CN111804302A - Cobalt-based electrocatalyst and low-voltage hydrogen production electrolytic cell thereof - Google Patents
Cobalt-based electrocatalyst and low-voltage hydrogen production electrolytic cell thereof Download PDFInfo
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- CN111804302A CN111804302A CN202010712627.5A CN202010712627A CN111804302A CN 111804302 A CN111804302 A CN 111804302A CN 202010712627 A CN202010712627 A CN 202010712627A CN 111804302 A CN111804302 A CN 111804302A
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- electrolytic cell
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- based electrocatalyst
- hydrogen
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- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 32
- 239000001257 hydrogen Substances 0.000 title claims abstract description 32
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 32
- 239000010411 electrocatalyst Substances 0.000 title claims abstract description 25
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 21
- 229910017052 cobalt Inorganic materials 0.000 title claims description 17
- 239000010941 cobalt Substances 0.000 title claims description 17
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 title claims description 17
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims abstract description 47
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 19
- 239000003792 electrolyte Substances 0.000 claims abstract description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 11
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 6
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 5
- 238000001354 calcination Methods 0.000 claims description 5
- 239000004202 carbamide Substances 0.000 claims description 5
- 229910052759 nickel Inorganic materials 0.000 claims description 5
- 239000002243 precursor Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- 229910052786 argon Inorganic materials 0.000 claims description 3
- 238000001816 cooling Methods 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 3
- -1 polytetrafluoroethylene Polymers 0.000 claims description 3
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 3
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 3
- 239000000243 solution Substances 0.000 claims description 3
- 238000005406 washing Methods 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 2
- 238000000034 method Methods 0.000 abstract description 6
- 230000007613 environmental effect Effects 0.000 abstract description 2
- 229910000428 cobalt oxide Inorganic materials 0.000 abstract 2
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 abstract 2
- 230000001590 oxidative effect Effects 0.000 abstract 1
- 235000011187 glycerol Nutrition 0.000 description 13
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000005868 electrolysis reaction Methods 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 239000002028 Biomass Substances 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000010349 cathodic reaction Methods 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 239000002073 nanorod Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
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Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/75—Cobalt
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/755—Nickel
-
- B01J35/23—
-
- B01J35/33—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- 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
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
The invention discloses a low-voltage hydrogen production electrolytic cell, which takes cobalt oxide as an electrocatalyst, takes glycerol-KOH as electrolyte and electrolyzes water to produce hydrogen with high efficiency. The prepared cobalt oxide electrocatalyst is used as a cathode and an anode respectively to construct an electrolytic cell, and a large amount of hydrogen is produced in the process of oxidizing water and glycerol, so that the method has good environmental protection benefit and economic benefit.
Description
Technical Field
The invention relates to an electrolytic cell with high-efficiency hydrogen production performance under low voltage.
Background
In recent years, development of new clean energy has been accelerated by increasingly serious energy and environmental problems. The hydrogen energy is a recognized clean energy source, the hydrogen energy is high, the combustion product is water and has no pollution, and the hydrogen energy is taken as a zero-carbon energy source. At present, the hydrogen production method mainly comprises water electrolysis, biomass hydrogen production, fossil fuel hydrogen production and the like; the latter two methods, however, produce environmental pollutants, while the electrolytic cell produces hydrogen without pollutants, and are a good choice. However, the hydrogen production efficiency of the traditional water electrolysis reaction is mainly limited by the oxidation half reaction, the reaction kinetics is slow, and a higher overpotential is needed. In the prior report, Tantai provides a water electrolysis hydrogen production system (application publication No. CN 102758212A), the invention relates to a method and a device for producing hydrogen by electrolyzing water at low voltage, but the invention has too many additional devices and complicated devices; in addition, the polar plate made of the activated carbon has higher cost, and each operation link has corresponding errors. Wangyonggang and the like relate to a device and a method for producing hydrogen by electrolyzing water by a two-step method in a three-electrode system double-electrolytic cell (application publication number: CN 105734600A), and like the traditional water electrolysis, the device and the method need higher external voltage, consume more energy and have high hydrogen production cost. Therefore, the invention designs the electrolytic cell which is simple and easy to implement, low in cost and high in hydrogen production efficiency, and has important practical application significance.
Disclosure of Invention
The invention aims to solve the defects in the prior art and provide the electrolytic cell which is simple and easy to implement, low in cost and high in hydrogen production efficiency.
In order to achieve the purpose, the invention provides the following technical scheme:
a cobalt-based electrocatalyst, prepared by the steps of:
(1) 30ml of water is taken, and 3 mmol of Co (NO) is added under the condition of stirring3)2•6H2O;
(2) Then adding 15 mmol of urea, and stirring for 30 minutes;
(3) adding the mixed solution stirred in the step (2) and the cleaned nickel sheet into a polytetrafluoroethylene lining, carrying out hydrothermal reaction at constant temperature of 120 ℃ for 6 hours, naturally cooling to room temperature, centrifuging, washing and drying to obtain a precursor/NF;
(4) and (4) placing the precursor/NF prepared in the step (3) in a tubular furnace, and calcining at the constant temperature of 350 ℃ for 1 hour to obtain the cobalt-based electrocatalyst.
Wherein, the size specification of the nickel sheet in the step (3) is 2 cm multiplied by 4 cm. And (4) calcining in argon to obtain CoO/NF.
The invention provides an electrolytic cell prepared by adopting the cobalt-based electrocatalyst, which takes the cobalt-based electrocatalyst as a cathode and an anode.
The electrolytic cell takes KOH and glycerol solution as electrolyte; the concentration of KOH in the electrolyte was 1M, and the concentration of glycerol was 0.5M.
The electrolytic cell applies a voltage of 0.1-0.6V in the hydrogen production process.
Compared with the prior art, the invention has the following advantages:
1. the invention takes the oxide of cobalt as the electro-catalyst, and utilizes the electrolytic cell to electrically oxidize the glycerol pollutants and simultaneously improve the hydrogen production efficiency.
2. In the invention, urea is added in the preparation process of the cobalt-based electrocatalyst, and the CoO/NF electrocatalyst is prepared by utilizing the reduction action of the urea at high temperature.
3. Compared with the traditional electrolytic water system, the electrolytic cell provided by the invention adopts a glycerol electrolytic system, so that glycerol pollutants are oxidized and decomposed, the cell voltage is effectively reduced, and high-efficiency hydrogen production is realized.
Drawings
FIG. 1 is an X-ray diffraction (XRD) pattern of a cobalt-based electrocatalyst, CoO/NF, prepared according to one embodiment of the present invention;
FIG. 2 is a Scanning Electron Micrograph (SEM) of a cobalt-based electrocatalyst CoO/NF prepared according to one embodiment of the present invention;
FIG. 3 is a schematic view of an electrolytic cell according to a second embodiment of the present invention; in the figure, the cathode and the anode are tested by using the electrocatalyst prepared in the first example and using 1MKOH and 1MKOH +0.5M glycerol as electrolytes respectively;
FIG. 4 shows the results of Oxygen Evolution Reaction (OER) and Hydrogen Evolution Reaction (HER) tests of an electrolytic cell constructed with the CoO/NF electrocatalyst as the cathode and anode in example two.
Detailed Description
The present invention will be described in detail with reference to specific examples.
Example one preparation example of a cobalt-based electrocatalyst
In a beaker, 3 mmol of Co (NO) at room temperature3)2•6H2Stirring O and 15 mmol urea in a beaker with 30ml water solution for 30 minutes, transferring to a polytetrafluoroethylene lining, putting a clean nickel sheet, and carrying out hydrothermal reaction at constant temperature of 120 ℃ for 6 hours; after reacting for 6 hours, naturally cooling to room temperature, washing, centrifuging and drying to obtain the product, namely the precursor. And putting the product into a muffle furnace, and calcining and reacting for 1 hour at the constant temperature of 350 ℃ in argon to obtain the CoO/NF.
As shown in FIG. 1, the resulting product was prepared in accordance with CoO Standard card (JCPDS: number 48-1719) as a pure phase CoO electrocatalyst. As shown in FIG. 2, the prepared CoO is a nanorod with an average length of 3 μm.
Example two: electrolytic cell construction and test examples
The test procedure was as follows:
as shown in FIG. 3, the CoO/NF (NF: Ni plate) electrocatalyst prepared in example one was used as a cathode and an anode, and Oxygen Evolution Reaction (OER) and Hydrogen Evolution Reaction (HER) tests were performed in 1MKOH and 1MKOH +0.5M glycerol, respectively, with a constant voltage applied.
As can be seen from fig. 4, the co/NF electrocatalyst is used as the cathode and anode to effectively perform the water electrolysis reaction with the relative hydrogen production efficiency, and the addition of glycerol not only promotes the oxidation current density of water but also promotes the hydrogen production efficiency. For anodic oxidation reactionIn water electrolysis systems, the oxidation reaction of water requires a higher voltage of 0.497V to reach 50mA cm-2While the glycerol electrolysis system can reach 50mA cm only by 0.283V-2. For the cathodic reaction, HER of the electrolytic water system and the glycerol electrolytic system respectively need voltages of-1.478V and-1.389V to reach 50mA cm-2. To reach 50mA cm-2The cell voltage of the conventional electrolytic water system needs 1.975V, while the cell voltage of the glycerin electrolytic system is 1.672V, which is reduced by 0.303V. This is because the glycerol oxidation reaction greatly promotes the Hydrogen Evolution Reaction (HER) instead of the slow four-electron OER reaction. Therefore, the glycerol electrolytic cell has excellent hydrogen production efficiency.
Claims (6)
1. A cobalt-based electrocatalyst, characterized in that it is prepared by the steps of:
(1) 30ml of water is taken, and 3 mmol of Co (NO) is added under the condition of stirring3)2•6H2O;
(2) Then adding 15 mmol of urea, and stirring for 30 minutes;
(3) adding the mixed solution stirred in the step (2) and the cleaned nickel sheet into a polytetrafluoroethylene lining, carrying out hydrothermal reaction at constant temperature of 120 ℃ for 6 hours, naturally cooling to room temperature, centrifuging, washing and drying to obtain a precursor/NF;
(4) and (4) placing the precursor/NF prepared in the step (3) in a tubular furnace, and calcining at the constant temperature of 350 ℃ for 1 hour to obtain the cobalt-based electrocatalyst.
2. A cobalt-based electrocatalyst according to claim 1, characterised in that the calcination in step (4) is carried out in argon.
3. The cobalt-based electrocatalyst according to claim 2, wherein the nickel sheet has a size specification of 2 cm x 4 cm.
4. A low-voltage hydrogen-producing electrolytic cell produced by using the cobalt-based electrocatalyst according to any one of claims 1 to 3, wherein the cobalt-based electrocatalyst is used as a cathode and an anode.
5. The low-voltage hydrogen-producing electrolytic cell according to claim 4, wherein the electrolytic cell takes KOH and glycerol solution as electrolyte; the concentration of KOH in the electrolyte is 1M, and the concentration of glycerol is 0.5M.
6. The low-voltage hydrogen-production electrolytic cell according to claim 5, wherein the electrolytic cell applies a voltage of 0.1-0.6V in the hydrogen production process.
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114086202A (en) * | 2021-11-20 | 2022-02-25 | 南昌航空大学 | Non-noble metal catalyst for glycerol oxidation-assisted hydrogen production |
Citations (2)
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CN106807378A (en) * | 2015-11-27 | 2017-06-09 | 中国科学院大连化学物理研究所 | A kind of hexagon nickel cobalt oxide oxygen-separating catalyst and its preparation method and application |
CN109939711A (en) * | 2019-03-07 | 2019-06-28 | 华东师范大学 | Glycerol auxiliary water decomposing hydrogen-production and the bifunctional electrocatalyst and preparation method of glycerol oxidation |
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- 2020-07-22 CN CN202010712627.5A patent/CN111804302A/en active Pending
Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN106807378A (en) * | 2015-11-27 | 2017-06-09 | 中国科学院大连化学物理研究所 | A kind of hexagon nickel cobalt oxide oxygen-separating catalyst and its preparation method and application |
CN109939711A (en) * | 2019-03-07 | 2019-06-28 | 华东师范大学 | Glycerol auxiliary water decomposing hydrogen-production and the bifunctional electrocatalyst and preparation method of glycerol oxidation |
Non-Patent Citations (2)
Title |
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SHASHA ZHU,等: "CoO/NF nanowires promote hydrogen and oxygen production for overall water splitting in alkaline media", 《INTERNATIONAL JOURNAL OF HYDROGEN ENERGY》 * |
V.L. OLIVEIRA ET AL.: "Studies of the reaction products resulted from glycerolelectrooxidation on Ni-based materials in alkaline medium", 《ELECTROCHIMICA ACTA》 * |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114086202A (en) * | 2021-11-20 | 2022-02-25 | 南昌航空大学 | Non-noble metal catalyst for glycerol oxidation-assisted hydrogen production |
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Application publication date: 20201023 |