CN103302304A - Preparation method of nickel or nickel alloy nanotube - Google Patents
Preparation method of nickel or nickel alloy nanotube Download PDFInfo
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- CN103302304A CN103302304A CN2013102260780A CN201310226078A CN103302304A CN 103302304 A CN103302304 A CN 103302304A CN 2013102260780 A CN2013102260780 A CN 2013102260780A CN 201310226078 A CN201310226078 A CN 201310226078A CN 103302304 A CN103302304 A CN 103302304A
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Abstract
The invention relates to the technical field of preparation of a metal or alloy nanotube, in particular to a preparation method of a nickel or nickel alloy nanotube. The preparation method of the nickel or nickel alloy nanotube comprises the following steps: (1) performing a reaction on nickel salt solution or mixed metal salt solution comprising nickel salt and aqueous alkali to generate a precursor colloid; (2) processing the precursor colloid under the hydrothermal condition to obtain a nanowire; and (3) performing the catalytic reaction on the surface of the nanowire and catalyzing the performance of a reducing agent and nickel ions by taking the surface of the nanowire as an active point so as to form a tubular structure of nickel and nickel alloy. Compared with the prior art, the preparation method disclosed by the invention does not require a hard template; equipment required by the preparation method is simple; the preparation method can be used only by improving a common reactor and constant temperature equipment; and moreover, the process is simple and easy to operate and the cost is low.
Description
Technical field
The present invention relates to the technical field of metal or alloy nanotube preparation, particularly the preparation method of a kind of nickel or nickel alloy nanotube.
Background technology
Nickel or Ni alloy powder are widely used in the industrial production as a kind of effective microwave absorbing material.The electromagnetic performance of nickel or Ni alloy powder except the nanometer that is subjected to material, hollowization influence, is influenced by the fibrillatable of material also.How realizing the high-quality of ferromagnetic nano pipe, low-cost assembling, obtain stable, consistent ferromagnetic nano tubular structure, is the key that increases substantially the ripple absorbent properties of nickel or nickel alloy powder powder material.
Nickel or nickel alloy nanotube owing to have the one dimension hollow-core construction, can obtain special light, electricity, magnetic property; Simultaneously, at the inner assembling of nanotube ferromagnetic nano particle, can obtain interior dispatch from foreign news agency, the distinct compound one-dimensional nano structure of magnetic property.Find by literature search, Jianchun Bao is at " Advanced Materials " (Vol.13, No.21,2003) delivered the report of " Template synthesis of an array of nickel nanotubules and its magnetic behavior " (template prepares nickel nanotube and magnetic property research thereof) on, this article has been reported a kind of by utilizing alumina formwork, adopt electrodeposition process successfully to prepare high-sequential, be about the preparation method of the nickel nanotube of 35um.Xiufeng Han is at " Advanced Materials " (Vol.21, No.45,2009) delivered the article of " Structural and Magnetic Properties of Various Ferromagnetic Nanotubes " (the structure and magnetic properties energy of multiple ferromagnetic nano pipe) on, article has been reported and has been utilized alumina formwork, adopt electrodeposition process successfully to prepare interior external diameter, thickness, Fe that length is different, Co, Ni and ferromagnetic metal alloy are (as NiFe, CoPt, CoFeB and CoCrPt) preparation method of nanotube.The template that above method adopts is based on hard template (aluminum oxide porous film), by prepared by electrodeposition nickel or nickel alloy nanotube.The nanotube for preparing in hard template by electrodeposition process, need remove hard template by chemical treatment, just can obtain required material, but for being about several microns, internal diameter has only the nanotube of tens nanometers even several nanometers, and this method is removed hard template can compare difficulty.
Summary of the invention
The object of the invention is to provide the preparation method of a kind of nickel or nickel alloy nanotube, to solve nickel of the prior art or the nickel alloy nanotube prepares nanotube by electrodeposition process in hard template, need remove hard template by chemical treatment, just can obtain required material, but for being about several microns, internal diameter has only the nanotube of tens nanometers even several nanometers, and this method is removed hard template can compare the difficult technologies problem.
The object of the invention is achieved through the following technical solutions:
The preparation method of a kind of nickel or nickel alloy nanotube may further comprise the steps:
(1) nickel salt solution or comprise the mixed salt solution of nickel salt and the aqueous slkali reaction generates the presoma colloid;
(2) described presoma colloid is handled under hydrothermal condition and is obtained nano wire;
(3) in above-mentioned nanowire surface generation catalytic reaction, be the reaction of active site catalytic reducer and nickel ion with the nanowire surface, form the tubular structure of nickel or nickel alloy.
Preferably, described step (1) further comprises:
Nickel salt solution or the mixed salt solution that comprises nickel salt are heated to T1, under agitation, pour aqueous slkali into nickel salt solution or comprise in the mixed salt solution of nickel salt, stir, obtain the presoma colloid of homogeneous.
Preferably, described nickel salt solution concentration or the total concentration that comprises the mixed salt solution of nickel salt are 0.1-0.3mol/L, and the concentration of described alkali lye is 0.1-0.3mol/L, and T1 is 50-80 ℃.
Preferably, described nickel salt be selected from nickelous sulfate, nickel chloride, nickel nitrate or nickel acetate wherein one or more.
Preferably, the described mixed metal salt of nickel salt that comprises is for also comprising wherein one or more the mixed metal salt of cobaltous sulfate, cobalt acetate, cobalt nitrate, cobalt chloride, frerrous chloride, ferrous sulfate except comprising nickel salt.
Preferably, described alkali is selected from NaOH, potassium hydroxide, calcium hydroxide or ammoniacal liquor.
Preferably, described step (2) further comprises:
The presoma colloid is imported in the reactor, and the reactor sealing is incubated a period of time after reactor is heated to T2, and cooling naturally is taken out, and cleaning gets nano wire.
Preferably, T2 is 110-180 ℃, and temperature retention time is 12-48 hour.
Preferably, described step (3) further comprises:
Nano wire dilutes with appropriate amount of deionized water, ultrasonic processing 10-40 minute is heated to T3 afterwards, regulates the pH value to 2-12, reducing agent is heated to T4 to be poured in the nano wire afterwards, constantly stir simultaneously, drip little amount of catalyst, a large amount of bubbles are emerged subsequently, reaction is acutely carried out, occur a large amount of black precipitates in the solution, treat no longer to produce in the solution bubble, i.e. reaction is finished substantially.
Preferably, T3 is 80-95 ℃, and T4 is 80-95 ℃.
Preferably, described reducing agent is selected from hypophosphite, boron hydride, hydrazine hydrate, sodium tungstate or potassium tungstate, and the concentration of described reducing agent is 0.01-1mol/L.
Preferably, also comprise step (4):
The tubular structure of gained is respectively after ammoniacal liquor, deionized water, acetone washing, dry in baking oven, namely obtain nickel or nickel alloy nanotube through aftertreatment technology again.
Preferably, described aftertreatment technology is 200～600 ℃ hydrogen reducing processing.
Preferably, described nanotube is Powdered, includes water, nickel hydroxide, nickel oxide, hydrogen and steam in the described nanotube, and the nanotube external diameter is 60-300nm, and internal diameter is the 20-100 nanometer, and pipe range is the 3-6 micron.
Preferably, the composition of described nanotube is binary, ternary or the quaternary alloy of pure nickel or nickel.
Compared with prior art, the present invention has following beneficial effect:
1, preparation method of the present invention does not need hard template, and equipment needed thereby is simple, only need just to be improved on common response device and thermostatic equipment and can use, and technological operation is simple, and is with low cost;
2, nickel and the nickel alloy ball nanotube of preparation method's preparation of the present invention are amorphous or crystallite attitude, can do further heat treatment at 200～600 ℃, obtain the nickel and nickel alloy tube sprills of complete crystallization;
3, the external diameter size can be controlled by regulating presoma nanowire diameter and reaction temperature and time in the nanotube of preparation method's preparation of the present invention, can access the nanotube of different interior external diameter sizes;
4, preparation method of the present invention can prepare binary, the ternary of pure nickel or heterogeneity, the nanotube powder of quaternary nickel alloy by the concentration of selecting different reducing agents and regulating reducing agent.
Description of drawings
Fig. 1 is Ni (SO
4)
0.3(OH)
1.4The XRD collection of illustrative plates of nano wire;
Fig. 2 is the XRD collection of illustrative plates of Ni-P nanotube;
Fig. 3 is Ni (SO
4)
0.3(OH)
1.4The TEM photo of nano wire;
Fig. 4 is the TEM photo of Ni-P nanotube.
The specific embodiment
The present invention proposes in the aqueous solution directly reaction first and generates glue nuclear, glue nuclear again by hydro-thermal reaction to the presoma nano wire, in nanowire surface generation catalytic reaction, preparation nickel and nickel alloy nanotube.The prepared nanotube of the present invention is expected to be applied in fields such as effective catalyst, adsorbent and photoelectricity, electromagnetic device, microwave absorbing material and bio-pharmaceuticals owing to its particular structure.
The preparation method of nickel of the present invention or nickel alloy nanotube may further comprise the steps: nickel salt solution or comprise the mixed salt solution of nickel salt and the aqueous slkali reaction generates the presoma colloid; Described presoma colloid obtains nano wire by hydro-thermal reaction; In above-mentioned nanowire surface generation catalytic reaction, be the reaction of active site catalytic reducer and nickel ion with the nanowire surface, form the tubular structure of nickel or nickel alloy; Described tubular structure obtains nickel or nickel alloy nanotube through aftertreatment technology.
Below in conjunction with drawings and Examples technical scheme of the present invention is further described.
The preparation of embodiment 1 nickel-phosphor alloy nanotube
Nickelous sulfate, inferior sodium phosphate and NaOH are mixed with the solution of 2mol/L, 2mol/L and 2mol/L respectively, get 7.5ml nickelous sulfate (2mol/L) in the beaker of 250ml, add the 45ml deionized water again, nickelous sulfate after the dilution was heated 8 minutes in 90 ± 1 ℃ constant temperature water bath, then the NaOH (2mol/L) of 7.5ml is slowly poured in the nickel sulfate solution after the dilution, the limit bevelling stirs, and obtains the nickel hydroxide colloid of homogeneous at last.The nickel hydroxide colloid is placed the reactor of 100ml, sealing, insulation is 24 hours in 120 ℃ oil bath pan, and cooling naturally is taken out and is used washed with de-ionized water 6 times, and obtaining concentration is the Ni (SO of 0.018mol/L
4)
0.3(OH)
1.4Nanowire suspension (wherein contains Ni (SO
4)
0.3(OH)
1.4Nano wire 1.18 grams).Ni (SO
4)
0.3(OH)
1.4Nano thread structure and form are respectively as Fig. 1 and shown in Figure 3.Get the above-mentioned Ni (SO of 10ml
4)
0.3(OH)
1.4Nanowire suspension is diluted to 45ml, handles 20 minutes in 600 watts of Ultrasound Instrument, places 90 ± 1 ℃ constant temperature water bath to heat again 10 minutes, behind acetic acid regulator solution pH=4, pours 3ml ortho phosphorous acid sodium solution (2mol/L) into Ni (SO
4)
0.3(OH)
1.4Nano wire adds 1 palladium bichloride (1g/L) at last, and reaction is acutely carried out, a large amount of black precipitates appear in the solution, the back washing is filtered in the black precipitate of gained, and drying is 2 hours in 55 ℃ of baking ovens, and nickel-phosphorus is amorphous and crystallite attitude (as shown in Figure 2) in the gained powder.Phosphorus content is 8.92% in last gained nickel-phosphorus nanotube alloy powder, and the external diameter of pipe size is 60-300nm, and the internal diameter size is the 20-100 nanometer, and pipe range is 3-6 micron (as shown in Figure 4).
The preparation of embodiment 2 nickel-boron alloy nanotube
Nickelous sulfate, sodium borohydride and ammoniacal liquor are mixed with the solution of 2mol/L, 2mol/L and 2mol/L respectively, get 9ml nickelous sulfate (2mol/L) in the beaker of 250ml, add the 45ml deionized water again, nickelous sulfate after the dilution was heated 8 minutes in 85 ± 1 ℃ constant temperature water bath, then the ammoniacal liquor of 9ml is slowly poured in the nickel sulfate solution after the dilution, the limit bevelling stirs, and obtains the cobalt hydroxide colloid of homogeneous at last.The nickel hydroxide colloid is placed the reactor of 100ml, sealing, insulation is 24 hours in 120 ℃ oil bath pan, naturally cooling, take out and use washed with de-ionized water 6 times, obtaining concentration is the nickel hydroxide nano line suspension (wherein containing nickel hydroxide nano line 1.37 grams) of 0.018mol/L.Get the above-mentioned nickel hydroxide nano line of 10ml suspension, be diluted to 45ml, handled 20 minutes in 600 watts of Ultrasound Instrument, place 85 ± 1 ℃ constant temperature water bath to heat again 10 minutes, behind acetic acid regulator solution pH=2, (2mol/L) pours the nickel hydroxide nano line into the 3ml sodium borohydride solution, add 1 palladium bichloride (1g/L) at last, reaction is acutely carried out, occur a large amount of black precipitates in the solution, the back washing is filtered in the black precipitate of gained, drying is 2 hours in 55 ℃ of baking ovens, nickel-boron is amorphous and crystallite attitude in the gained powder, obtains the nickel-boron nanotube of complete crystallization after 300 ℃ of heat treatment.Boron content is 7.53% in last gained nickel-boron nanotube alloy powder, external diameter of pipe size 60-300nm, internal diameter size 20-100 nanometer, pipe range 3-6 micron.
The preparation of embodiment 3 nickel-cobalt-phosphorus alloy nanotube
With nickelous sulfate, cobaltous sulfate, inferior sodium phosphate and NaOH are mixed with the solution of 2mol/L, 2mol/L, 2mol/L and 2mol/L respectively, get 5ml nickelous sulfate (2mol/L) and 2.5ml cobaltous sulfate (2mol/L) in the beaker of 250ml, add the 45ml deionized water again, nickelous sulfate cobalt after the dilution was heated 8 minutes in 90 ± 1 ℃ constant temperature water bath, then the NaOH (2mol/L) of 7.5ml is slowly poured in the nickelous sulfate cobalt liquor after the dilution, the limit bevelling stirs, and obtains the nickel hydroxide cobalt colloid of homogeneous at last.Nickel hydroxide cobalt colloid is placed the reactor of 100ml, sealing, insulation is 12 hours in 180 ℃ oil bath pan, naturally cooling, take out and use washed with de-ionized water 6 times, obtaining concentration is the nickel hydroxide cobalt nanowire suspension (wherein hydrogeneous cobalt nickel oxide nano wire 1.17 grams) of 0.018mol/L.Get the above-mentioned nickel hydroxide cobalt nanowire of 10ml suspension, be diluted to 45ml, handled 40 minutes in 600 watts of Ultrasound Instrument, place 90 ± 1 ℃ constant temperature water bath to heat again 10 minutes, behind acetic acid regulator solution pH=6, pour 3ml ortho phosphorous acid sodium solution (2mol/L) into the nickel hydroxide cobalt nanowire, add 1 palladium bichloride (1g/L) at last, reaction is acutely carried out, occur a large amount of black precipitates in the solution, the back washing is filtered in the black precipitate of gained, drying is 2 hours in 55 ℃ of baking ovens, nickel-cobalt in the gained powder-phosphorus is amorphous and crystallite attitude, obtains the nickel-cobalt-phosphorus nanotube of complete crystallization after 300 ℃ of heat treatment.Phosphorus content is 18% in last gained nickel-cobalt-phosphorus nanotube alloy powder, external diameter of pipe size 100-200nm, internal diameter size 40-100 nanometer, pipe range 3-6 micron.
The preparation of embodiment 4 Ni-Fes-phosphorus alloy nanotube
With nickelous sulfate, ferrous sulfate, inferior sodium phosphate and NaOH are mixed with the solution of 2mol/L, 2mol/L, 2mol/L and 2mol/L respectively, get 2ml nickelous sulfate (2mol/L) and 1ml ferrous sulfate (2mol/L) in the beaker of 250ml, add the 45ml deionized water again, sulfuric acid ferronickel after the dilution was heated 8 minutes in 90 ± 1 ℃ constant temperature water bath, then the NaOH (2mol/L) of 3ml is slowly poured in the nickelous sulfate ferrous solution after the dilution, the limit bevelling stirs, and obtains the hydroxide ferronickel colloid of homogeneous at last.Hydroxide ferronickel colloid is placed the reactor of 100ml, sealing, insulation is 24 hours in 120 ℃ oil bath pan, naturally cooling, take out and use washed with de-ionized water 6 times, obtaining concentration is the nickel hydroxide Fe nanowire suspension (wherein containing nickel hydroxide Fe nanowire 0.45 gram) of 0.018mol/L.Get the above-mentioned nickel hydroxide Fe nanowire of 10ml suspension, be diluted to 45ml, handled 20 minutes in 600 watts of Ultrasound Instrument, place 90 ± 1 ℃ constant temperature water bath to heat again 10 minutes, behind acetic acid regulator solution pH=12, pour 3ml ortho phosphorous acid sodium solution (2mol/L) into the nickel hydroxide Fe nanowire, add 1 palladium bichloride (1g/L) at last, reaction is acutely carried out, occur a large amount of black precipitates in the solution, the back washing is filtered in the black precipitate of gained, drying is 2 hours in 55 ℃ of baking ovens, Ni-Fe-phosphorus is amorphous and crystallite attitude in the gained powder, obtains the Ni-Fe-phosphorus nanotube of complete crystallization after 300 ℃ of heat treatment.Phosphorus content is 18% in last gained Ni-Fe-phosphorus nanotube alloy powder, external diameter of pipe size 60-200nm, internal diameter size 20-60 nanometer, pipe range 2-6 micron.
The preparation of embodiment 5 nickel-cobalt-iron-phosphorus alloy nanotube
With nickelous sulfate, cobaltous sulfate, ferrous sulfate, inferior sodium phosphate and potassium hydroxide are mixed with 2mol/L respectively, 2mol/L, 2mol/L, the solution of 2mol/L and 2mol/L, get 4ml nickelous sulfate (2mol/L), 1.5ml cobaltous sulfate (2mol/L), 1.5ml ferrous sulfate (2mol/L), in the beaker of 250ml, add the 45ml deionized water again, nickelous sulfate ferro-cobalt after the dilution was heated 8 minutes in 90 ± 1 ℃ constant temperature water bath, then the potassium hydroxide (2mol/L) of 7.5ml is slowly poured in the nickelous sulfate ferro-cobalt solution after the dilution, the limit bevelling stirs, and obtains the nickel hydroxide ferro-cobalt colloid of homogeneous at last.Nickel hydroxide ferro-cobalt colloid is placed the reactor of 100ml, sealing, insulation is 24 hours in 120 ℃ oil bath pan, naturally cooling, take out and use washed with de-ionized water 6 times, obtaining concentration is the nickel hydroxide ferro-cobalt nanowire suspension (wherein hydrogeneous cobalt nickel oxide Fe nanowire 1.06 grams) of 0.018mol/L.Get the above-mentioned nickel hydroxide ferro-cobalt of 10ml nanowire suspension, be diluted to 45ml, handled 20 minutes in 600 watts of Ultrasound Instrument, place 90 ± 1 ℃ constant temperature water bath to heat again 10 minutes, behind acetic acid regulator solution pH=4, pour 3ml ortho phosphorous acid sodium solution (2mol/L) into nickel hydroxide ferro-cobalt nano wire, add 1 palladium bichloride (1g/L) at last, reaction is acutely carried out, occur a large amount of black precipitates in the solution, the back washing is filtered in the black precipitate of gained, drying is 2 hours in 55 ℃ of baking ovens, nickel-cobalt in the gained powder-iron-phosphorus is amorphous and crystallite attitude, obtains the nickel-cobalt-iron-phosphorus nanotube of complete crystallization after 300 ℃ of heat treatment.Phosphorus content is 16% in last gained nickel-cobalt-iron-phosphorus nanotube alloy powder, external diameter of pipe size 80-180nm, internal diameter size 40-80 nanometer, pipe range 2-4 micron.
More than disclosed only be several specific embodiments of the application, but the application is not limited thereto, any those skilled in the art can think variation, all should drop in the application's the protection domain.
Claims (15)
1. the preparation method of a nickel or nickel alloy nanotube is characterized in that, may further comprise the steps:
(1) nickel salt solution or comprise the mixed salt solution of nickel salt and the aqueous slkali reaction generates the presoma colloid;
(2) described presoma colloid is handled under hydrothermal condition and is obtained nano wire;
(3) in above-mentioned nanowire surface generation catalytic reaction, be the reaction of active site catalytic reducer and nickel ion with the nanowire surface, form the tubular structure of nickel or nickel alloy.
2. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube is characterized in that, described step (1) further comprises:
Nickel salt solution or the mixed salt solution that comprises nickel salt are heated to T1, under agitation, pour aqueous slkali into nickel salt solution or comprise in the mixed salt solution of nickel salt, stir, obtain the presoma colloid of homogeneous.
3. the preparation method of nickel as claimed in claim 2 or nickel alloy nanotube, it is characterized in that, described nickel salt solution concentration or the total concentration that comprises the mixed salt solution of nickel salt are 0.1-0.3mol/L, and the concentration of described alkali lye is 0.1-0.3mol/L, and T1 is 50-80 ℃.
4. the preparation method of nickel as claimed in claim 1 or 2 or nickel alloy nanotube is characterized in that, described nickel salt be selected from nickelous sulfate, nickel chloride, nickel nitrate or nickel acetate wherein one or more.
5. the preparation method of nickel as claimed in claim 1 or 2 or nickel alloy nanotube, it is characterized in that the described mixed metal salt of nickel salt that comprises is for also comprising wherein one or more the mixed metal salt of cobaltous sulfate, cobalt acetate, cobalt nitrate, cobalt chloride, frerrous chloride, ferrous sulfate except comprising nickel salt.
6. the preparation method of nickel as claimed in claim 1 or 2 or nickel alloy nanotube is characterized in that, described alkali is selected from NaOH, potassium hydroxide, calcium hydroxide or ammoniacal liquor.
7. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube is characterized in that, described step (2) further comprises:
The presoma colloid is imported in the reactor, and the reactor sealing is incubated a period of time after reactor is heated to T2, and cooling naturally is taken out, and cleaning gets nano wire.
8. the preparation method of nickel as claimed in claim 7 or nickel alloy nanotube is characterized in that, T2 is 110-180 ℃, and temperature retention time is 12-48 hour.
9. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube is characterized in that, described step (3) further comprises:
Nano wire dilutes with appropriate amount of deionized water, ultrasonic processing 10-40 minute is heated to T3 afterwards, regulates the pH value to 2-12, reducing agent is heated to T4 to be poured in the nano wire afterwards, constantly stir simultaneously, drip little amount of catalyst, a large amount of bubbles are emerged subsequently, reaction is acutely carried out, occur a large amount of black precipitates in the solution, treat no longer to produce in the solution bubble, i.e. reaction is finished substantially.
10. the preparation method of nickel as claimed in claim 9 or nickel alloy nanotube is characterized in that, T3 is 80-95 ℃, and T4 is 80-95 ℃.
11. the preparation method as claim 1 or 9 described nickel or nickel alloy nanotube is characterized in that described reducing agent is selected from hypophosphite, boron hydride, hydrazine hydrate, sodium tungstate or potassium tungstate, the concentration of described reducing agent is 0.01-1mol/L.
12. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube is characterized in that, also comprises step (4):
The tubular structure of gained is respectively after ammoniacal liquor, deionized water, acetone washing, dry in baking oven, namely obtain nickel or nickel alloy nanotube through aftertreatment technology again.
13. the preparation method of nickel as claimed in claim 12 or nickel alloy nanotube is characterized in that, described aftertreatment technology is that 200～600 ℃ hydrogen reducing is handled.
14. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube, it is characterized in that, described nanotube is Powdered, include water, nickel hydroxide, nickel oxide, hydrogen and steam in the described nanotube, the nanotube external diameter is 60-300nm, internal diameter is the 20-100 nanometer, and pipe range is the 3-6 micron.
15. the preparation method of nickel as claimed in claim 1 or nickel alloy nanotube is characterized in that, the composition of described nanotube is binary, ternary or the quaternary alloy of pure nickel or nickel.
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| CN105033277A (en) * | 2015-08-13 | 2015-11-11 | 张弘 | Preparation technology of superfine spherical nickel, cobalt and iron ternary alloy powder |
| CN107952458A (en) * | 2017-11-02 | 2018-04-24 | 天津大学 | Preparation method applied to the nickel phosphorus catalyst of efficient electric catalyzing manufacturing of hydrogen |
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