CN104888779A - Preparation method of Cu nanoparticle-loaded ordered mesoporous carbon catalyst - Google Patents
Preparation method of Cu nanoparticle-loaded ordered mesoporous carbon catalyst Download PDFInfo
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- CN104888779A CN104888779A CN201510221357.7A CN201510221357A CN104888779A CN 104888779 A CN104888779 A CN 104888779A CN 201510221357 A CN201510221357 A CN 201510221357A CN 104888779 A CN104888779 A CN 104888779A
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Abstract
The invention discloses a preparation method of a Cu nanoparticle-loaded ordered mesoporous carbon catalyst. A carbon source precursor, a template and a copper salt are co-assembled in a solvent so that the Cu nanoparticle-loaded ordered mesoporous carbon catalyst is prepared. The Cu nanoparticle-loaded ordered mesoporous carbon catalyst is a nanoscale catalyst. Copper particles with the sizes of 5-25nm are inlaid in channels and surfaces of the ordered mesoporous carbon so that migration and agglomeration in the reaction process are not produced easily. The Cu nanoparticle-loaded ordered mesoporous carbon catalyst has high stability in normal pressure continuous fixed bed gas phase methanol oxidation carbonylation synthesis of dimethyl carbonate, has good reaction activity and has a good industrial application prospect.
Description
Technical field
The invention belongs to the heterogeneous catalysis field of chemical, be specifically related to a kind of preparation method of ordered mesopore carbon loaded Cu nano-particle catalyst.
Background technology
Dimethyl carbonate is the simplest organic carbonate, nontoxic and be easy to biodegradation, and be the basic material of other carbonic ester of non-phosgene green syt and polyester material, be also important innoxious solvent and octane number additive, market application foreground is wide.Take methyl alcohol as raw material, high by oxidative carbonylation route synthesis DMC equilibrium conversion, having the advantages such as the low and green syt of cost, is one of route of important Coal Clean efficiency utilization.
At present, there is chlorion and to run off in course of reaction the deactivation prob caused in the catalyst being active component with the chloride of copper or palladium in vapor phase method reaction, can improve catalytic activity although add auxiliary agent or improve preparation method and improve stability, the deactivation prob of catalyst fails to solve at all.Active carbon (AC) becomes the excellent catalyst carrier of vapor phase method methanol oxidation carbonylation due to its stable chemical property, good electronic conductivity and larger specific area; And adopt non-chlorine mantoquita to be that the problems such as the catalysqt deactivation that Cl ion causes are avoided introducing in copper source from source, become the Main way of research in recent years.
The people such as Li Zhong are by Cu (CH
3cOO)
2be immersed on AC, direct pyrolysis obtains Cu
2o/AC catalyst, catalytic activity is good.Chemical modification is carried out on AC surface group and can affect Cu (CH
3cOO)
2dispersion and pyrolytic process, cause catalyst surface to disperse copper species (Cu/Cu
+/cu
2+) grain size and the change of valence state, and then affect catalytic activity.Adopt hydrazine hydrate chemical preparation AC supported copper catalyst based, hydrazine hydrate addition can affect Cu species valence state, and when the mol ratio of hydrazine hydrate/copper nitrate material is 0.75, AC surface is with Cu
2o is main, and catalytic activity is higher.Adopting AC load basic copper nitrate, CuO/AC can be obtained respectively, Cu by strictly regulating and controlling heat-treat condition
2o/AC and Cu
0/ AC catalyst, the order of catalytic activity size is CuO < Cu
2o < Cu
0.Ren Jun etc. for raw material, obtain Cu through sol gel, high temperature cabonization and KOH activation with copper nitrate and soluble starch
0/ AC catalyst, when carbonization, activation temperature are respectively 500 DEG C and 850 DEG C, when KOH: C=1, the specific area of catalyst reaches 1690m
2/ g, Micropore volume rate is 72.4%, and catalytic activity is the highest.
Although active carbon (AC) load to show good oxidation carbonylation without chlorine copper-based catalysts active, still there is the problem that catalytic activity declines along with the carrying out of reaction in such catalyst.Cu is thought in the research of Zheng Huayan etc.
0o in simple substance Cu adsorption reaction atmosphere in/AC catalyst
2be converted into Cu
2o, along with the carrying out of reaction, Cu
2o grain growth, there occurs obvious agglomeration, causes catalytic activity to reduce.
Summary of the invention
The object of the invention is to propose to inlay 5 ~ 25nm copper particle in a kind of nanoscale, surface and duct, there is the ordered mesopore carbon Catalysts and its preparation method of high activity and stability.The present invention adopts nanoscale, has the Cu nano particle of the ordered mesopore carbon of suitable pore passage structure (OMC) load height dispersion, significantly improve activated centre quantity on the one hand, utilize the valence state of the reproducibility regulation activity copper species of carbon to make it maintain active best zeroth order on the other hand, the activity of catalyst and stability are significantly promoted.
The present invention adopts following technical scheme:
A preparation method for ordered mesopore carbon loaded Cu nano-particle catalyst, adopts carbon source precursor, template, mantoquita to obtain ordered mesopore carbon loaded Cu nano-particle catalyst by the mode of assembling altogether in a solvent.
The preparation method of described ordered mesopore carbon loaded Cu nano-particle catalyst, described carbon source precursor is the phenol resin oligomer comprising phenol/formaldehyde resins, resorcin/formaldehyde resin, urea/phenol/formaldehyde resins.
The preparation method of described ordered mesopore carbon loaded Cu nano-particle catalyst, the template of employing is the triblock copolymer or its mixing that comprise P123, F127, F108.
The preparation method of described ordered mesopore carbon loaded Cu nano-particle catalyst, the mantoquita of employing is the organic/inorganic copper compound comprising copper sulphate, copper nitrate, Schweinfurt green, cupric tartrate, copper citrate.
The preparation method of described mesoporous carbon-loaded Cu nano-particle catalyst, the solvent of employing is ethanol, water or its mixing.
The preparation method of described mesoporous carbon-loaded Cu nano-particle catalyst; described template, carbon source precursor, mantoquita and solvent in mass ratio 1: 0.5 ~ 2: 0.02 ~ 0.2: 10 ~ 30 ratios feed intake; 0.1 ~ 10h is reacted under magnetic agitation; after discarding solvent; hot polymerization 1 ~ 72h at 70 ~ 150 DEG C; under inert atmosphere protection, carbonization 1 ~ 10h at 300 DEG C ~ 900 DEG C, obtained mesoporous carbon-loaded Cu nano-particle catalyst.
The preparation method of described mesoporous carbon-loaded Cu nano-particle catalyst, described preparation method is specially: joined by template in solvent, and room temperature lower magnetic force is stirred to and dissolves to obtain solution A completely; The ethanolic solution of the ethanolic solution of carbon source precursor and mantoquita slowly to be joined successively in solution A and to stir 2h; After stirring terminates, solution at room temperature leaves standstill 4h, discards supernatant liquor, the colloidal sol of lower floor's thickness is placed in air dry oven, temperature is set to 85 DEG C, keeps 24h; After drying terminates; sample is placed in the tube furnace of nitrogen protection; 300 ~ 350 DEG C are warming up to the heating rate of 1 DEG C/min; constant temperature keeps 3h; then be warming up to 600 ~ 900 DEG C with the heating rate of 3 DEG C/min, constant temperature keeps 2h, finally; sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
The preparation method of described mesoporous carbon-loaded Cu nano-particle catalyst, described preparation method is specially: join in etoh solvent by template and mantoquita, and room temperature lower magnetic force is stirred to and dissolves to obtain solution A completely; The ethanolic solution of carbon source precursor slowly to be joined in solution A and to stir 2h, dissolution homogeneity is layered in surface plate; Make solvent volatilization 4h under 30 DEG C of conditions, sample is placed in air dry oven, hot polymerization 24h at 100 DEG C; Then, sample is placed in the tube furnace of nitrogen protection, is warming up to 350 DEG C with the heating rate of 1 DEG C/min; constant temperature keeps 3h, is then warming up to 800 DEG C with the heating rate of 5 DEG C/min, and constant temperature keeps 2h; finally, sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
The concrete steps that above-mentioned copper-based catalysts is used for Oxidative Carbonylation Synthesis of DMC are feedstock mol ratio CO: O
2be 5: 1 ~ 15: 1, reaction temperature 120 DEG C ~ 160 DEG C, Feed space velocities is 2000h
-1~ 5000
-1, catalyst amount is 0.2 ~ 2g.
The present invention with carbon source precursor, surfactant templates and organic/inorganic mantoquita for raw material, the method of being assembled altogether by solvent volatilization induction ternary prepares the catalyst of ordered mesopore carbon loaded Cu nano particle, prepared catalyst is nanoscale, the copper particle of 5 ~ 25nm is embedded in duct and the surface of ordered mesopore carbon, in course of reaction, not easily there is migration and reunite, high for stability in the reaction of normal pressure continuous Fixed Bed Gas Phase methanol oxidation carbonylation Synthesis of dimethyl carbonate, reactivity is good, has good prospects for commercial application.
Prepared by the present invention is nanoscale without chlorine copper-based catalysts, in the duct being embedded in ordered mesopore carbon (OMC) due to the copper particle of 5 ~ 25nm and surface, in course of reaction, not easily there is migration and reunite, reactivity for normal pressure continuous Fixed Bed Gas Phase methanol oxidation carbonylation Synthesis of dimethyl carbonate is high, good stability.The space-time yield of DMC reaches 226mg/ (gh), and active in declining in reaction 100h, activity is much higher than Cu prepared by existing Solid-state Ion-exchange
+/ Y catalyst.
Accompanying drawing explanation
Fig. 1 is the transmission electron microscope of Cu-OMC catalyst prepared by embodiment 1;
Fig. 2 is the transmission electron microscope of Cu-OMC catalyst prepared by embodiment 2;
Fig. 3 is the transmission electron microscope of Cu-OMC catalyst prepared by embodiment 3;
Detailed description of the invention
Below in conjunction with specific embodiment, the present invention is described in detail.
The resol used in the present invention adopts conventional method preparation, and phenol/formaldehyde molar ratio is generally 1: 2.5 ~ 1: 1, and resorcin/formaldehyde molar ratio is generally 1: 5 ~ 1: 2, and employing NaOH is catalyst, also can directly purchase.
Embodiment 1
Join in 32g ethanol by 3.2g triblock copolymer F127, room temperature lower magnetic force is stirred to and dissolves completely.The ethanolic solution of the resol (phenol/formaldehyde) of 8g 25% and 4mL are dissolved with 0.08g Cu (NO
3)
23H
2the ethanolic solution of O (nitrate trihydrate copper) slowly to join successively in above-mentioned solution and stirs 2h.After stirring terminates, solution is in room. and leave standstill 4h under temperature, discard supernatant liquor, the colloidal sol of lower floor's thickness is placed in air dry oven, temperature is set to 85 DEG C, keep 24h.After drying terminates, sample is placed in the tube furnace of nitrogen protection, is warming up to 350 DEG C with the heating rate of 1 DEG C/min; constant temperature keeps 3h, is then warming up to 900 DEG C with the heating rate of 3 DEG C/min, and constant temperature keeps 2h; finally, sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
The transmission electron microscope test result of the present embodiment gained catalyst as shown in Figure 1.Can find out, Cu-OMC catalyst has the hexagonal mesoporous structure of orderly two dimension, and embedding cloth is in OMC equably for the Cu nano particle that particle diameter is about 10nm, and part is exposed in mesopore orbit.
The micro-trans-chromatogram arrangement of the continuous fixed bed of normal pressure is adopted to carry out active testing to catalyst.0.45g (about 0.5ml) catalyst is placed in the middle part of reactor.Methyl alcohol is introduced, with O by micro-sampling pump
2, CO tow channel gas is mixed into vaporizer, reactor (temperature of reactor is 140 DEG C) is entered together after (140 DEG C) vaporization in vaporizer, after flowing through beds, product flows out from bottom and enters gas chromatograph (Agilent company 6890N) by automatic sampling valve and carries out on-line analysis.Dimethyl carbonate space-time yield 220.4mg/ (gh), methanol conversion 12.58%, dimethyl carbonate selective 90.6%.
Embodiment 2.
Under the condition of 40 DEG C, by 0.06g Cu (CH
3cOO)
2h
2o and 3.2g triblock copolymer F127 joins in 16g ethanol, stirs 30min to dissolving completely.The ethanolic solution of the resol (resorcin/formaldehyde) of 8g 25% slowly to be joined in above-mentioned solution and to stir 2h, dissolution homogeneity is layered in surface plate, make solvent volatilization 4h under 30 DEG C of conditions, sample is placed in air dry oven, hot polymerization 24h at 100 DEG C.Then, sample is placed in the tube furnace of nitrogen protection, is warming up to 350 DEG C with the heating rate of 1 DEG C/min; constant temperature keeps 3h, is then warming up to 800 DEG C with the heating rate of 5 DEG C/min, and constant temperature keeps 2h; finally, sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
The transmission electron microscope test result of catalyst is as Fig. 2.Can find out, Cu-OMC catalyst has six side's phase meso-hole structures of high-sequential, and the Cu nano particle that particle diameter is about 3 ~ 7nm is evenly dispersed in carbon matrix, and part is exposed in the duct of OMC.
The micro-trans-chromatogram arrangement of the continuous fixed bed of normal pressure is adopted to carry out active testing to catalyst.0.45g (about 0.5ml) catalyst is placed in the middle part of reactor.Methyl alcohol is introduced, with O by micro-sampling pump
2, CO tow channel gas is mixed into vaporizer, reactor (temperature of reactor is 130 DEG C) is entered together after (130 DEG C) vaporization in vaporizer, after flowing through beds, product flows out from bottom and enters gas chromatograph (Agilent company 6890N) by automatic sampling valve and carries out on-line analysis.Dimethyl carbonate space-time yield 230.5mg/ (gh), methanol conversion 11.65%, dimethyl carbonate selective 95.6%.
Embodiment 3
Join in 32g ethanol by 3.2g triblock copolymer F127, room temperature lower magnetic force is stirred to and dissolves completely.The ethanolic solution ethanolic solution of the resol (phenol/formaldehyde) of 8g 25% and 4mL being dissolved with 0.08g cupric oxalate slowly to join successively in above-mentioned solution and stirs 2h.After stirring terminates, solution at room temperature leaves standstill 4h, discards supernatant liquor, the colloidal sol of lower floor's thickness is placed in air dry oven, hot polymerization 24h at 85 DEG C.Then, sample is placed in the tube furnace of nitrogen protection, is warming up to 300 DEG C with the heating rate of 1 DEG C/min; constant temperature keeps 3h, is then warming up to 600-900 DEG C with the heating rate of 2-3 DEG C/min, and constant temperature keeps 2-3h; finally, sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
The transmission electron microscope test result of catalyst as shown in Figure 3.Can find out, Cu-OMC catalyst has the hexagonal mesoporous structure of two dimension of high-sequential, and the Cu nano particle that particle diameter is about 10 ~ 20nm is evenly dispersed in carbon matrix, wherein, and the multi-layer mesoporous carbon of Cu particle penetration of greater particle size.
The micro-trans-chromatogram arrangement of the continuous fixed bed of normal pressure is adopted to carry out active testing to catalyst.0.45g (about 0.5ml) catalyst is placed in the middle part of reactor.Methyl alcohol is introduced, with O by micro-sampling pump
2, CO tow channel gas is mixed into vaporizer, reactor (temperature of reactor is 140 DEG C) is entered together after (140 DEG C) vaporization in vaporizer, after flowing through beds, product flows out from bottom and enters gas chromatograph (Agilent company 6890N) by automatic sampling valve and carries out on-line analysis.Dimethyl carbonate space-time yield 226.1mg/ (gh), methanol conversion 12.8%, dimethyl carbonate selective 93.6%.
Should be understood that, for those of ordinary skills, can be improved according to the above description or convert, and all these improve and convert the protection domain that all should belong to claims of the present invention.
Claims (8)
1. a preparation method for ordered mesopore carbon loaded Cu nano-particle catalyst, is characterized in that, adopts carbon source precursor, template, mantoquita to obtain ordered mesopore carbon loaded Cu nano-particle catalyst by the mode of assembling altogether in a solvent.
2. the preparation method of ordered mesopore carbon loaded Cu nano-particle catalyst according to claim 1, it is characterized in that, described carbon source precursor is the phenol resin oligomer comprising phenol/formaldehyde resins, resorcin/formaldehyde resin, urea/phenol/formaldehyde resins.
3. the preparation method of ordered mesopore carbon loaded Cu nano-particle catalyst according to claim 2, is characterized in that, the template of employing is the triblock copolymer or its mixing that comprise P123, F127, F108.
4. the preparation method of ordered mesopore carbon loaded Cu nano-particle catalyst according to claim 3, is characterized in that, the mantoquita of employing is the organic/inorganic copper compound comprising copper sulphate, copper nitrate, Schweinfurt green, cupric tartrate, copper citrate.
5. the preparation method of mesoporous carbon-loaded Cu nano-particle catalyst according to claim 4, is characterized in that, the solvent of employing is ethanol, water or its mixing.
6. according to the preparation method of the arbitrary described mesoporous carbon-loaded Cu nano-particle catalyst of claim 1-5; it is characterized in that; described template, carbon source precursor, mantoquita and solvent in mass ratio 1: 0.5 ~ 2: 0.02 ~ 0.2: 10 ~ 30 ratios feed intake; 0.1 ~ 10h is reacted under magnetic agitation; after discarding solvent, hot polymerization 1 ~ 72h at 70 ~ 150 DEG C, under inert atmosphere protection; carbonization 1 ~ 10h at 300 DEG C ~ 900 DEG C, obtained mesoporous carbon-loaded Cu nano-particle catalyst.
7. the preparation method of mesoporous carbon-loaded Cu nano-particle catalyst according to claim 6, it is characterized in that, described preparation method is specially: joined by template in solvent, and room temperature lower magnetic force is stirred to and dissolves to obtain solution A completely; The ethanolic solution of the ethanolic solution of carbon source precursor and mantoquita slowly to be joined successively in solution A and to stir 2h; After stirring terminates, solution at room temperature leaves standstill 4h, discards supernatant liquor, the colloidal sol of lower floor's thickness is placed in air dry oven, temperature is set to 85 DEG C, keeps 24h; After drying terminates; sample is placed in the tube furnace of nitrogen protection; 300 ~ 350 DEG C are warming up to the heating rate of 1 DEG C/min; constant temperature keeps 3h; then be warming up to 600 ~ 900 DEG C with the heating rate of 3 DEG C/min, constant temperature keeps 2h, finally; sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
8. the preparation method of mesoporous carbon-loaded Cu nano-particle catalyst according to claim 6, it is characterized in that, described preparation method is specially: join in etoh solvent by template and mantoquita, and room temperature lower magnetic force is stirred to and dissolves to obtain solution A completely; The ethanolic solution of carbon source precursor slowly to be joined in solution A and to stir 2h, dissolution homogeneity is layered in surface plate; Make solvent volatilization 4h under 30 DEG C of conditions, sample is placed in air dry oven, hot polymerization 24h at 100 DEG C; Then, sample is placed in the tube furnace of nitrogen protection, is warming up to 350 DEG C with the heating rate of 1 DEG C/min; constant temperature keeps 3h, is then warming up to 800 DEG C with the heating rate of 5 DEG C/min, and constant temperature keeps 2h; finally, sample drops to room temperature under nitrogen protection, obtains Cu-OMC catalyst.
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Cited By (11)
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| CN105521782A (en) * | 2015-12-16 | 2016-04-27 | 中国矿业大学 | Preparation method of Cu nanoparticles-embedded ordered mesoporous carbon catalyst |
| CN105536783A (en) * | 2015-12-23 | 2016-05-04 | 上海大学 | A preparing method of an ordered mesoporous carbon-supported Ru nanometer catalyst |
| CN106542515A (en) * | 2016-10-20 | 2017-03-29 | 中国石油化工股份有限公司 | A kind of synthetic method of meso-porous carbon material |
| CN107837808A (en) * | 2017-11-30 | 2018-03-27 | 上海拓径新材料科技股份有限公司 | The method that the copper-loaded method of macromolecule resin prepares copper-loaded solid carbon |
| CN108786815A (en) * | 2017-05-02 | 2018-11-13 | 中国科学院大连化学物理研究所 | A kind of mesoporous carbon-supported catalysts and its application in polyetheramine synthesis |
| CN109252183A (en) * | 2018-10-22 | 2019-01-22 | 华东师范大学 | It is a kind of to prepare the order mesoporous carbon electrode material method of supported copper and electro-catalysis application |
| CN109382084A (en) * | 2017-08-04 | 2019-02-26 | 中国石油化工股份有限公司 | A kind of meso-porous carbon material and its preparation method and application |
| CN109806873A (en) * | 2019-01-26 | 2019-05-28 | 华南理工大学 | A method of preparing the meso-porous carbon material of load Ni using solid-state synthetic method |
| CN109935797A (en) * | 2017-12-19 | 2019-06-25 | 中国科学院大连化学物理研究所 | A kind of ordered mesopore carbon embeds the preparation method of high dispersion metal atom |
| CN111548273A (en) * | 2020-05-09 | 2020-08-18 | 中国科学技术大学 | Method for preparing dimethyl carbonate by using copper/cuprous oxide nanosheet catalyst to thermally catalyze methanol and carbon dioxide |
| CN113716657A (en) * | 2021-09-22 | 2021-11-30 | 北京林业大学 | Preparation method and application of green recyclable metal oxide embedded ordered mesoporous carbon particle electrode |
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| CN105521782A (en) * | 2015-12-16 | 2016-04-27 | 中国矿业大学 | Preparation method of Cu nanoparticles-embedded ordered mesoporous carbon catalyst |
| CN105536783A (en) * | 2015-12-23 | 2016-05-04 | 上海大学 | A preparing method of an ordered mesoporous carbon-supported Ru nanometer catalyst |
| CN106542515A (en) * | 2016-10-20 | 2017-03-29 | 中国石油化工股份有限公司 | A kind of synthetic method of meso-porous carbon material |
| CN106542515B (en) * | 2016-10-20 | 2019-02-22 | 中国石油化工股份有限公司 | A kind of synthetic method of meso-porous carbon material |
| CN108786815A (en) * | 2017-05-02 | 2018-11-13 | 中国科学院大连化学物理研究所 | A kind of mesoporous carbon-supported catalysts and its application in polyetheramine synthesis |
| CN108786815B (en) * | 2017-05-02 | 2021-05-25 | 中国科学院大连化学物理研究所 | Mesoporous carbon-based catalyst and application thereof in polyether amine synthesis |
| CN109382084B (en) * | 2017-08-04 | 2021-08-06 | 中国石油化工股份有限公司 | Mesoporous carbon material and preparation method and application thereof |
| CN109382084A (en) * | 2017-08-04 | 2019-02-26 | 中国石油化工股份有限公司 | A kind of meso-porous carbon material and its preparation method and application |
| CN107837808A (en) * | 2017-11-30 | 2018-03-27 | 上海拓径新材料科技股份有限公司 | The method that the copper-loaded method of macromolecule resin prepares copper-loaded solid carbon |
| CN109935797B (en) * | 2017-12-19 | 2021-04-02 | 中国科学院大连化学物理研究所 | Preparation method of ordered mesoporous carbon embedded with highly dispersed metal atoms |
| CN109935797A (en) * | 2017-12-19 | 2019-06-25 | 中国科学院大连化学物理研究所 | A kind of ordered mesopore carbon embeds the preparation method of high dispersion metal atom |
| CN109252183B (en) * | 2018-10-22 | 2021-03-26 | 华东师范大学 | Method for preparing copper-loaded ordered mesoporous carbon electrode material and electrocatalysis application |
| CN109252183A (en) * | 2018-10-22 | 2019-01-22 | 华东师范大学 | It is a kind of to prepare the order mesoporous carbon electrode material method of supported copper and electro-catalysis application |
| CN109806873A (en) * | 2019-01-26 | 2019-05-28 | 华南理工大学 | A method of preparing the meso-porous carbon material of load Ni using solid-state synthetic method |
| CN111548273A (en) * | 2020-05-09 | 2020-08-18 | 中国科学技术大学 | Method for preparing dimethyl carbonate by using copper/cuprous oxide nanosheet catalyst to thermally catalyze methanol and carbon dioxide |
| CN111548273B (en) * | 2020-05-09 | 2021-10-01 | 中国科学技术大学 | Method for preparing dimethyl carbonate by using copper/cuprous oxide nanosheet catalyst to thermally catalyze methanol and carbon dioxide |
| CN113716657A (en) * | 2021-09-22 | 2021-11-30 | 北京林业大学 | Preparation method and application of green recyclable metal oxide embedded ordered mesoporous carbon particle electrode |
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Application publication date: 20150909 |