natural gas that has been desulfurized by the wet process, a gas inlet and a dry gas outlet are arranged on the drying device, and the gas inlet of the drying device 2 is connected to a wet desulfurization gas outlet of the wet desulfurization device 1.
  • the drying device 2 comprises two drying units, as shown in Fig. 4.
  • Fig. 4 is a structural schematic view of a natural gas desulfurization apparatus with two drying units provided in an embodiment of the present invention.
  • the apparatus of Fig. 4 includes a dryer 2-1 and a dewatering filter 2-2.
  • the drying device 2 comprises a first drying unit and a second drying unit.
  • the first drying unit is a dryer 2-1.
  • a gas inlet and a dry gas outlet are arranged on the dryer and the gas inlet of the dryer 2-1 is connected to the wet desulfurization gas outlet of the wet desulfurization device 1.
  • the dryer 2-1 is internally filled with desiccant.
  • the desiccant can include CaSO 4 and /or CaCl 2 .
  • the second drying unit can be a dewatering filter 2-2.
  • a gas inlet and a dry gas outlet are arranged on the dewatering filter and the gas inlet of the dewatering filter 2-2 is connected to the dry gas outlet of the dryer 2-1.
  • the dry desulfurization device 3 is used for removing organic sulfides in natural gas after drying.
  • a gas inlet and a dry desulfurization gas outlet are arranged on the dry desulfurization device and the gas inlet of the drying device 3 is connected to the dry gas outlet of the drying device 2.
  • the dry desulfurization device 3 comprises a dry desulfurization vessel used for containing a dry desulfurizer, a gas inlet arranged at the bottom of the dry desulfurization vessel, and a dry desulfurization gas outlet arranged at the top of the dry desulfurization vessel.
  • the dry desulfurizer includes CuO and adjuvants, and the adjuvants include MnO and/or Al 2 O 3 .
  • the present invention provides a composite desulfurization apparatus which connects wet desulfurization and dry desulfurization in series.
  • the natural gas to be desulfurized is led into the wet desulfurization device using an alkali-functionalized protic ionic liquid (MLB-PILs) as a desulfurizer to remove inorganic sulfides represented by H 2 S.
  • MLB-PILs alkali-functionalized protic ionic liquid
  • H 2 S alkali-functionalized protic ionic liquid
  • the natural gas removed of inorganic sulfur enters the drying device for drying and dewatering.
  • the dewatered natural gas enters the dry desulfurization device to remove organic sulfides to obtain a desulfurized natural gas.
  • the desulfurization apparatus provided by the present invention uses the wet desulfurization device to remove inorganic sulfides in natural gas, uses the dry desulfurization device to remove organic sulfides in natural gas, and has an excellent desulfurization effect.
  • the two desulfurization devices in the desulfurization apparatus can be arranged separately, so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle. More specifically, the desulfurization apparatus provided by the present invention has the following advantages:
  • the alkali-functionalized protic ionic liquid is used as a desulfurizer of the wet desulfurization device.
  • the raw materials are easily available and cheap and adopt simple synthesis processes.
  • a 48wt%3-diaminopropane acetic acid solution is used as a desulfurizer of the wet desulfurization device. This is superior to other H 2 S absorbents in terms of absorbing capacity, viscosity, and cost, and is more suitable to be used as a desulfurizer of natural gas.
  • the wet desulfurizer in a saturated absorption state can be regenerated by such methods as heating and pressure reduction. Compared with a fresh absorbent, the absorbing capacity of the regenerated absorbent is reduced by about 7.5%only, so it can be reused.
  • the wet desulfurization device and the dry desulfurization device can be arranged separately, so that the vehicle space can be used more efficiently and more space can be saved for other components.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Drying Of Gases (AREA)
  • Gas Separation By Absorption (AREA)
  • Treating Waste Gases (AREA)

Abstract

The invention pertains to the field of desulfurization and particularly relates to a natural gas desulfurization apparatus. The natural gas desulfurization apparatus provided by the invention comprises a wet desulfurization device, which is provided with a natural gas inlet and a wet desulfurization gas outlet and in which the desulfurizer is an alkali-functionalized protic ionic liquid; a drying device with a gas inlet connected to the wet desulfurization gas outlet; and a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying device. The desulfurization apparatus provided by the invention uses the wet desulfurization device to remove inorganic sulfides in natural gas, uses the dry desulfurization device to remove organic sulfides in natural gas, and has an excellent desulfurization effect; and the two desulfurization devices in the desulfurization apparatus can be arranged separately, so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle.

Description

NATURAL GAS DESULFURIZATION APPARATUS TECHNICAL FIELD
The present invention pertains to the field of desulfurization and particularly relates to a natural gas desulfurization apparatus for use with an SOFC system.
BACKGROUND ART
Natural gas typically contains acid gases such as inorganic sulfides (mainly H 2S) and organic sulfides. Their presence will not only corrode the equipment, but also cause toxic damage to the SOFC stack, which will seriously affect the safety of the stack. Therefore, natural gas needs to be desulfurized and purified before entering the stack. Moreover, in order to achieve the desulfurization effect required by SOFC, a conventional desulfurization apparatus currently in use is relatively heavy and bulky and so is not convenient for installation and use on a vehicle.
SUMMARY OF THE INVENTION
The present invention provides a natural gas desulfurization apparatus. The natural gas desulfurization apparatus provided by the present invention comprises a wet desulfurization device and a dry desulfurization device and has an excellent desulfurization effect, and the two desulfurization devices can be arranged separately, so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle.
The present invention provides a natural gas desulfurization apparatus, comprising:
a wet desulfurization device, which is provided with a natural gas inlet and a wet desulfurization gas outlet, and in which the desulfurizer is an alkali-functionalized protic ionic liquid;
a drying device with a gas inlet connected to the wet desulfurization gas outlet; and
a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying  device.
The wet desulfurization device can comprise a wet desulfurization vessel for containing the alkaline-functionalized protic ionic liquid, a natural gas inlet arranged at the bottom of the wet desulfurization vessel, and a wet desulfurization gas outlet arranged at the top of the wet desulfurization vessel.
Several layers of orifice plates can be arranged in the wet desulfurization vessel, a certain predetermined distance being reserved between two adjacent layers of the orifice plates, and the orifices of two adjacent layers of the orifice plates are interlaced or offset.
The position of the bottommost layer of the orifice plates can be flush with the level of the ionic liquid contained in the wet desulfurization vessel.
A certain predetermined distance can be kept between the topmost layer of the orifice plates and the top of the wet desulfurization vessel.
The number of layers of the orifice plates can be 2 to 5.
The natural gas inlet can be provided with an inlet gas filter; and the wet desulfurization gas outlet can be provided with an outlet gas filter.
The wet desulfurization device can be further provided with an ionic liquid regeneration outlet.
The drying device can comprise a first drying unit and a second drying unit, the first drying unit can be a dryer filled with desiccant, and the second drying unit can be a dewatering filter;
In one embodiment, a gas inlet of the dryer is connected to the wet desulfurization gas outlet, a dry gas outlet of the dryer is connected to a gas inlet of the dewatering filter, and a dry gas outlet of the dewatering filter is connected to a gas inlet of the dry desulfurization device.
The dry desulfurization device can comprise a dry desulfurization vessel used for containing a dry desulfurizer, a gas inlet arranged at the bottom of the dry desulfurization vessel, and a dry desulfurization gas outlet arranged at the top of the dry desulfurization vessel.
Compared with the prior art, the present invention provides a natural gas desulfurization apparatus. The natural gas desulfurization apparatus provided by the present invention comprises a wet desulfurization device, which is provided with a natural gas inlet and a wet  desulfurization gas outlet and in which the desulfurizer is an alkali-functionalized protic ionic liquid. A drying device with a gas inlet connected to the wet desulfurization gas outlet; and a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying device. The present invention provides a composite desulfurization apparatus, which connects wet desulfurization and dry desulfurization in series. During operation of the apparatus, firstly the natural gas to be desulfurized is led into the wet desulfurization device using an alkali-functionalized protic ionic liquid (MLB-PILs) as a desulfurizer to remove inorganic sulfides represented by H 2S. The natural gas from which inorganic sulfur has been removed enters the drying device for drying and dewatering. Lastly, the dewatered natural gas enters the dry desulfurization device to remove organic sulfides to obtain a desulfurized natural gas. The desulfurization apparatus provided by the present invention uses the wet desulfurization device to remove inorganic sulfides in natural gas, uses the dry desulfurization device to remove organic sulfides in natural gas, and has an excellent desulfurization effect. The two desulfurization devices in the desulfurization apparatus can be arranged separately so that the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle.
BRIEF DESCRIPTION OF THE DRAWINGS
The drawings used in the description are briefly described below. These are just some embodiments of the present invention.
Fig. 1 is a structural schematic view of a natural gas desulfurization apparatus.
Fig. 2 is a structural schematic view of a wet desulfurization device.
Fig. 3 is a structural schematic view of an integrated adapter.
Fig. 4 is a structural schematic view of a natural gas desulfurization apparatus with two drying units.
DETAILED DESCRIPTION
Embodiments of the present invention will be described below in conjunction with the  drawings. The described embodiments are only some of the embodiments of the present invention.
The present invention provides a natural gas desulfurization apparatus, comprising:
a wet desulfurization device, which is provided with a natural gas inlet and a wet desulfurization gas outlet and in which the desulfurizer is an alkali-functionalized protic ionic liquid;
a drying device with a gas inlet connected to the wet desulfurization gas outlet; and
a dry desulfurization device with a gas inlet connected to a dry gas outlet of the drying device.
Fig. 1 is a structural schematic view of a natural gas desulfurization apparatus provided in an embodiment of the present invention. The apparatus of Fig. 1 includes a wet desulfurization device 1, a drying device 2, and a dry desulfurization device 3. Fig. 2 is a structural schematic view of a wet desulfurization device provided in an embodiment of the present invention. The device of Fig. 2 includes a natural gas inlet 11, a wet desulfurization vessel 12, an alkali-functionalized protic ionic liquid 13, an orifice plate 14, a wet desulfurization gas outlet 15, and an ionic liquid regeneration outlet 16.
The natural gas desulfurization apparatus provided by the present invention comprises a wet desulfurization device 1, a drying device 2 and a dry desulfurization device 3. The wet desulfurization device 1 is used for removing inorganic sulfides in natural gas (e.g., H 2S) . A natural gas inlet 11 and a wet desulfurization gas outlet 15 are arranged on the wet desulfurization device and the desulfurizer in the wet desulfurization device 1 is an alkali-functionalized protic ionic liquid 13, preferably a 3-diaminopropane acetic acid ( [TDMAPAH] [Ac] ) solution. The concentration of the 3-diaminopropane acetic acid solution can be 40 to 50 wt%, such as 48 wt%. The wet desulfurization device 1 comprises a wet desulfurization vessel used for containing the alkaline-functionalized protic ionic liquid 12. A natural gas inlet 11 arranged at the bottom of the wet desulfurization vessel 12 and a wet desulfurization gas outlet 15 arranged at the top of the wet desulfurization vessel 12. The included angle between the natural gas inlet 11 and the wet desulfurization gas outlet 15 is 90°. In order to prevent the ionic liquid contained in the wet desulfurization vessel 12 from overflowing due to vibration of the vehicle, several layers of orifice plates 14 are arranged in the wet desulfurization vessel 12, with a predetermined distance maintained  between two adjacent layers of the orifice plates. The orifices of two adjacent layers of the orifice plates are interlaced or offset. This can effectively block the ionic liquid from surging out and prevent the ionic liquid from entering the wet desulfurization gas outlet 15. The position of the bottommost layer of the orifice plates in the wet desulfurization vessel 12 is flush with the level of the ionic liquid 13 contained in the wet desulfurization vessel 12. This setting method can effectively prevent the ionic liquid from oscillating back and forth. A certain distance is kept between the topmost layer of the orifice plates and the top of the wet desulfurization vessel 12. The existence of this distance can reserve a certain space for the gathering of the gas separated from the liquid phase, thereby keeping the gas pressure relatively stable. The number of layers of the orifice plates 14 in the wet desulfurization vessel 12 is 2 to 5, may be 2, 3, 4 or 5.
In order to prevent the particulate matter in the natural gas from entering the ionic liquid, the natural gas inlet 11 is provided with an inlet gas filter. In order to prevent the particulate matter in the desulfurizer from escaping with the gas, the wet desulfurization gas outlet 15 is provided with an outlet gas filter. The natural gas inlet 11 is equipped with a gas inlet adapter and the wet desulfurization gas outlet 15 is equipped with a gas outlet adapter. One embodiment is equipped with an adapter and provided with a filter. The filter is not arranged separately but integrated on the adapter at the gas inlet/outlet, as shown in Fig. 3. Fig. 3 is a structural schematic view of an integrated adapter provided in an embodiment of the present invention. Fig. 3 shows an adapter body 11 and a filter element 112. The filter element 112 is arranged at an internal step of the adapter body 111, and the filter 112 is a sintered filter element. The size of the filtration pores is 0.1 to 1 μm, and may be 0.5 μm.
In an embodiment provided by the present invention, the wet desulfurization device 1 is further provided with an ionic liquid regeneration outlet 1-6. The ionic liquid regeneration outlet 1-6 is arranged at the bottom of the wet desulfurization vessel 12 and a valve is arranged on the ionic liquid regeneration outlet. In the present invention, via the ionic liquid regeneration outlet 1-6, the wet desulfurizer in a saturated absorption state can be discharged out of the wet desulfurization device 1, and then is desorbed and regenerated by such methods as heating and pressure reduction. The regenerated wet desulfurizer can be reused in the wet desulfurization device 1.
In the present invention, the drying device 2 is used for dewatering and drying the natural gas that has been desulfurized by the wet process, a gas inlet and a dry gas outlet are arranged  on the drying device, and the gas inlet of the drying device 2 is connected to a wet desulfurization gas outlet of the wet desulfurization device 1.
The drying device 2 comprises two drying units, as shown in Fig. 4. Fig. 4 is a structural schematic view of a natural gas desulfurization apparatus with two drying units provided in an embodiment of the present invention. The apparatus of Fig. 4 includes a dryer 2-1 and a dewatering filter 2-2. The drying device 2 comprises a first drying unit and a second drying unit. The first drying unit is a dryer 2-1. A gas inlet and a dry gas outlet are arranged on the dryer and the gas inlet of the dryer 2-1 is connected to the wet desulfurization gas outlet of the wet desulfurization device 1. The dryer 2-1 is internally filled with desiccant. The desiccant can include CaSO 4 and /or CaCl 2. In the present invention, the second drying unit can be a dewatering filter 2-2. A gas inlet and a dry gas outlet are arranged on the dewatering filter and the gas inlet of the dewatering filter 2-2 is connected to the dry gas outlet of the dryer 2-1.
In the present invention, the dry desulfurization device 3 is used for removing organic sulfides in natural gas after drying. A gas inlet and a dry desulfurization gas outlet are arranged on the dry desulfurization device and the gas inlet of the drying device 3 is connected to the dry gas outlet of the drying device 2. The dry desulfurization device 3 comprises a dry desulfurization vessel used for containing a dry desulfurizer, a gas inlet arranged at the bottom of the dry desulfurization vessel, and a dry desulfurization gas outlet arranged at the top of the dry desulfurization vessel. Here, the dry desulfurizer includes CuO and adjuvants, and the adjuvants include MnO and/or Al 2O 3.
The present invention provides a composite desulfurization apparatus which connects wet desulfurization and dry desulfurization in series. During operation of the apparatus, firstly the natural gas to be desulfurized is led into the wet desulfurization device using an alkali-functionalized protic ionic liquid (MLB-PILs) as a desulfurizer to remove inorganic sulfides represented by H 2S. Then the natural gas removed of inorganic sulfur enters the drying device for drying and dewatering. Lastly, the dewatered natural gas enters the dry desulfurization device to remove organic sulfides to obtain a desulfurized natural gas.
The desulfurization apparatus provided by the present invention uses the wet desulfurization device to remove inorganic sulfides in natural gas, uses the dry desulfurization device to remove organic sulfides in natural gas, and has an excellent desulfurization effect. The two desulfurization devices in the desulfurization apparatus can be arranged separately, so that  the vehicle space can be used more effectively, thereby solving to some extent the problem of difficult installation and arrangement of the desulfurization apparatus caused by the limited space of the vehicle. More specifically, the desulfurization apparatus provided by the present invention has the following advantages:
1) The alkali-functionalized protic ionic liquid is used as a desulfurizer of the wet desulfurization device. The raw materials are easily available and cheap and adopt simple synthesis processes.
2) For example, a 48wt%3-diaminopropane acetic acid solution is used as a desulfurizer of the wet desulfurization device. This is superior to other H 2S absorbents in terms of absorbing capacity, viscosity, and cost, and is more suitable to be used as a desulfurizer of natural gas.
3) The wet desulfurizer in a saturated absorption state can be regenerated by such methods as heating and pressure reduction. Compared with a fresh absorbent, the absorbing capacity of the regenerated absorbent is reduced by about 7.5%only, so it can be reused.
4) Several layers of orifice plates can be arranged in the wet desulfurization device to effectively prevent violent oscillation of the ionic liquid and effectively stop the solution from entering the upstream pipeline along with the gas.
5) Due to the existence of a prepositive wet desulfurization device, the design size of the dry desulfurization device can be reduced significantly and can ensure one year of operation of the vehicle though the volume is reduced remarkably.
6) The wet desulfurization device and the dry desulfurization device can be arranged separately, so that the vehicle space can be used more efficiently and more space can be saved for other components.
Above are merely some implementations of the present invention. Various changes and modifications may be made without departing from the scope of protection of the invention.

Claims (10)

  1. A natural gas desulfurization apparatus, comprising:
    a wet desulfurization device having a natural gas inlet and a wet desulfurization gas outlet, and containing an alkali-functionalized protic ionic liquid as a desulfurizer;
    a drying device having a gas inlet connected to the wet desulfurization gas outlet, and a dry gas outlet; and
    a dry desulfurization device having a gas inlet connected to the dry gas outlet of the drying device.
  2. The natural gas desulfurization apparatus according to claim 1, wherein the wet desulfurization device comprises:
    a wet desulfurization vessel containing the alkaline-functionalized protic ionic liquid;
    the natural gas inlet arranged at the bottom of the wet desulfurization vessel; and
    the wet desulfurization gas outlet arranged at the top of the wet desulfurization vessel.
  3. The natural gas desulfurization apparatus according to claim 2, wherein:
    layers of orifice plates are arranged in the wet desulfurization vessel;
    a predetermined distance is defined between two adjacent layers of orifice plates, and
    the orifices of two adjacent layers of the orifice plates are offset.
  4. The natural gas desulfurization apparatus according to claim 3, wherein the position of a bottommost layer of the orifice plates is flush with the level of the ionic liquid contained in the wet desulfurization vessel.
  5. The natural gas desulfurization apparatus according to claim 3 or 4, wherein a predetermined distance is defined between the topmost layer of the orifice plates and the top of the wet desulfurization vessel.
  6. The natural gas desulfurization apparatus according to claim 3, 4, or 5, wherein the  number of layers of the orifice plates is 2 to 5.
  7. The natural gas desulfurization apparatus according to any preceding claim, wherein the natural gas inlet is provided with an inlet gas filter; and the wet desulfurization gas outlet is provided with an outlet gas filter.
  8. The natural gas desulfurization apparatus according to any preceding claim, wherein the wet desulfurization device is further provided with an ionic liquid regeneration outlet.
  9. The natural gas desulfurization apparatus according to any preceding claim, wherein:
    the drying device comprises a first drying unit and a second drying unit;
    the first drying unit is a dryer filled with desiccant, and the second drying unit is a dewatering filter;
    a gas inlet of the dryer is connected to the wet desulfurization gas outlet;
    a dry gas outlet of the dryer is connected to a gas inlet of the dewatering filter; and
    a dry gas outlet of the dewatering filter is connected to a gas inlet of the dry desulfurization device.
  10. The natural gas desulfurization apparatus according to any preceding claim, wherein the dry desulfurization device comprises:
    a dry desulfurization vessel used for containing a dry desulfurizer;
    a gas inlet arranged at the bottom of the dry desulfurization vessel; and
    a dry desulfurization gas outlet arranged at the top of the dry desulfurization vessel.
PCT/CN2021/102847 2020-06-29 2021-06-28 Natural gas desulfurization apparatus WO2022001985A1 (en)

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CN203820739U (en) * 2014-04-25 2014-09-10 桑德环境资源股份有限公司 Biogas treatment system
CN204265720U (en) * 2014-11-20 2015-04-15 中国石油大学(北京) For pretreatment system and the film separating system of high sulfur-bearing and carbon dioxide containing gas
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