CN114164445B - V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst - Google Patents
V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst Download PDFInfo
- Publication number
- CN114164445B CN114164445B CN202111682383.1A CN202111682383A CN114164445B CN 114164445 B CN114164445 B CN 114164445B CN 202111682383 A CN202111682383 A CN 202111682383A CN 114164445 B CN114164445 B CN 114164445B
- Authority
- CN
- China
- Prior art keywords
- fen
- catalyst
- full
- gts
- hydropower
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Active
Links
- 239000003054 catalyst Substances 0.000 title claims abstract description 41
- 238000006243 chemical reaction Methods 0.000 claims abstract description 26
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 23
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 16
- 239000010411 electrocatalyst Substances 0.000 claims abstract description 15
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 5
- 238000010438 heat treatment Methods 0.000 claims abstract description 5
- 239000002105 nanoparticle Substances 0.000 claims abstract description 5
- 238000001027 hydrothermal synthesis Methods 0.000 claims abstract description 4
- 238000011065 in-situ storage Methods 0.000 claims abstract description 4
- 238000005121 nitriding Methods 0.000 claims abstract description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 81
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 9
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 6
- 229910002804 graphite Inorganic materials 0.000 claims description 6
- 239000010439 graphite Substances 0.000 claims description 6
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 229910001030 Iron–nickel alloy Inorganic materials 0.000 claims description 3
- 229910017855 NH 4 F Inorganic materials 0.000 claims description 3
- 229910052786 argon Inorganic materials 0.000 claims description 3
- 238000001816 cooling Methods 0.000 claims description 3
- 239000012153 distilled water Substances 0.000 claims description 3
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 claims description 3
- 239000002243 precursor Substances 0.000 claims description 3
- 239000012300 argon atmosphere Substances 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims description 2
- 238000005303 weighing Methods 0.000 claims description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 16
- 239000001257 hydrogen Substances 0.000 abstract description 16
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 16
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 13
- 239000001301 oxygen Substances 0.000 abstract description 13
- 229910052760 oxygen Inorganic materials 0.000 abstract description 13
- 230000000694 effects Effects 0.000 abstract description 5
- 229910052759 nickel Inorganic materials 0.000 abstract description 3
- 239000012692 Fe precursor Substances 0.000 abstract 1
- 238000006460 hydrolysis reaction Methods 0.000 abstract 1
- 230000008707 rearrangement Effects 0.000 abstract 1
- 230000002195 synergetic effect Effects 0.000 abstract 1
- 230000003197 catalytic effect Effects 0.000 description 8
- NIPNSKYNPDTRPC-UHFFFAOYSA-N N-[2-oxo-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 NIPNSKYNPDTRPC-UHFFFAOYSA-N 0.000 description 7
- 238000010586 diagram Methods 0.000 description 6
- 238000001228 spectrum Methods 0.000 description 6
- 238000000354 decomposition reaction Methods 0.000 description 5
- 239000000463 material Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 238000013112 stability test Methods 0.000 description 4
- 229910052723 transition metal Inorganic materials 0.000 description 4
- 239000013078 crystal Substances 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- -1 transition metal nitrides Chemical class 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000000026 X-ray photoelectron spectrum Methods 0.000 description 2
- 239000004480 active ingredient Substances 0.000 description 2
- 230000002776 aggregation Effects 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 230000001588 bifunctional effect Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000003795 desorption Methods 0.000 description 2
- 125000005842 heteroatom Chemical group 0.000 description 2
- 238000002173 high-resolution transmission electron microscopy Methods 0.000 description 2
- 239000000543 intermediate Substances 0.000 description 2
- 230000000269 nucleophilic effect Effects 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 125000004429 atom Chemical group 0.000 description 1
- 230000006399 behavior Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000012876 carrier material Substances 0.000 description 1
- 238000003776 cleavage reaction Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000001747 exhibiting effect Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 150000001247 metal acetylides Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 150000003568 thioethers Chemical class 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
Classifications
-
- 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
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/054—Electrodes comprising electrocatalysts supported on a carrier
-
- 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
-
- 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
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/055—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the substrate or carrier material
-
- 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
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
-
- 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 V-Ni constructed based on doping and heterojunction strategies 3 FeN/Ni@N-GTs full-hydropower catalyst. Firstly, growing a V-doped Ni Fe precursor on a nitrogen-doped graphene tube carrier by a hydrothermal method, then heating to 470 ℃ in a tube furnace, introducing ammonia gas, and nitriding for 2 hours to obtain V-doped Ni which grows on the nitrogen-doped graphene tube in situ 3 Electrocatalyst comprising FeN and Ni nanoparticles, i.e. V-Ni 3 FeN/Ni@N-GTs. Based on V doping to Ni 3 Effective regulation and control of Ni, fe electronic structure in FeN, V-Ni 3 The electric charge rearrangement induced by the heterojunction interface of FeN and Ni and the synergistic effect of good conductivity and the like of the nitrogen-doped graphene tube carrier show excellent electrocatalytic activity and stability in hydrogen evolution reaction and oxygen evolution reaction in alkaline medium; simultaneously used as an anode catalyst and a cathode catalyst for catalyzing full hydrolysis reaction, and the cell voltage of only 1.55V can reach 10mA cm ‑2 And exhibits excellent stability.
Description
Technical Field
The invention belongs to the technical field of electrocatalytic materials, and particularly relates to a V-Ni constructed based on doping and heterojunction strategies 3 FeN/Ni@N-GTs full-hydropower catalystPreparation and application.
Background
Hydrogen energy is widely regarded as a sustainable alternative energy source by virtue of the advantages of higher mass specific energy density and no carbon emissions, and can solve the environmental problems caused by the consumption of traditional fossil energy sources. Electrocatalytic pyrolysis water is an effective way to obtain clean hydrogen fuel involving two half reactions: both cathodic Hydrogen Evolution (HER) and anodic Oxygen Evolution (OER) reactions are achieved depending on highly efficient electrocatalysts. To date, pt-and Ir/Ru-oxide based catalysts have remained considered ideal electrocatalysts for HER and OER. However, their large-scale commercial application is hampered by the expensive cost and relatively low reserves. A full-hydropower catalyst capable of having both HER and OER functions in the same electrolyte would reduce the cost of electrocatalytic cleavage of water. In recent years, some non-noble metal-based bifunctional electrocatalysts have been developed by researchers, mainly transition metal phosphides, sulfides, carbides, nitrides, and the like. Among them, transition metal nitrides are becoming ideal materials for full-hydropower catalysts by virtue of their low resistance, wide d-band, excellent corrosion resistance and good mechanical strength.
Since the surface electronic structure of the catalyst is a main factor affecting the catalytic activity, effective strategies can be adopted to optimize the catalyst electronic structure and improve the catalytic activity. First, heteroatom doping has been considered as an effective strategy for modulating the electronic structure of the procatalyst. The hetero atoms with different electronegativity are introduced into the transition metal nitride crystal lattice to induce the redistribution of electron density, and the electron structure of the main catalyst is accurately regulated and controlled, so that the adsorption and desorption behaviors of intermediates in the reaction process are optimized, and the activity of the catalyst is further improved. In addition, the heterojunction structure formed by materials with different work functions can induce charges to be rearranged at a heterogeneous interface to form a relatively stable local electrophilic/nucleophilic region, and can meet the requirement of an ideal hydrogen evolution and oxygen evolution bifunctional electrocatalyst on charge distribution. Finally, in order to improve the overall conductivity of the transition metal nitride, it is an effective method to introduce a carbon material having excellent conductivity as a skeletonMeanwhile, the agglomeration of active ingredients in the catalytic process can be avoided, and the exposed active sites are increased, so that the hydrogen evolution and oxygen evolution activities are improved. In summary, the method combines doping and heterojunction strategies, and prepares the V-doped Ni grown on the nitrogen-doped graphene tube in situ by using the nitrogen-doped graphene tube as a carrier through a hydrothermal and nitriding method 3 Full hydropower catalyst composed of FeN and Ni nano particles, namely V-Ni 3 FeN/Ni@N-GTs. The catalyst shows high-efficiency and stable electrocatalytic activity for hydrogen evolution and oxygen evolution reactions in alkaline medium. And by V-Ni 3 FeN/Ni@N-GTs are simultaneously used as a cathode catalyst and an anode catalyst to carry out full water decomposition to generate 10mA cm -2 Only a cell voltage of 1.55V is required and exhibits excellent stability.
Disclosure of Invention
The invention aims to provide a method for constructing V-Ni based on doping and heterojunction strategies 3 FeN/Ni@N-GTs full-hydropower catalyst. The specific invention comprises the following steps:
1. the nitrogen-doped graphene tube is used as a carrier, and V-doped Ni grown on the nitrogen-doped graphene tube in situ is obtained through a hydrothermal and nitriding method 3 Full hydropower catalyst V-Ni composed of FeN and Ni nano particles 3 FeN/Ni@N-GTs are prepared by the following method:
(1) Weigh 4mmol NH 4 F,8mmol CH 4 N 2 O and 0.08-0.15 mmol Na 3 VO 4 Dissolving in 70mL of distilled water, weighing 2mmol of nickel nitrate and ferric nitrate according to a molar ratio of 5:1, dissolving in the solution, transferring into a reaction kettle, immersing a nitrogen-doped graphene tube growing on a graphite sheet into the reaction kettle, performing a hydrothermal reaction at a reaction temperature of 120 ℃ for 6 hours, and washing and drying a product to obtain a V-doped NiFe precursor loaded on the nitrogen-doped graphene tube;
(2) Placing the product obtained in the step (1) into a tubular furnace, heating to 470 ℃ in an argon atmosphere, closing argon, introducing ammonia gas for 2 hours at the set temperature, and cooling to room temperature to obtain the full-hydropower catalyst V-Ni 3 FeN/Ni@N-GTs。
2. The full-hydroelectric catalyst V-Ni 3 FeN/Ni@N-GTs show excellent electrocatalytic performance in alkaline medium, and can reach 10mA cm only by using a cell voltage of 1.55V as a full-hydropower catalyst -2 And exhibits excellent stability.
The V-Ni constructed based on doping and heterojunction strategies 3 Compared with the prior art, the FeN/Ni@N-GTs full-hydropower catalyst has the advantages that:
(1) Heterogeneous atom V is introduced into the electrocatalyst, and host material Ni is accurately regulated and controlled 3 The electronic structures of Ni and Fe in FeN are optimized, so that the adsorption and desorption actions of an intermediate in the reaction process are optimized, and the activity of the catalyst is improved;
(2) Doping Ni with V 3 The heterojunction formed by the FeN and Ni nano particles can induce charges to be rearranged at a heterogeneous interface, so that a relatively stable local electrophilic/nucleophilic region is formed, and the catalytic activity of hydrogen evolution/oxygen evolution of the heterojunction is respectively improved;
(3) The nitrogen doped graphene tube with excellent conductivity is introduced as a carrier, so that the overall conductivity of the catalyst can be improved, the aggregation of active ingredients in the catalytic process can be avoided, and the exposed active sites are increased, so that the hydrogen evolution and oxygen evolution performances are improved.
Drawings
FIG. 1 is a schematic diagram of a full water-splitting catalyst V-Ni prepared in example 1 3 SEM photograph of FeN/Ni@N-GTs, (a) 2 μm, (b) 500nm;
FIG. 2 is a schematic diagram showing a full water-splitting catalyst V-Ni obtained in example 1 3 TEM (a) photographs of FeN/Ni@N-GTs, and HRTEM (b);
FIG. 3 is a full water-splitting catalyst V-Ni prepared in example 1 3 XRD spectra of FeN/Ni@N-GTs;
FIG. 4 shows a full water-splitting catalyst V-Ni prepared in example 1 3 XPS spectrum of FeN/Ni@N-GTs, (a) V2 p spectrum, (b) Ni 2p spectrum, and (c) Fe 2p spectrum;
FIG. 5 shows the electrocatalyst V-Ni prepared in example 1 3 Hydrogen evolution reaction Performance graph of FeN/Ni@N-GTs in 1mol/L KOH solution for electrocatalytically decomposing water, (a) LSV graph (iR correction), (b) Tafel slope plot, (c) stability test plot;
FIG. 6 shows the electrocatalyst V-Ni prepared in example 1 3 Oxygen evolution reaction performance diagram of FeN/Ni@N-GTs in 1mol/L KOH solution for electrocatalytically decomposing water, (a) LSV curve diagram (iR correction), (b) Tafel slope diagram, (c) stability test diagram;
FIG. 7 shows the electrocatalyst V-Ni prepared in example 1 3 FeN/Ni@N-GTs are used as cathode and anode catalysts simultaneously and are applied to an electrocatalytic full water decomposition performance graph, (a) an LSV curve graph (iR correction) and (b) a stability test graph.
Detailed Description
The present invention is described in further detail below in connection with specific examples, which, however, do not limit the scope of the invention in any way.
Example 1
The full hydropower catalyst V-Ni of this example 3 The preparation method of the FeN/Ni@N-GTs comprises the following steps:
(1) Weigh 0.108mmol Na 3 VO 4 、4mmol NH 4 F and 8mmol CH 4 N 2 O is dissolved in 70mL of distilled water, 2mmol of nickel nitrate and ferric nitrate are weighed according to the mol ratio of 5:1, dissolved in the solution, transferred to a reaction kettle (100 mL), and simultaneously, a nitrogen-doped graphene tube growing on a graphite sheet is immersed in the reaction kettle for hydrothermal reaction, the reaction temperature is 120 ℃, the reaction time is 6h, and then the product is washed and dried, so that a V-doped NiFe precursor loaded on the nitrogen-doped graphene tube is obtained;
(2) Putting the product obtained in the step (1) into a tubular furnace, heating to 470 ℃ at 5 ℃/min in Ar atmosphere, closing argon, introducing ammonia gas for 2h at the temperature, and cooling to room temperature to obtain the full-hydropower catalyst V-Ni 3 FeN/Ni@N-GTs。
SEM pictures of different magnifications of the full-hydropower catalyst are shown in figures 1 (a) and (b) in the specification, and the carrier material is uniformly tubular, the diameter is 200-250 nm, and the V-Ni 3 FeN/Ni is granular and uniformly anchored on the surface of the nitrogen-doped graphene tube, and the grain size is 10-30 nm. TEM and HRTEM pictures of the fluorescent lamp are shown in the specificationIn the drawings, FIGS. 2 (a), (b), it is clear from FIG. 2 (a) that V-Ni 3 The granular structure of FeN/Ni is clearly seen from FIG. 2 (b) as two different interplanar spacings d where a lattice fringe having a d value of 0.203nm corresponds to the (111) crystal plane of metallic Ni and a lattice fringe having a d value of 0.266nm corresponds to Ni 3 The (110) crystal plane of FeN, the result confirms the V-Ni in the product 3 Successful preparation of FeN/Ni heterojunction. The XRD patterns are shown in figure 3, and the characteristic peaks at 41.3 degrees, 48.0 degrees, 70.3 degrees and 85.2 degrees are matched with Ni 3 The (1 1 1), (2 0), (2 2 0) and (3 1) planes of FeN coincide (JCDF # 50-1434), characteristic peaks at 44.3 DEG, 51.6 DEG and 76.1 DEG are attributed to the (1 1 1), (2 0) and (3 1) planes of Ni (JCDF # 04-0850), and this result confirms that Ni in the product 3 FeN coexists with Ni. The XPS spectrum of figure 4 characterizes the surface composition and chemical valence state of the full hydropower catalyst, and the V element is successfully doped into Ni as can be seen from the V spectrum of figure 4 (a) 3 As can be seen from the Ni 2p spectra of FIG. 4 (b) and the Fe 2p spectra of FIG. 4 (c), in FeN, compared with undoped Ni 3 FeN, doped Ni 3 The d-band centers of Ni and Fe in FeN are shifted to the low-energy direction, which shows that the doping of V element effectively adjusts Ni 3 Electronic structure of FeN.
The electrocatalytic performance test of the product adopts a three-electrode system, and the V-Ni is loaded 3 The graphite sheet of the FeN/Ni@N-GTs electrocatalyst is used as a working electrode, a Pt electrode (oxygen evolution reaction) and a graphite electrode (hydrogen evolution reaction) are used as counter electrodes, a Hg/HgO electrode is used as a reference electrode, a KOH aqueous solution of 1mol/L is used as electrolyte, and a CHI 760E electrochemical workstation is used for testing the catalytic activity and stability of the hydrogen evolution reaction and the oxygen evolution reaction of the product. FIG. 5 (a), (b) and (c) are the electrocatalysts V-Ni prepared in this example 3 Performance of FeN/Ni@N-GTs for electrocatalytic decomposition water hydrogen evolution reaction, as can be seen from the graph, the catalyst has a current density of 10mA cm -2 At the time of hydrogen evolution reaction, the overpotential was 66mV and the Tafel slope was 88mV dec -1 And at 10mAcm -2 The lower part can be kept for 35 hours without obvious change of current density, which shows that the hydrogen evolution device has good hydrogen evolution stability; FIG. 6 (a), (b) and (c) are the electrocatalysts V-Ni prepared in this example 3 Performance of FeN/Ni@N-GTs for electrocatalytic decomposition of water to oxygen reaction, as can be seen from the graph, the catalyst has a current density of 10mA cm -2 When the overpotential of the oxygen evolution reaction was 252mV, the Tafel slope was 29mV dec -1 And at 10mA cm -2 The lower part can be kept for 35 hours without obvious change of current density, which shows that the oxygen evolution stability is good.
The graphite sheet carrying the product of example 1 was used as both anode and cathode, a two-electrode system electrolytic cell was constructed, 1mol/L KOH aqueous solution was used as electrolyte, and the catalytic activity and stability of the electrode for catalyzing full water decomposition were tested by using CHI 660E electrochemical workstation, as shown in FIG. 7 (a) and (b), the electrocatalyst V-Ni prepared in this example 3 FeN/Ni@N-GTs have excellent electrocatalytic full water dissolving performance and generate 10mA cm -2 Only a cell voltage of 1.55V was required and the catalytic activity was kept substantially unchanged by the 35 hour current stability test, exhibiting excellent stability.
Claims (3)
1. V-Ni constructed based on doping and heterojunction strategy 3 The FeN/Ni@N-GTs full-hydropower catalyst is characterized in that V doped Ni grown on a nitrogen doped graphene tube in situ is obtained through a hydrothermal and nitriding method 3 The full-hydropower catalyst composed of FeN and Ni nano particles is characterized by being prepared by the following steps:
(1) Weigh 4mmol NH 4 F,8mmol CH 4 N 2 O and 0.08-0.15 mmol Na 3 VO 4 Dissolving in 70mL of distilled water, weighing 2mmol of nickel nitrate and ferric nitrate according to a molar ratio of 5:1, dissolving in the solution, transferring into a reaction kettle, immersing a nitrogen-doped graphene tube growing on a graphite sheet into the reaction kettle, performing a hydrothermal reaction at a reaction temperature of 120 ℃ for 6 hours, and washing and drying a product to obtain a V-doped NiFe precursor loaded on the nitrogen-doped graphene tube;
(2) Placing the product obtained in the step (1) into a tube furnace, heating to a set temperature in an argon atmosphere, closing argon, and introducing at the set temperatureAfter ammonia gas for a certain time, cooling to room temperature to obtain the full-hydropower catalyst V-Ni 3 FeN/Ni@N-GTs。
2. The full hydropower catalyst V-Ni as defined in claim 1 3 The FeN/Ni@N-GTs are characterized in that the heating rate in the step (2) is 5 ℃/min, the set temperature is 470 ℃, and the ammonia gas introducing time is 2h.
3. The full hydropower catalyst V-Ni as defined in claim 1 3 The FeN/Ni@N-GTs are characterized in that the electrocatalyst shows excellent electrocatalyst performance in alkaline medium, and can reach 10mA cm only by 1.55V cell voltage as a full-hydropower catalyst -2 And exhibits excellent stability.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN202111682383.1A CN114164445B (en) | 2021-12-30 | 2021-12-30 | V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN202111682383.1A CN114164445B (en) | 2021-12-30 | 2021-12-30 | V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst |
Publications (2)
Publication Number | Publication Date |
---|---|
CN114164445A CN114164445A (en) | 2022-03-11 |
CN114164445B true CN114164445B (en) | 2024-03-26 |
Family
ID=80489054
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
CN202111682383.1A Active CN114164445B (en) | 2021-12-30 | 2021-12-30 | V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst |
Country Status (1)
Country | Link |
---|---|
CN (1) | CN114164445B (en) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN114606512B (en) * | 2022-03-30 | 2023-08-22 | 青岛科技大学 | Ru doped W 4.6 N 4 Particle @ nitrogen doped graphene tube hydrogen evolution electrocatalyst |
CN114752946B (en) * | 2022-04-11 | 2023-06-20 | 四川大学 | Preparation method of electrocatalytic electrolysis water bipolar plate |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2017091955A1 (en) * | 2015-11-30 | 2017-06-08 | South University Of Science And Technology Of China | Bifunctional electrocatalyst for water splitting and preparation method thereof |
CN106887576A (en) * | 2017-03-22 | 2017-06-23 | 中国科学院理化技术研究所 | Carrier loaded nano silicon nitride ferronickel composite of the nitrogen co-doped nitrogen carbon material of a kind of cobalt and its preparation method and application |
CN113659153A (en) * | 2021-07-13 | 2021-11-16 | 江苏大学 | Preparation method of bifunctional transition metal nitride heterojunction electrocatalyst for oxygen reduction/oxygen precipitation reaction |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10815580B2 (en) * | 2017-08-10 | 2020-10-27 | Board Of Trustees Of The University Of Arkansas | 3D reduced graphene oxide foams embedded with nanocatalysts, synthesizing methods and applications of same |
-
2021
- 2021-12-30 CN CN202111682383.1A patent/CN114164445B/en active Active
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2017091955A1 (en) * | 2015-11-30 | 2017-06-08 | South University Of Science And Technology Of China | Bifunctional electrocatalyst for water splitting and preparation method thereof |
CN106887576A (en) * | 2017-03-22 | 2017-06-23 | 中国科学院理化技术研究所 | Carrier loaded nano silicon nitride ferronickel composite of the nitrogen co-doped nitrogen carbon material of a kind of cobalt and its preparation method and application |
CN113659153A (en) * | 2021-07-13 | 2021-11-16 | 江苏大学 | Preparation method of bifunctional transition metal nitride heterojunction electrocatalyst for oxygen reduction/oxygen precipitation reaction |
Non-Patent Citations (2)
Title |
---|
Engineering the electronic states of Ni3FeN via zinc ion regulation for promoting oxygen electrocatalysis in rechargeable Zn–air batteries;He Xiaoyang, et al.;J. Mater. Chem. A(第9期);2301-2307 * |
Improving the HER activity of Ni3FeN to convert the superior OER electrocatalyst to an efficient bifunctional electrocatalyst for overall water splitting by doping with molybdenum;Liu Xiaolei, et al.;Electrochimica Acta(第333期);135488 * |
Also Published As
Publication number | Publication date |
---|---|
CN114164445A (en) | 2022-03-11 |
Similar Documents
Publication | Publication Date | Title |
---|---|---|
Cao et al. | Aqueous electrocatalytic N 2 reduction under ambient conditions | |
Yang et al. | Advances and challenges of Fe-MOFs based materials as electrocatalysts for water splitting | |
Gao et al. | One-step preparation of cobalt-doped NiS@ MoS2 core-shell nanorods as bifunctional electrocatalyst for overall water splitting | |
Song et al. | Amorphous MoS2 coated Ni3S2 nanosheets as bifunctional electrocatalysts for high-efficiency overall water splitting | |
Li et al. | Heterostructured MoO2@ MoS2@ Co9S8 nanorods as high efficiency bifunctional electrocatalyst for overall water splitting | |
Cao et al. | Improved hydrogen generation via a urea-assisted method over 3D hierarchical NiMo-based composite microrod arrays | |
Zhou et al. | Surface reconstruction and charge distribution enabling Ni/W5N4 Mott-Schottky heterojunction bifunctional electrocatalyst for efficient urea-assisted water electrolysis at a large current density | |
Zhao et al. | Hierarchical Ni3S2-CoMoSx on the nickel foam as an advanced electrocatalyst for overall water splitting | |
CN114164445B (en) | V-Ni constructed based on doping and heterojunction strategy 3 FeN/Ni@N-GTs full-hydropower catalyst | |
Wang et al. | Cu–MoS2/rGO hybrid material for enhanced hydrogen evolution reaction performance | |
Lu et al. | Co-doped NixPy loading on Co3O4 embedded in Ni foam as a hierarchically porous self-supported electrode for overall water splitting | |
Qu et al. | Ni2P/C nanosheets derived from oriented growth Ni-MOF on nickel foam for enhanced electrocatalytic hydrogen evolution | |
Zhao et al. | Cobalt-molybdenum carbide@ graphitic carbon nanocomposites: metallic cobalt promotes the electrochemical hydrogen evolution reaction | |
Pan et al. | Activation of rhodium selenides for boosted hydrogen evolution reaction via heterostructure construction | |
Sun et al. | One-pot synthesis of N and P Co-doped carbon layer stabilized cobalt-doped MoP 3D porous structure for enhanced overall water splitting | |
CN111617780B (en) | Nitrogen-doped nickel-molybdenum-based composite sulfide for stable hydrogen production by water electrolysis and preparation method thereof | |
Zhang et al. | Nitrogen doped carbon encapsulated hierarchical NiMoN as highly active and durable HER electrode for repeated ON/OFF water electrolysis | |
Wu et al. | Self-supported hollow Co (OH) 2/NiCo sulfide hybrid nanotube arrays as efficient electrocatalysts for overall water splitting | |
Wang et al. | Homogeneous pseudoamorphous metal phosphide clusters for ultra stable hydrogen generation by water electrolysis at industrial current density | |
CN111229267B (en) | Supported phosphorus-doped metal oxyhydroxide nanosheet material and preparation method and application thereof | |
Liu et al. | Catkin-derived mesoporous carbon-supported molybdenum disulfide and nickel hydroxyl oxide hybrid as a bifunctional electrocatalyst for driving overall water splitting | |
Duan et al. | Bifunctional CoP electrocatalysts for overall water splitting | |
Lin et al. | Rapid fabrication of FexNi2− xP4O12 and graphene hybrids as electrocatalyst for highly efficient oxygen evolution reaction | |
Liu et al. | Valence regulation of Ru/Mo2C heterojunction for efficient acidic overall water splitting | |
Li et al. | MoP-NC nanosphere supported Pt nanoparticles for efficient methanol electrolysis |
Legal Events
Date | Code | Title | Description |
---|---|---|---|
PB01 | Publication | ||
PB01 | Publication | ||
SE01 | Entry into force of request for substantive examination | ||
SE01 | Entry into force of request for substantive examination | ||
GR01 | Patent grant | ||
GR01 | Patent grant |