CN106784871A - A kind of Preparation method and use of nitrogen-doped carbon area load mononuclear catalyst - Google Patents
A kind of Preparation method and use of nitrogen-doped carbon area load mononuclear catalyst Download PDFInfo
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- CN106784871A CN106784871A CN201611035644.XA CN201611035644A CN106784871A CN 106784871 A CN106784871 A CN 106784871A CN 201611035644 A CN201611035644 A CN 201611035644A CN 106784871 A CN106784871 A CN 106784871A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/96—Carbon-based electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention discloses a kind of Preparation method and use of nitrogen-doped carbon area load mononuclear catalyst; the method is using infusion process in silica surface carrying transition metal salt; it is dispersed in ethylenediamine and carbon tetrachloride solution after drying; reflow treatment; gained black thing is after the roasting carbonization of protective atmosphere high temperature; silica is removed with hydrofluoric acid, the mononuclear catalyst of nitrogen-doped carbon area load is obtained final product（M/NC, M=Fe, Co, Ni, Cu）.Prepared catalyst has specific surface area higher, activity higher, higher stability.The method composition is controllable, and nanostructured is controllable, for the hydrogen reduction electrocatalysis material of high-specific surface area and good durability provides very big possibility.The method is simple and easy to apply, with low cost, and fabulous catalytic performance is showed in electrochemical oxygen reduction reaction, with good prospects for commercial application.
Description
Technical field
The present invention relates to a kind of Preparation method and use of nitrogen-doped carbon area load mononuclear catalyst.
Background technology
Energy problem is one of 21 century maximum problem, is the important substance basis of economic growth and social development.Should
The energy crisis caused to conventional fossil fuel consumption and the method for environmental problem mainly have two kinds：One is improving fossil combustion
Material utilization ratio, delays fuel to exhaust time, short-term relief energy shortage；The second is Renewable Energy Development technology is explored, from
Fundamentally release the dependence to fossil fuel.With second industrial revolution, the mankind march toward Electrification Age, the integration of electric energy with
Using particularly critical.With increasing and expanding economy for population, energy demand is increasing.Increasing scientific researcher
Spared no effort to find sustainable energy equipment, such as fuel cell, solar cell, metal-air battery, lithium ion
Battery, ultracapacitor etc..Compared to conventional heat engines, fuel cell is a kind of high working efficiency, environmentally friendly, response speed
The fast novel power generation device of degree, chemical energy directly can be converted into electric energy by it, and efficiency is very high, therefore it turns into the main of 21 century
The energy has been trend of the times, and because not limited by Carnot cycle, its energy conversion efficiency is in 45%~60%, and thermal power generation and core
The efficiency of electricity is about 30%~40%.Fuel cell is of great interest as environmentally friendly energy device.But
During fuel cell realizes commercial applications, one of greatest problem for running into is exactly that the catalyst of Cathodic oxygen reduction is asked
Topic.At present, the difficult point for overcoming needed for fuel cell development essentially consists in the catalytic efficiency for improving cathode material.And with high capacity amount
Commercial catalysts based on Pt/C, because noble metal reserves are rare, price is high, promote people actively to find exploitation excellent performance
And noble metal alternative catalysts with low cost.With Fe, Co, Ni are the non-noble transition metal of representative, because its have it is unsaturated
3d electron orbits, are regulated and controled by the reasonable design to its structure/composition etc., are expected to replace hair of the noble metal in electrochemical catalysis
Exhibition and application.
The present invention is for the problem for existing, there is provided a kind of nitrogen-doped carbon area load mononuclear catalyst, and this is urged
Agent is used for fuel battery negative pole redox reactions.The catalyst in the basic conditions, shows superior catalysis activity, steady
Qualitative and methanol tolerance ability.
The content of the invention
Present invention aim at, there is provided a kind of preparation method and use of nitrogen-doped carbon area load mononuclear catalyst
On the way.The method, in silica surface carrying transition metal salt, ethylenediamine and carbon tetrachloride is dispersed in after drying using infusion process
In solution, reflow treatment, gained black thing removes silica, i.e., after the roasting carbonization of protective atmosphere high temperature with hydrofluoric acid
Obtain the mononuclear catalyst (M/NC, M=Fe, Co, Ni, Cu) of nitrogen-doped carbon area load.Prepared catalyst have compared with
Specific surface area, activity higher, higher stability high.The method is controllable for synthetic ingredient, and nanostructured is controllable, is ratio high
The hydrogen reduction electrocatalysis material of surface area and good durability provides very big possibility.The method is simple and easy to apply, into
This is cheap, fabulous catalytic performance is showed in electrochemical oxygen reduction reaction, with good prospects for commercial application.
A kind of preparation method of nitrogen-doped carbon area load mononuclear catalyst of the present invention, follow these steps into
OK：
A, infusion process：It is iron chloride, ferric acetyl acetonade, copper chloride, chlorine in 0.5-3g silica surfaces loading metal-salt
Change nickel or cobalt chloride；
B, the silica of step a impregnating metal salt is dispersed in ethylenediamine and tetrachloro after 100-150 DEG C of drying of temperature
Change in carbon mixed liquor, in 60-100 DEG C of reflow treatment 6-10h of temperature, obtain mixture；
C, the mixture that step b is obtained is calcined 3-8h in nitrogen atmosphere, silica is removed with hydrofluoric acid；
D, the product for obtaining step c washing drying, obtain final product the mononuclear catalyst of nitrogen-doped carbon area load.
Silica is porous silica or nano SiO 2 particle in step a.
The purposes of the nitrogen-doped carbon area load mononuclear catalyst that methods described is obtained, by the catalyst preparation into electricity
Pole, for the purposes in catalytic oxygen reduction reaction.
A kind of Preparation method and use of nitrogen-doped carbon area load mononuclear catalyst of the present invention, infusion process
In silica surface carrying transition metal salt, it is dispersed in ethylenediamine and carbon tetrachloride solution after drying, reflow treatment, gained
Black thing removes silica after the roasting carbonization of protective atmosphere high temperature with hydrofluoric acid or strong base solution, obtains final product nitrogen-doped carbon
The scattered nitrogen complex metal of monokaryon of area load.The characteristics of the method is：Prepare nitrogen-doped carbon area load monokaryon
Metallic catalyst, metal forms complex and is dispersed in nitrogen-doped carbon surface with nitrogen in the catalyst, and the nitrogen content of doping is higher.
The metal of load is one or more in the transition metal such as Fe, Co, Ni, Cu, by the catalyst preparation into electrode, for being catalyzed
Redox reactions.Reaction mass used is the conventional raw material of industry, facilitates, is easy to get, inexpensive.
Can not only obtain in the basic conditions, showing the catalysis more excellent than business Pt/C (20%) by the method
ORR activity, stability and methanol tolerance ability, and process conditions are simple, are convenient for scale and continuously produce.
Compared with existing technique, the method for the invention has obvious different：
1. no matter a kind of nitrogen-doped carbon area load mononuclear catalyst that method of the present invention is obtained is in catalysis
Level higher has been reached in activity, stability and methanol tolerance ability.
2. nitrogen-doped carbon area load mononuclear catalyst is prepared, and metal forms complex and divides with nitrogen in the catalyst
Nitrogen-doped carbon surface is dispersed in, the nitrogen content of doping is higher.
3. nitrogen-doped carbon area load mononuclear catalyst is prepared, and the metal of load is Fe, Co, Ni, Cu, and this is catalyzed
Agent is prepared into electrode, for catalytic oxygen reduction reaction.
4. the raw material used by the method for the invention is the conventional industrial goods being easy to get.
Brief description of the drawings
Fig. 1 is the Fe/NC-10 catalyst X-ray synchrotron radiation figures of preparation in the embodiment of the present invention 1, and wherein a is contrast material
Material iron foil；B is catalyst Fe/NC-10.
Fig. 2 is the nitrogen-doped carbon area load iron catalyst N1s x-ray photoelectron power spectrums of preparation in the embodiment of the present invention 1
Figure, wherein a is NC；B is Fe/NC-1；C is Fe/NC-5；D is Fe/NC-10；E is Fe/NC-15.
Fig. 3 is the rotating disk electrode (r.d.e) polarization of the nitrogen-doped carbon area load iron catalyst of preparation in the embodiment of the present invention 1
Curve map, disc rotation speed is 1600rpm, and wherein a is NC；B is Fe/NC-1；C is Fe/NC-5；D is Fe/NC-10；E is Fe/
NC-15；F is Pt/C (20%).
Fig. 4 is the stability and methanol tolerance energy of the Fe/NC-10 catalytic oxygen reduction reactions of preparation in the embodiment of the present invention 1
Power is tested, and reaction potential is -0.2V (silver/silver chloride reference electrode), and methyl alcohol addition concentration is 0.5mol/L, and wherein a is Fe/
NC-10；B is Pt/C (20%).
Fig. 5 is the rotating circular disk of the nitrogen-doped carbon area load metallic catalyst of preparation in the embodiment of the present invention 2,3,4,5
Electrode polarization curve map, disc rotation speed is 1600rpm, and wherein a is Ni/NC-10；B is Cu/NC-10；C is Co/NC-10；D is
Fe-2/NC-5。
Specific embodiment
Below by specific embodiment, the invention will be further described：
Embodiment 1
Catalyst preparation
A, infusion process：In 1g porous silica area load iron chloride；
B, by step a dipping iron chloride silica be dispersed in 8.7g ethylenediamines and tetrachloro after 110 DEG C of dryings of temperature
Change in carbon mixed liquor, in 90 DEG C of reflow treatment 6h of temperature, obtain mixture；
C, the mixture for obtaining step b remove two after 900 DEG C of roasting 3h of temperature in nitrogen atmosphere with 8% hydrofluoric acid
Silica, after washing is dried, obtains final product scattered nitrogen coordination iron catalyst (Fe/NC-X, the X table of monokaryon of nitrogen-doped carbon area load
Show silicon dioxide carried iron percentage composition), the X-ray synchrotron radiation result of resulting product is referring to Fig. 1, X-ray photoelectricity
Sub- power spectrum collection of illustrative plates is referring to Fig. 2.
Electrochemical property test
The catalyst fines of the acquisition of 5mg embodiments 1 is weighed, isopropanol waters of the 500uL containing 0.05% naphthol solution is scattered in
(water is 4 with isopropanol volume ratio to solution:1) after, ultrasound is uniform, takes 10uL and drop in rotating circular disk device pyrolytic graphite electrode (Φ
=5mm) on, it is complete that room temperature makes dispersion liquid volatilize, and uses the property of its catalytic oxygen reduction reaction of rotating disk electrode (r.d.e) device to test
Can, respectively as reference electrode and to electrode, 0.1mol/L potassium hydroxide aqueous solutions are used as electrolysis for silver/silver chlorate and platinum electrode
Liquid, referring to Fig. 3, electrode process electron transfer number is referring to Fig. 4 for specific rotating disk electrode (r.d.e) polarization curve；
The scattered nitrogen coordination iron catalyst of monokaryon of nitrogen-doped carbon (NC) area load for preparing, catalytic effect is best
Be Fe/NC-10 rise spike potential be in 0.06V (silver/silver chloride electrode), half wave potential is in -0.125V, electrocatalytic reaction mistake
Average electron shifts number close to 4.0 in journey.
Embodiment 2
Catalyst preparation
A, infusion process：Copper chloride is loaded in 1g silica nanoparticle surfaces (Cu load capacity is 10%)；
B, by step a dipping copper chloride nano SiO 2 particle be dispersed in 8.7g second two after 110 DEG C of dryings of temperature
In amine and carbon tetrachloride mixed liquor, in 90 DEG C of reflow treatment 6h of temperature, mixture is obtained；
C, the mixture for obtaining step b remove two after 900 DEG C of roasting 3h of temperature in nitrogen atmosphere with 8% hydrofluoric acid
Silica, and use FeCl3Solution removes Cu nano particles；
After d, the product for obtaining step c washing are dried, the scattered nitrogen of monokaryon of nitrogen-doped carbon (NC) area load is obtained final product
Complex copper catalyst (Cu/NC-10).
Electrochemical property test
The catalyst fines of the acquisition of 5mg embodiments 2 is weighed, isopropanol waters of the 500uL containing 0.05% naphthol solution is scattered in
(water is 4 with isopropanol volume ratio to solution:1) after, ultrasound is uniform, takes 10uL and drop in rotating circular disk device pyrolytic graphite electrode (Φ
=5mm) on, it is complete that room temperature makes dispersion liquid volatilize, and uses the property of its catalytic oxygen reduction reaction of rotating disk electrode (r.d.e) device to test
Can, respectively as reference electrode and to electrode, 0.1mol/L potassium hydroxide aqueous solutions are used as electrolysis for silver/silver chlorate and platinum electrode
Liquid, referring to Fig. 5, electrode process electron transfer number is referring to Fig. 4 for specific rotating disk electrode (r.d.e) polarization curve；
The scattered nitrogen coordination iron catalyst of monokaryon of nitrogen-doped carbon (NC) area load for preparing, catalytic effect is best
Be Cu/NC-10 rise spike potential be in 0.06V (silver/silver chloride electrode), half wave potential is in -0.125V, electrocatalytic reaction mistake
Average electron shifts number close to 4.0 in journey.
Embodiment 3
Catalyst preparation
A, infusion process：0.5g porous silica area loads cobalt chloride (Co load capacity is 10%)；
B, the porous silica of step a impregnating metal cobalt chlorides is dispersed in 8.7g second two after 110 DEG C of dryings of temperature
In amine and carbon tetrachloride mixed liquor, in 90 DEG C of reflow treatment 6h of temperature, mixture is obtained；
C, the mixture for obtaining step b 900 DEG C of roasting 3h of temperature in nitrogen atmosphere, with concentration for 8% hydrofluoric acid is removed
Remove silica；
After d, the product for obtaining step c washing are dried, the scattered nitrogen of monokaryon of nitrogen-doped carbon (NC) area load is obtained final product
Coordination Co catalysts (Co/NC-10).
Electrochemical property test
The catalyst fines of the acquisition of 5mg embodiments 3 is weighed, isopropanol waters of the 500uL containing 0.05% naphthol solution is scattered in
(water is 4 with isopropanol volume ratio to solution:1) after, ultrasound is uniform, takes 10uL and drop in rotating circular disk device pyrolytic graphite electrode (Φ
=5mm) on, it is complete that room temperature makes dispersion liquid volatilize, and uses the property of its catalytic oxygen reduction reaction of rotating disk electrode (r.d.e) device to test
Can, respectively as reference electrode and to electrode, 0.1mol/L potassium hydroxide aqueous solutions are used as electrolysis for silver/silver chlorate and platinum electrode
Liquid, referring to Fig. 5, electrode process electron transfer number is referring to Fig. 4 for specific rotating disk electrode (r.d.e) polarization curve；
The scattered nitrogen coordination iron catalyst of monokaryon of nitrogen-doped carbon (NC) area load for preparing, catalytic effect is best
Be Co/NC-10 rise spike potential be in 0.06V (silver/silver chloride electrode), half wave potential is in -0.125V, electrocatalytic reaction mistake
Average electron shifts number close to 4.0 in journey.
Embodiment 4
Catalyst preparation
A, infusion process：0.5g porous silica area loads nickel chloride (Ni load capacity is 10%)；
B, the porous silica of step a impregnating metal nickel chlorides is dispersed in 8.7g second two after 110 DEG C of dryings of temperature
In amine and carbon tetrachloride mixed liquor, in 90 DEG C of reflow treatment 6h of temperature, mixture is obtained；
C, the mixture for obtaining step b 900 DEG C of roasting 3h of temperature in nitrogen atmosphere, with concentration for 8% hydrofluoric acid is removed
Remove silica；
After d, the product for obtaining step c washing are dried, the scattered nitrogen of monokaryon of nitrogen-doped carbon (NC) area load is obtained final product
Coordination Raney nickel (Ni/NC-10).
Electrochemical property test
The catalyst fines of the acquisition of 5mg embodiments 4 is weighed, isopropanol waters of the 500uL containing 0.05% naphthol solution is scattered in
(water is 4 with isopropanol volume ratio to solution:1) after, ultrasound is uniform, takes 10uL and drop in rotating circular disk device pyrolytic graphite electrode (Φ
=5mm) on, it is complete that room temperature makes dispersion liquid volatilize, and uses the property of its catalytic oxygen reduction reaction of rotating disk electrode (r.d.e) device to test
Can, respectively as reference electrode and to electrode, 0.1mol/L potassium hydroxide aqueous solutions are used as electrolysis for silver/silver chlorate and platinum electrode
Liquid, referring to Fig. 3, electrode process electron transfer number is referring to Fig. 4 for specific rotating disk electrode (r.d.e) polarization curve；
The scattered nitrogen coordination iron catalyst of monokaryon of nitrogen-doped carbon (NC) area load for preparing, catalytic effect is best
Be Ni/NC-10 rise spike potential be in 0.06V (silver/silver chloride electrode), half wave potential is in -0.125V, electrocatalytic reaction mistake
Average electron shifts number close to 4.0 in journey.
Embodiment 5
Catalyst preparation
A, infusion process：2.5g porous silica area loads ferric acetyl acetonade (Fe load capacity is 5%)；
B, the porous silica of step a impregnating metal ferric acetyl acetonades is dispersed in 8.7g after 110 DEG C of dryings of temperature
In ethylenediamine and carbon tetrachloride mixed liquor, in 90 DEG C of reflow treatment 6h of temperature, mixture is obtained；
C, the mixture for obtaining step b 900 DEG C of roasting 3h of temperature in nitrogen atmosphere, with concentration for 8% hydrofluoric acid is removed
Remove silica；
After d, the product for obtaining step c washing are dried, the scattered nitrogen of monokaryon of nitrogen-doped carbon (NC) area load is obtained final product
Coordination iron catalyst (Fe-2/NC-5).
Electrochemical property test
The catalyst fines of the acquisition of 5mg embodiments 5 is weighed, isopropanol waters of the 500uL containing 0.05% naphthol solution is scattered in
(water is 4 with isopropanol volume ratio to solution:1) after, ultrasound is uniform, takes 10uL and drop in rotating circular disk device pyrolytic graphite electrode (Φ
=5mm) on, it is complete that room temperature makes dispersion liquid volatilize, and uses the property of its catalytic oxygen reduction reaction of rotating disk electrode (r.d.e) device to test
Can, respectively as reference electrode and to electrode, 0.1mol/L potassium hydroxide aqueous solutions are used as electrolysis for silver/silver chlorate and platinum electrode
Liquid, referring to Fig. 5, electrode process electron transfer number is referring to Fig. 4 for specific rotating disk electrode (r.d.e) polarization curve；
The scattered nitrogen coordination iron catalyst of monokaryon of nitrogen-doped carbon (NC) area load for preparing, catalytic effect is best
Be Fe-2/NC-10 rise spike potential be in 0.06V (silver/silver chloride electrode), half wave potential is in -0.125V, electrocatalytic reaction
During average electron shift number close to 4.0.
Claims (3)
1. a kind of preparation method of nitrogen-doped carbon area load mononuclear catalyst, it is characterised in that follow these steps to carry out：
A, infusion process：It is iron chloride, ferric acetyl acetonade, copper chloride, nickel chloride or chlorination in silica surface loading metal-salt
Cobalt；
B, the silica of step a impregnating metal salt is dispersed in ethylenediamine and carbon tetrachloride after 100-150 DEG C of drying of temperature
In mixed liquor, in 60-100 DEG C of reflow treatment 6-10h of temperature, mixture is obtained；
C, the mixture for obtaining step b are calcined 3-8 h in nitrogen atmosphere, and silica is removed with hydrofluoric acid；
D, the product for obtaining step c washing drying, obtain final product the mononuclear catalyst of nitrogen-doped carbon area load.
2. the preparation method of nitrogen-doped carbon area load mononuclear catalyst according to claim 1, it is characterised in that step
Silica is porous silica or nano SiO 2 particle in rapid a.
3. according to claim 1 method obtain nitrogen-doped carbon area load mononuclear catalyst purposes, its feature
It is by the catalyst preparation into electrode, for the purposes in catalytic oxygen reduction reaction.
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108246332A (en) * | 2018-01-16 | 2018-07-06 | 浙江大学 | A kind of non-noble metal supported catalyst of two dimension and its preparation method and application |
| CN109023417A (en) * | 2018-07-25 | 2018-12-18 | 吉林大学 | Cementite-cobalt/nitrogen-doped carbon nanocomposite preparation method and application |
| CN109675603A (en) * | 2018-12-28 | 2019-04-26 | 西安交通大学 | A kind of carbon-supported catalysts and its preparation method and application of silica protection |
| CN110124722A (en) * | 2019-06-11 | 2019-08-16 | 河北科技大学 | A kind of monatomic catalyst of nitrogen-doped carbon Base Metal and its preparation method and application |
| CN110620242A (en) * | 2018-06-19 | 2019-12-27 | 中国科学院上海硅酸盐研究所 | Iron/nitrogen binary doped carbon catalyst loaded with ruthenium nanoparticles and preparation method thereof |
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| CN108246332A (en) * | 2018-01-16 | 2018-07-06 | 浙江大学 | A kind of non-noble metal supported catalyst of two dimension and its preparation method and application |
| CN110620242A (en) * | 2018-06-19 | 2019-12-27 | 中国科学院上海硅酸盐研究所 | Iron/nitrogen binary doped carbon catalyst loaded with ruthenium nanoparticles and preparation method thereof |
| CN109023417A (en) * | 2018-07-25 | 2018-12-18 | 吉林大学 | Cementite-cobalt/nitrogen-doped carbon nanocomposite preparation method and application |
| CN109675603A (en) * | 2018-12-28 | 2019-04-26 | 西安交通大学 | A kind of carbon-supported catalysts and its preparation method and application of silica protection |
| CN110124722A (en) * | 2019-06-11 | 2019-08-16 | 河北科技大学 | A kind of monatomic catalyst of nitrogen-doped carbon Base Metal and its preparation method and application |
| CN110668415A (en) * | 2019-09-19 | 2020-01-10 | 山东科技大学 | Method for preparing atomic-scale dispersed metal nitrogen carbon material based on fumed silica |
| CN110668415B (en) * | 2019-09-19 | 2022-06-28 | 山东科技大学 | Method for preparing atomic-scale dispersed metal nitrogen carbon material based on fumed silica |
| CN112382768A (en) * | 2020-11-17 | 2021-02-19 | 中国科学院新疆理化技术研究所 | Preparation method and application of iron and nitrogen co-doped hierarchical ordered porous carbon catalyst |
| CN112645327A (en) * | 2020-12-21 | 2021-04-13 | 中国烟草总公司郑州烟草研究院 | Preparation method of porous carbon core-shell composite material |
| CN113422070A (en) * | 2021-06-18 | 2021-09-21 | 福州大学 | Preparation method of iron-based dopamine supramolecular modification-based copper hydroxide two-dimensional nanocomposite |
| CN113774410A (en) * | 2021-10-25 | 2021-12-10 | 齐鲁工业大学 | Nitrogen-doped mesoporous hollow carbon nanosphere loaded metal catalyst and preparation method and application thereof |
| CN113774410B (en) * | 2021-10-25 | 2022-09-13 | 齐鲁工业大学 | Nitrogen-doped mesoporous hollow carbon nanosphere loaded metal catalyst and preparation method and application thereof |
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