CN107487766A - A kind of three-dimensional porous carbon material of Heteroatom doping and preparation method thereof - Google Patents
A kind of three-dimensional porous carbon material of Heteroatom doping and preparation method thereof Download PDFInfo
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Abstract
The invention provides a kind of preparation method of the three-dimensional porous carbon material of Heteroatom doping, belong to carbon material preparation field, the present invention mixes after gluconate is carbonized in advance with element polymer, it is carbonized again, obtain carbonized product, after carbonized product mixes with inorganic acid, the three-dimensional porous carbon material of Heteroatom doping is obtained.This method, as raw material precursor, after doped chemical macromolecule, obtains the carbon material of Heteroatom doping, preparation method is simple, and cost is cheap, and pollution-free using single raw materials of glucose hydrochlorate.In the present invention, gluconate has many carbon oxygen elements, can discharge carbon dioxide during carbonization in advance, carbon material is expanded pore-creating, element polymer is the high polymer material containing hetero atom nitrogen, phosphorus etc., and the three-dimensional porous carbon material of different Heteroatom doping amounts can be made by control element macromolecule.
Description
Technical field
The present invention relates to porous carbon materials preparation field, more particularly to a kind of three-dimensional porous carbon material of Heteroatom doping and its
Preparation method.
Background technology
With the consumption of the energy and the continuous deterioration of environment, storage and the transformation technology of new energy receive extensive weight
Depending on, such as the technology such as lithium ion battery, fuel cell and ultracapacitor.In these new energy technologies, as carrier and urge
The C-base composte material of agent plays the effect of key.Because the carbon material containing metal is high, stably there is cost is prepared
Property lack and the shortcomings of resistance to acids and bases difference, and the Heteroatom doping carbon material without metal overcomes these shortcomings.Three-dimensional multistage is more
Hole carbon nanomaterial, because its hole is various, specific surface area is big, and more reaction channels are provided for reaction medium, electronics etc.,
Catalytic efficiency can be greatly improved；Other carbon material also has many merits such as stable chemical performance, good conductivity.Therefore, three
The carbon nanomaterial for tieing up porous Heteroatom doping has a wide range of applications in new energy and adsorbing domain.
According to the species source of presoma or carrier, doping carbon nanomaterial mainly has two classes：First, carbon material is as load
Body, such as graphene, CNT and commercial activated carbons.Generally, the preparation of this kind of material is related to precursor synthesis, Ran Houshui
Heat or the equal reaction of High Temperature Gas introduce small molecule containing hetero atom and obtain the carbon material of Heteroatom doping, preparation method is complicated, into
This is higher.Second, biological material presoma carbon material, be mainly derived from the organism of nature, as timber, plant leaf,
Rice etc., reduces production cost.But the catalyst of biomass presoma is generally required carbonization, activation or obtained using template
Obtain loose structure, because biomass thermal stability is poor, substantial amounts of component volatilization.Therefore, prepared by biomass presoma carbon material
Journey easily causes pollution, and hetero atom structures controllability is not strong, is unfavorable for theoretical research and large-scale production.
The content of the invention
In view of this, it is an object of the invention to provide a kind of three-dimensional porous carbon material of Heteroatom doping and its preparation side
Method, using single raw materials of glucose hydrochlorate as raw material precursor, after element polymer adulterates, obtain Heteroatom doping
Three-dimensional porous carbon material, preparation method is simple, and cost is cheap, pollution-free.
In order to realize foregoing invention purpose, the present invention provides following technical scheme：
A kind of preparation method of the three-dimensional porous carbon material of Heteroatom doping, comprises the following steps：
(1) gluconate is carbonized in advance, obtains pre- carbide；
(2) the pre- carbide that the step (1) obtains is mixed with element polymer, obtains doped products；
(3) doped products that the step (2) obtains are carbonized, obtain carbonized product；
(4) after the carbonized product that the step (3) obtains is mixed with inorganic acid, the three-dimensional porous carbon of Heteroatom doping is obtained
Material.
Preferably, gluconate includes calcium gluconate and/or sodium gluconate in the step (1).
Preferably, the temperature being carbonized in advance in the step (1) is 100~600 DEG C, time of the pre- carbonization for 0.1~
3h。
Preferably, the mass ratio of pre- carbide and element polymer is 100 in the step (2)：2~20.
Preferably, the element polymer includes one kind in polypyrrole, polyaniline, polyamide, polyurethane and polyphosphazene
Or a variety of mixture.
Preferably, the element polymer is mixed in the form of element polymer solution with pre- carbide, and the element is high
The concentration of molecular solution is 0.01~0.1g/mL.
Preferably, the temperature of carbonization is 400~1000 DEG C in the step (3), and the time of the carbonization is 0.2~6h.
Preferably, inorganic acid includes hydrochloric acid or sulfuric acid in the step (4).
Present invention also offers the three-dimensional porous carbon material of Heteroatom doping made from preparation method described in above-mentioned technical proposal,
The heteroatomic doping is calculated as 0.1~5% with weight/mass percentage composition, and the hetero atom includes N, P and B.
The invention provides a kind of preparation method of the three-dimensional porous carbon material of Heteroatom doping, and gluconate is in advance after carbonization
Mix, then be carbonized with element polymer, obtain carbonized product, after carbonized product mixes with inorganic acid, obtain hetero atom and mix
Miscellaneous three-dimensional porous carbon material.This method uses single raw materials of glucose hydrochlorate as raw material precursor, by doped chemical high score
After son, the carbon material of Heteroatom doping is obtained, preparation method is simple, and cost is cheap, and pollution-free.In the present invention, gluconic acid
Salt has many carbon oxygen elements, can discharge carbon dioxide during carbonization in advance, carbon material is expanded pore-creating；Element polymer be containing
The high polymer material of hetero atom nitrogen, phosphorus, oxygen etc., different miscellaneous originals can be made by the high molecular species of control element and dosage
The three-dimensional porous carbon material of sub, different dopings, realize the controllability of doped chemical species and doping.
Brief description of the drawings
The present invention is further detailed explanation with reference to the accompanying drawings and detailed description.
Fig. 1 is the flow chart that the embodiment of the present invention prepares the three-dimensional porous carbon material of Heteroatom doping；
Fig. 2 is the three-dimensional porous carbon material optical detection photo of Heteroatom doping made from the embodiment of the present invention 1；
Fig. 3 is the three-dimensional porous carbon material ESEM of Heteroatom doping made from the embodiment of the present invention 1；
Fig. 4 be the three-dimensional porous carbon material of Heteroatom doping made from the embodiment of the present invention 1 nitrogen adsorption desorption curve with
And graph of pore diameter distribution, wherein being the nitrogen adsorption desorption curve of the three-dimensional porous carbon material of a Heteroatom dopings, b is Heteroatom doping
The graph of pore diameter distribution of three-dimensional porous carbon material.
Embodiment
The invention provides a kind of preparation method of the three-dimensional porous carbon material of Heteroatom doping, comprise the following steps：
(1) gluconate is carbonized in advance, obtains pre- carbide；
(2) the pre- carbide that the step (1) obtains is mixed with element polymer, obtains doped products；
(3) doped products that the step (2) obtains are carbonized, obtain carbonized product；
(4) carbonized product that the step (3) obtains is mixed with inorganic acid, obtains the three-dimensional porous carbon materials of Heteroatom doping
Material.
Gluconate is carbonized by the present invention in advance, obtains pre- carbide.In the present invention, the gluconate bag
Include calcium gluconate and/or sodium gluconate.In the present invention, when the gluconate includes calcium gluconate and glucose
During sour sodium, there is no special restriction to the mass ratio of the calcium gluconate and sodium gluconate, using the Portugal of any mass ratio
The mixture of grape Calciofon and sodium gluconate.In the present invention, the gluconate has many carbon oxygen elements, pre- carbonization
When can discharge carbon dioxide, make carbon material expand pore-creating.In the present invention, the particle diameter of the gluconate is preferably 100
~300 mesh, more preferably 150~200 mesh.Present invention preferably employs the mode of grinding to reach the particle diameter, and the grinding is preferred
Carried out in agate mortar；The time of the grinding is preferably 10~20min, more preferably 15min.The present invention is to the grape
The source of sugar lime does not have any special restriction, using commercial goods well known to those skilled in the art.
In the present invention, the temperature of the pre- carbonization is preferably 100~600 DEG C, more preferably 200~500 DEG C, most 300
~400 DEG C；The time of the pre- carbonization is preferably 0.1~3h, more preferably 0.5~2.5h, most preferably 1.5~2.0h.
In the present invention, the pre- carbonization is carried out preferably in air atmosphere.In the present invention, the pre- carbonization can be by gluconate
In carbon oxygen element oxidation, discharge carbon dioxide, make carbon material expand pore-creating.
The present invention does not have special restriction to the device of the pre- carbonization, is filled using carbonization well known to those skilled in the art
Put, in the present invention, it is preferred to be Muffle furnace.The mould of the invention that use that is carbonized in advance to gluconate progress does not have
Special restriction, using carbonization mould well known to those skilled in the art, in the present invention, it is preferred to be corundum crucible.This
Invention according to carbonization mould of different shapes preferably by being made the three-dimensional porous carbon material of Heteroatom doping of different shapes.
After the completion of pre- carbonization, the present invention obtains the pre- carbide preferably through being cooled to room temperature.The present invention is to described cold
But mode does not have special restriction, using the type of cooling well known to those skilled in the art, is preferably in the present invention
Natural cooling.
After obtaining pre- carbide, the present invention mixes the pre- carbide with element polymer, obtains doped products.At this
In invention, the mass ratio of the pre- carbide and element polymer is preferably 100：2~20, more preferably 100：5~15, it is optimal
Elect 100 as：10.In the present invention, the element polymer is containing heteroatomic high polymer material, contains the miscellaneous original such as nitrogen, phosphorus, oxygen
Son, different hetero atoms, the three-dimensional porous carbon of different dopings can be made by the high molecular species of control element and dosage
Material.
In the present invention, the element polymer preferably includes polypyrrole, polyaniline, polyamide, polyurethane and polyphosphazene
In one or more mixtures.In the present invention, the element polymer preferably in the form of element polymer solution with
Pre- carbide mixing, the concentration of the element polymer solution is preferably 0.01~0.1g/mL, more preferably 0.02~0.08g/
mL；The solvent of the element polymer solution is preferably water or ethanol.
The present invention does not have special restriction to the charging sequence of the pre- carbide and element polymer, will preferably be carbonized in advance
Thing is added in element polymer.The present invention does not have special restriction to the concrete mode of the mixing, using art technology
Hybrid mode known to personnel.In the present invention, it is preferred to be ultrasonic mixing, the ultrasound can make element polymer abundant
It is uniformly blended into pre- carbide.In the present invention, the ultrasonic power is preferably 30~50 KHzs, more preferably 40,000
Hertz；The ultrasonic time is preferably 0.5~3h, more preferably 1.5~2h；The ultrasonic temperature is preferably room temperature, no
Need extra heating or cooling.
After the completion of ultrasound, preferred pair ultrasound system of the present invention is aged and dried successively, obtains doped products.In this hair
In bright, the time of the ageing is preferably 3~10h, more preferably 6~8h；The temperature of the ageing is preferably room temperature, it is not necessary to
Extra heating or cooling.In the present invention, it is described ageing enable to element polymer further it is full and uniform be mixed into it is pre-
In carbide.
After the completion of ageing, preferred pair ageing system of the present invention is dried.The present invention does not have to the concrete mode of the drying
There is special restriction, using drying mode well known to those skilled in the art, in the present invention, it is preferred to be drying, it is described
The temperature of drying is preferably 30~105 DEG C, more preferably 50~100 DEG C, most preferably 80~90 DEG C；The time of the drying is excellent
Elect 2~6 hours, more preferably 4~5h as.
After obtaining doped products, the doped products are carbonized by the present invention, obtain carbonized product.In the present invention,
The temperature of the carbonization is preferably 400~1000 DEG C, more preferably 600~900 DEG C, most preferably 700~800 DEG C；The carbon
The time of change is preferably 0.2~6h, more preferably 1~4h, most preferably 2~3h.In the present invention, doped products are warming up to carbon
Heating rate is preferably 1~10 DEG C/min when changing temperature, more preferably 4~8 DEG C/min, most preferably 5~6 DEG C/min.At this
In invention, the carbonization is carried out in inert gas, and the present invention does not have special restriction to the species of the inert gas, is used
Inert gas well known to those skilled in the art, it is specific such as argon gas.The present invention is not special to the device of the carbonization
Restriction, using carbonizing plant well known to those skilled in the art, in the present invention, it is preferred to be Muffle furnace.
After the completion of carbonization, the product for the completion that is carbonized preferably is cooled to room temperature and obtains carbonized product by the present invention.The present invention is right
The mode of the cooling does not have special restriction, using the type of cooling well known to those skilled in the art, in the present invention
Preferably natural cooling.
After obtaining carbonized product, the present invention mixes the carbonized product with inorganic acid, and it is three-dimensional more to obtain Heteroatom doping
Hole carbon material.In the present invention, the inorganic acid preferably includes hydrochloric acid or sulfuric acid.In the present invention, the effect of the inorganic acid is
Remove the metallic element in carbonized product, such as calcium or sodium.In the present invention, the concentration of the inorganic acid be preferably 0.05~
1M, more preferably 0.2~0.6M；The present invention does not have special restriction to the mass ratio of the carbonized product and inorganic acid, can
Ensure that inorganic acid soak crosses carbonized product.
The present invention does not have special restriction to the feed way of the carbonized product and inorganic acid, using people in the art
Carbonized product, in embodiments of the present invention, is preferably added in inorganic acid by charging sequence known to member.
The present invention does not have any special restriction to the concrete mode of the mixing, and use is well known to those skilled in the art
Hybrid mode.In embodiments of the present invention, the mixing preferably includes ultrasound and immersion successively.In the present invention, institute
The power for stating ultrasound is preferably 30~50 KHzs, more preferably 40 KHzs；The ultrasonic time is preferably 0.5~2h,
More preferably 1~1.5h；The ultrasonic temperature is preferably room temperature, it is not necessary to extra heating or cooling.In the present invention, institute
Stating ultrasound can be such that inorganic acid is fully reacted with the metallic element in carbonized product, so that metallic element is more thorough with clearing.
After the completion of ultrasound, the present invention is preferably soaked the system that ultrasound obtains.In the present invention, the temperature of the immersion
Degree is preferably 30~100 DEG C, more preferably 50~80 DEG C, most preferably 60~70 DEG C；The time of the immersion is preferably 1~
20h, more preferably 5~10h.In the present invention, the immersion is able to ensure that inorganic acid and the metallic element in carbonized product are abundant
Reaction, so that metallic element is more thorough with clearing.
After the completion of mixing, mixed system is preferably carried out separation of solid and liquid, washs and be dried to obtain hetero atom by the present invention successively
Adulterate three-dimensional porous carbon material.Concrete operations of the present invention to the separation of solid and liquid do not have special restriction, using this area skill
Solid-liquid separation method known to art personnel, in the present invention, it is preferred to filter.
After the completion of separation of solid and liquid, the solid product that the present invention preferably obtains separation of solid and liquid is washed.In the present invention,
The detergent used that washs is preferably water.It is special that the present invention does not have to the number of the washing and the dosage of detergent
Limit, using detergent well known to those skilled in the art, solid product can be washed to neutrality.
After the completion of washing, preferably washed product is dried by the present invention, obtains the three-dimensional porous carbon material of Heteroatom doping.
The present invention does not have special restriction to the concrete mode of the drying, is using drying mode well known to those skilled in the art
Can, specifically, as dried.The present invention does not have special restriction to time of the drying, temperature, using those skilled in the art
It is well known, remove washed product in moisture, be dried to constant weight.
Present invention also offers the three-dimensional porous carbon material of Heteroatom doping made from preparation method described in above-mentioned technical proposal,
The hetero atom includes N, P and B, and the heteroatomic doping is preferably 0.1~5% in terms of weight/mass percentage composition, more preferably
For 0.6~4%, most preferably 3.4%.
In the present invention, micropore, mesoporous and macropore coexist in the three-dimensional porous carbon material of the Heteroatom doping.
To three-dimensional porous carbon material of Heteroatom doping provided by the invention and preparation method thereof and answered with reference to embodiment
With being described in detail, but they can not be interpreted as limiting the scope of the present invention.
Fig. 1 is the flow chart that the embodiment of the present invention prepares the three-dimensional porous carbon material of Heteroatom doping, and gluconate is carried out
Pre- carbonization, obtains pre- carbide, pre- carbide mixed with element polymer after by being aged, then mixed after being carbonized with inorganic acid
Close, the three-dimensional porous carbon material of Heteroatom doping is obtained by drying.
Embodiment 1
Calcium gluconate is ground 10 minutes in agate mortar, the calcium gluconate that particle diameter is 200 mesh is obtained, then puts
In cube corundum crucible, under Muffle furnace, air atmosphere, taken out after 200 DEG C of pre- carbonization 3h, natural cooling.It will obtain
Pre- carbide 30g soaking at room temperature concentration be 0.1g/mL polyaniline solutions 80mL in, the ultrasonic 0.5h under 40 KHzs,
It is aged 3h and dries 6h after 30 DEG C.Again under inert gas shielding, 400 DEG C of progress carbon are warming up to 1 DEG C/min programming rate
Change 6h, naturally cool to after room temperature and obtain carbonized product, carbonized product and 50mL, the hydrochloric acid that concentration is 0.4M are under 40 KHzs
Ultrasonic 2h, then 20h is soaked at 30 DEG C, obtain the miscellaneous original of cubic by filtering, being washed to neutrality, be dried to constant weight successively
Son adulterates three-dimensional porous carbon material.
Hetero atom species and Heteroatom doping amount are carried out to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 1
Detection, the hetero atom for measuring doping are nitrogen, and heteroatomic doping is 3.4%.
Optical detection, testing result such as Fig. 2 institutes are carried out to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 1
Show, as seen from Figure 2, the obtained three-dimensional porous carbon material of Heteroatom doping is cubic, is a kind of bulk of self-supporting
Structure.
Electronic Speculum detection, testing result such as Fig. 3 are scanned to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 1
It is shown, as seen from Figure 3, the tool that the obtained three-dimensional porous carbon material of Heteroatom doping is self-assembled into by numerous nanoscale carbon plates
There is the three-dimensional porous structure of a large amount of tens microns of macropore.
The specific surface area of the three-dimensional porous carbon material of Heteroatom doping made from embodiment 1 is surveyed using nitrogen adsorption method
Examination, shown in nitrogen adsorption result result such as Fig. 4 (a), hole is carried out to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 1
Footpath distribution tests, as a result as shown in Fig. 4 (b), Heteroatom doping made from embodiment 1 is shown it can be seen from Fig. 4 (a) and (b)
Three-dimensional porous carbon material is micro-, is situated between, the hierarchical porous structure of macropore, specific surface area 1609.4m2/ g, the average hole of nitrogen adsorption
Footpath is 3.6nm.
Embodiment 2
Sodium gluconate is ground 20 minutes in agate mortar, the calcium gluconate that particle diameter is 300 mesh is obtained, then puts
In round corundum crucible, under Muffle furnace, air atmosphere, taken out after 600 DEG C of pre- carbonization 0.1h, natural cooling.Will
To pre- carbide 40g soaking at room temperature concentration be 0.01 polyphosphazene solution 100mL in, ultrasonic 3h, old under 30 KHzs
Change 10h and dry 2h after 105 DEG C.Again under inert gas shielding, 1000 DEG C of progress are warming up to 10 DEG C/min programming rate
Be carbonized 0.2h, naturally cools to after room temperature and obtains carbonized product, and carbonized product and 80mL, the hydrochloric acid that concentration is 0.4M are in 50 kilo hertzs
Ultrasonic 0.5h under hereby, then 3h is soaked at 100 DEG C, obtain the miscellaneous of circle by filtering, being washed to neutrality, be dried to constant weight successively
Atom doped three-dimensional porous carbon material.
Hetero atom species and Heteroatom doping amount are carried out to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 2
Detection, the hetero atom for measuring doping are nitrogen and phosphorus, and heteroatomic doping is always 0.6%.
After testing, the three-dimensional porous carbon material of Heteroatom doping made from embodiment 2 is micro-, is situated between, the hierarchical porous structure of macropore,
Specific surface area is 1310m2/ g, the average pore size of nitrogen adsorption is 3.7nm.
Embodiment 3
Calcium gluconate is ground 15 minutes in agate mortar, the calcium gluconate that particle diameter is 100 mesh is obtained, then puts
In cylinder corundum crucible, under Muffle furnace, air atmosphere, taken out after 500 DEG C of pre- carbonization 2h, natural cooling.It will obtain
Pre- carbide 50g soaking at room temperature concentration be 0.05g/mL polypyrrole solution 100mL in, the ultrasonic 1h under 50 KHzs,
It is aged 8h and dries 5h after 90 DEG C.Again under inert gas shielding, 800 DEG C of progress carbon are warming up to 8 DEG C/min programming rate
Change 2h, naturally cool to after room temperature and obtain carbonized product, carbonized product and 100mL, the hydrochloric acid that concentration is 0.5M are in 30 KHzs
Lower ultrasonic 1.5h, then 10h is soaked at 80 DEG C, obtain the miscellaneous of cylinder by filtering, being washed to neutrality, be dried to constant weight successively
Atom doped three-dimensional porous carbon material.
Hetero atom species and Heteroatom doping amount are carried out to the three-dimensional porous carbon material of Heteroatom doping made from embodiment 3
Detection, the hetero atom for measuring doping are nitrogen, and heteroatomic doping is 4%.
After testing, the three-dimensional porous carbon material of Heteroatom doping made from embodiment 3 is micro-, is situated between, the hierarchical porous structure of macropore,
Specific surface area is 1276m2/ g, the average pore size of nitrogen adsorption is 3.8nm.
Described above is only the preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, under the premise without departing from the principles of the invention, some improvements and modifications can also be made, these improvements and modifications also should
It is considered as protection scope of the present invention.
Claims (9)
1. a kind of preparation method of the three-dimensional porous carbon material of Heteroatom doping, comprises the following steps：
(1) gluconate is carbonized in advance, obtains pre- carbide；
(2) the pre- carbide that the step (1) obtains is mixed with element polymer, obtains doped products；
(3) doped products that the step (2) obtains are carbonized, obtain carbonized product；
(4) carbonized product that the step (3) obtains is mixed with inorganic acid, obtains the three-dimensional porous carbon material of Heteroatom doping.
2. preparation method according to claim 1, it is characterised in that gluconate includes grape in the step (1)
Calciofon and/or sodium gluconate.
3. preparation method according to claim 1 or 2, it is characterised in that the temperature being carbonized in advance in the step (1) is
100~600 DEG C, the time of the pre- carbonization is 0.1~3h.
4. preparation method according to claim 1, it is characterised in that pre- carbide and element high score in the step (2)
The mass ratio of son is 100：2~20.
5. the preparation method according to claim 1 or 4, it is characterised in that the element polymer includes polypyrrole, polyphenyl
One or more mixtures in amine, polyamide, polyurethane and polyphosphazene.
6. preparation method according to claim 5, it is characterised in that the element polymer is with element polymer solution
Form mixes with pre- carbide, and the concentration of the element polymer solution is 0.01~0.1g/mL.
7. preparation method according to claim 1, it is characterised in that in the step (3) temperature of carbonization for 400~
1000 DEG C, the time of the carbonization is 0.2~6h.
8. preparation method according to claim 1, it is characterised in that inorganic acid includes hydrochloric acid or sulphur in the step (4)
Acid.
9. the three-dimensional porous carbon material of Heteroatom doping made from preparation method described in claim 1~8 any one, the miscellaneous original
The doping of son is calculated as 0.1~5% with weight/mass percentage composition, and the hetero atom includes N, P and B.
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| CN110182781A (en) * | 2019-05-24 | 2019-08-30 | 宿州学院 | A kind of preparation method of supercapacitor three-dimensional framework charcoal nanometer sheet |
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| CN115072698A (en) * | 2022-05-09 | 2022-09-20 | 中国空间技术研究院 | Heteroatom-doped aperture-controllable two-dimensional carbon material and preparation method thereof |
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| CN110182781A (en) * | 2019-05-24 | 2019-08-30 | 宿州学院 | A kind of preparation method of supercapacitor three-dimensional framework charcoal nanometer sheet |
| CN113697783A (en) * | 2021-08-03 | 2021-11-26 | 盐城工学院 | Porous g-C3N4Preparation method and application of nano-sheet |
| CN115072698A (en) * | 2022-05-09 | 2022-09-20 | 中国空间技术研究院 | Heteroatom-doped aperture-controllable two-dimensional carbon material and preparation method thereof |
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