CN107240641B - The preparation method of nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide - Google Patents
The preparation method of nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide Download PDFInfo
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- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 59
- 150000002910 rare earth metals Chemical class 0.000 title claims abstract description 48
- 238000005984 hydrogenation reaction Methods 0.000 title claims abstract description 46
- 238000002360 preparation method Methods 0.000 title claims abstract description 25
- 239000000463 material Substances 0.000 claims abstract description 65
- 238000000034 method Methods 0.000 claims abstract description 30
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 17
- 230000004913 activation Effects 0.000 claims abstract description 14
- 230000015556 catabolic process Effects 0.000 claims abstract description 14
- 239000013078 crystal Substances 0.000 claims abstract description 13
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 7
- 238000001914 filtration Methods 0.000 claims abstract description 6
- 230000008569 process Effects 0.000 claims abstract description 6
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 125
- 229910052697 platinum Inorganic materials 0.000 claims description 55
- 239000010408 film Substances 0.000 claims description 37
- 230000003197 catalytic effect Effects 0.000 claims description 29
- 239000010409 thin film Substances 0.000 claims description 20
- 239000001257 hydrogen Substances 0.000 claims description 17
- 229910052739 hydrogen Inorganic materials 0.000 claims description 17
- 150000001875 compounds Chemical class 0.000 claims description 16
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 15
- 230000005611 electricity Effects 0.000 claims description 15
- 238000006555 catalytic reaction Methods 0.000 claims description 12
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 11
- 230000008859 change Effects 0.000 claims description 11
- 230000009471 action Effects 0.000 claims description 8
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 7
- 230000000694 effects Effects 0.000 claims description 6
- 229910052763 palladium Inorganic materials 0.000 claims description 5
- 239000000758 substrate Substances 0.000 claims description 5
- 229910052693 Europium Inorganic materials 0.000 claims description 4
- 229910052779 Neodymium Inorganic materials 0.000 claims description 3
- 229910052772 Samarium Inorganic materials 0.000 claims description 3
- 150000002431 hydrogen Chemical class 0.000 claims description 3
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 2
- 239000003054 catalyst Substances 0.000 claims description 2
- 238000004845 hydriding Methods 0.000 claims description 2
- 125000004430 oxygen atom Chemical group O* 0.000 claims description 2
- 239000002689 soil Substances 0.000 claims description 2
- 238000002604 ultrasonography Methods 0.000 claims description 2
- 229910052702 rhenium Inorganic materials 0.000 claims 4
- 238000003487 electrochemical reaction Methods 0.000 claims 1
- 230000003993 interaction Effects 0.000 claims 1
- 239000012212 insulator Substances 0.000 abstract description 15
- 229910052751 metal Inorganic materials 0.000 abstract description 15
- 239000002184 metal Substances 0.000 abstract description 15
- 230000007704 transition Effects 0.000 abstract description 12
- 230000005012 migration Effects 0.000 abstract description 9
- 238000013508 migration Methods 0.000 abstract description 9
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 abstract description 8
- 230000005684 electric field Effects 0.000 abstract description 5
- 239000004065 semiconductor Substances 0.000 abstract description 4
- 239000011787 zinc oxide Substances 0.000 abstract description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 abstract description 3
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 abstract description 3
- 239000002245 particle Substances 0.000 abstract description 2
- ZYYBOACWJZNWQT-UHFFFAOYSA-N oxonickel samarium Chemical compound [Sm].[Ni]=O ZYYBOACWJZNWQT-UHFFFAOYSA-N 0.000 description 20
- 238000005259 measurement Methods 0.000 description 15
- 239000007789 gas Substances 0.000 description 12
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 10
- 229910052710 silicon Inorganic materials 0.000 description 10
- 239000010703 silicon Substances 0.000 description 10
- 241000209094 Oryza Species 0.000 description 8
- 235000007164 Oryza sativa Nutrition 0.000 description 8
- 235000009566 rice Nutrition 0.000 description 8
- VIKNJXKGJWUCNN-XGXHKTLJSA-N norethisterone Chemical compound O=C1CC[C@@H]2[C@H]3CC[C@](C)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 VIKNJXKGJWUCNN-XGXHKTLJSA-N 0.000 description 6
- YZCKVEUIGOORGS-IGMARMGPSA-N Protium Chemical compound [1H] YZCKVEUIGOORGS-IGMARMGPSA-N 0.000 description 4
- 241000720974 Protium Species 0.000 description 4
- -1 strontium rubidium oxygen Chemical compound 0.000 description 4
- 229910002353 SrRuO3 Inorganic materials 0.000 description 3
- 238000005286 illumination Methods 0.000 description 3
- 125000001967 indiganyl group Chemical group [H][In]([H])[*] 0.000 description 3
- 229910002244 LaAlO3 Inorganic materials 0.000 description 2
- 229910002370 SrTiO3 Inorganic materials 0.000 description 2
- 229910021542 Vanadium(IV) oxide Inorganic materials 0.000 description 2
- 239000005030 aluminium foil Substances 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 2
- 238000010348 incorporation Methods 0.000 description 2
- ZDNZHITXTQBUPT-UHFFFAOYSA-N nickel samarium Chemical compound [Ni].[Sm] ZDNZHITXTQBUPT-UHFFFAOYSA-N 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000005036 potential barrier Methods 0.000 description 2
- 230000009466 transformation Effects 0.000 description 2
- GRUMUEUJTSXQOI-UHFFFAOYSA-N vanadium dioxide Chemical compound O=[V]=O GRUMUEUJTSXQOI-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- WCYXDPQRKFQCSQ-UHFFFAOYSA-N [Nd].[Sm] Chemical compound [Nd].[Sm] WCYXDPQRKFQCSQ-UHFFFAOYSA-N 0.000 description 1
- PWKXVIXDLJPOMA-UHFFFAOYSA-N [Ni]=O.[Nd] Chemical compound [Ni]=O.[Nd] PWKXVIXDLJPOMA-UHFFFAOYSA-N 0.000 description 1
- XBAOPMPPZXHFEX-UHFFFAOYSA-N [Ni]=O.[Pr] Chemical compound [Ni]=O.[Pr] XBAOPMPPZXHFEX-UHFFFAOYSA-N 0.000 description 1
- KBZOVDSCFHXLPB-UHFFFAOYSA-N [O].[Ni].[Eu] Chemical compound [O].[Ni].[Eu] KBZOVDSCFHXLPB-UHFFFAOYSA-N 0.000 description 1
- MSTBZDLHMKORMU-UHFFFAOYSA-N [O].[Ni].[Nd].[Sm] Chemical compound [O].[Ni].[Nd].[Sm] MSTBZDLHMKORMU-UHFFFAOYSA-N 0.000 description 1
- FLWCYCMGKSKYDB-UHFFFAOYSA-N [Sm].[Pr] Chemical compound [Sm].[Pr] FLWCYCMGKSKYDB-UHFFFAOYSA-N 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 230000001427 coherent effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- RHSKZPGAGXXKCV-UHFFFAOYSA-N europium neodymium Chemical compound [Nd][Eu] RHSKZPGAGXXKCV-UHFFFAOYSA-N 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000005669 field effect Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000031068 symbiosis, encompassing mutualism through parasitism Effects 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/20—Multistable switching devices, e.g. memristors
- H10N70/24—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/011—Manufacture or treatment of multistable switching devices
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N70/00—Solid-state devices having no potential barriers, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
- H10N70/883—Oxides or nitrides
- H10N70/8836—Complex metal oxides, e.g. perovskites, spinels
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- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Catalysts (AREA)
Abstract
A kind of preparation and application method of the varistor based on hydrogenation rare-earth Ni-base oxide, belong to electron strong correlation material and field of electronic devices.The present invention, which is increased by adulterating proton in material with electric field strength, to be occurred gradually to migrate to trigger in material nickel element from the opposite weak electron non-local state metal of strong correlation electron localized modes insulator or semiconductor phase transition, to realize material resistance with the variation of applied voltage, i.e. realization current-voltage non-linear variation relation.Migration activation energy and soft breakdown characteristic of the proton in hydrogenation rare-earth Ni-base perovskite oxide are controlled by conditions such as the rare earth element type of control material, crystal structure, crystal particle crystal boundary state, stress states, to realize the control to material nonlinearity resistance dynamic changing process.Present invention can apply to varistor, filtering and rectifications, electric signal sensing, overvoltage protection etc..Compared with the traditional pressure sensitives non-linear resistance material such as zinc oxide, titanium oxide, device prepared by the present invention is more suitable for reducing atmosphere.
Description
Technical field
The invention belongs to electron strong correlation material and field of electronic devices, are related to a kind of based on hydrogenation rare-earth Ni-base perovskite
The preparation method of the nonlinear resistance of oxide.
Background technique
Rare-earth Ni-base perovskite oxide (ReNiO3: Re=Sm, Nd, Eu etc.) be a kind of classics metal insulator phase turn
Change (MIT) electron strong correlation state material [Nat.Commun., 2014,5,4860；Appl.Phys.Lett.,2015,107,
031905；Phys.Rev.Lett.,1999,82,3871；Phys.Rev.B,2004,69,153105；
PhaseTransitions,2008,81,729].It realizes the key changed from metallic state (or semiconductor form) to insulation posture
It is the relative adjustment by additional condition to nickel element valence state and nickel oxygen key angle.Except having and classical vanadium dioxide
(VO2) similar temperature causes outside phase-change characteristic, by protium to ReNiO3It carries out electron adulterated to trigger its electron strong correlation
Effect cause nickel element to be reduced into for electron orbit recombination be changed into high localized modes so that resistivity of material sharply increases 4-6
A order of magnitude [Nat.Commun., 2014,5,4860].At the same time, ReNiO3The proton of middle incorporation is in concentration gradient, electric field
The effects of under there is certain transportable characteristic, this has greatly widened hydrogenation ReNiO3Turn in function electronic device and hydrogen energy source
Application space in parallel operation part.Such as 2016, Y.Zhou etc. utilizes H-SmNiO3Proton conductive electronic isolation characteristic will
HSmNiO3Applied to fuel cell solid-state electrolyte, realize excellent electrochemical energy conversion performance [Nature, 2016,
Doi:10.1038/nature17653].2014, J.Shi etc. was using proton in HSmNiO3In electromigration characteristic be prepared for
Applied to Metal Oxide Semiconductor Field Effect Transistor (MOSFET).By the way that SmNiO will be hydrogenated3As MOSFET channel layer,
Using electric field controls proton in H-SmNiO3In relative migration can de-activated hydrogen cause phase transformation, realize between electric conduction source drain
Flow the adjusting [Nat.Commun., 2014,5,4860] of nearly 6 orders of magnitude.
The related rare-earth Ni-base perovskite compound (or hydrogenation rare-earth Ni-base perovskite compound) reported at present is in electronics
Application in terms of device is based primarily upon the variation that protium doping changes material static DC resistance.Such as by H-SmNiO3Make
For the channel layer (grid) of transistor, distribution of the proton in channel layer is controlled by electrode polarization, thus realize source electrode and
The adjusting variation of height configuration is shown in drain electrode.In contrast, for hydrogenation rare-earth Ni-base compound in strong dc electric field or alternating current
The practical application of nonlinear resistance reversible change due to caused by proton local migration there is no report under field action.We have found that
Migration occurs under the effect of certain activation energy and reduces and nickel oxygen octahedra for the proton mixed in hydrogenation rare-earth Ni-base compound
Bonding action, so as to cause material resistance nonlinear change.This characteristic makes the hydrogenatable non-linear electricity of rare-earth Ni-base compound
Resistance device can be applied to varistor, filtering and rectification, electric signal sensing, overvoltage protection etc..Compared to zinc oxide, oxidation
The conventional oxides non-linear resistance material such as titanium, hydrogenation rare-earth Ni-base compound nonlinear resistance are particularly suitable for reproducibility gas
Atmosphere.
Summary of the invention
The purpose of the present invention is to provide a kind of nonlinear resistance preparations based on hydrogenation rare-earth Ni-base perovskite oxide
Method is increased with electric field strength by doping proton (protium) in material and occurs gradually to migrate to trigger nickel element in material
It must change from strong correlation electron localized modes (insulator phase) to weak electron non-local state (metal or semiconductor phase), to realize material
Expect resistance with the variation (i.e. realization current-voltage non-linear variation relation) of applied voltage.By the rare earth element for controlling material
The conditions such as type, crystal structure, crystal particle crystal boundary state, stress state control proton in hydrogenation rare-earth Ni-base perovskite oxide
Migration activation energy and migration characteristic, to realize control to material nonlinearity resistance dynamic changing process.The hydrogenation is dilute
The Ni-based perovskite oxide nonlinear resistance of soil can be applied to varistor, filtering and rectification, electric signal sensing, overvoltage protection etc.
Aspect tool.Compared with the traditional pressure sensitives non-linear resistance material such as zinc oxide, titanium oxide, nonlinear resistance of the present invention is more applicable
In reducing atmosphere.
A kind of preparation method of the nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide, which comprises
Rare-earth Ni-base perovskite oxide block or thin-film material are provided, on rare-earth Ni-base perovskite oxide material surface
It prepares hydrogenating catalytic electrode material array and anneals under hydrogen atmosphere or by Electrochemical hydriding process, realize to rare-earth Ni-base
The hydrogenation treatment and proton of perovskite compound material are adulterated.
Using two different catalysis electrodes or a catalysis electrode and a hearth electrode as the input/output terminal of electric signal.
When triggering can be lower than proton activation energy, the oxygen atom in the proton and nickel oxygen octahedra mixed in rare-earth Ni-base compound is hydrogenated
In at bonded state, material is in high resistance state；When triggering can be higher than proton activation energy, hydrogenate in rare-earth Ni-base compound
Oxygen atom of the proton of incorporation from nickel oxygen octahedra is activated at bonded state, so that material be made to be in low because of soft breakdown
Resistance states realize the dynamic characteristic of non-linear resistance variation.
Further, the crystal structure of the rare-earth Ni-base perovskite oxide material is ABO3Perovskite structure
ReNiO3: Re (A) combinations for Rare Earth Elements Determination or a variety of rare earth elements, preferably samarium (Re=Sm), neodymium (Re=Nd),
Europium (Re=Eu), praseodymium (Re=Pr), samarium neodymium (Re=SmxNd1-x, 0 < x < 1), samarium praseodymium (Re=SmxPr1-x, 0 < x < 1), europium neodymium (Re
=EuxNd1-x, 0 < x < 1)；Europium spreads (Re=EuxPr1-x, 0 < x < 1)；Nickel element (Ni) occupies the position the B in perovskite structure.
Further, the rare-earth Ni-base perovskite oxide material is thin-film material, and thickness is micro- to 100 between 1 nanometer
Between rice, the quasi- monocrystalline thin-film material or polycrystalline material of the epitaxial growth in single crystalline substrate can be.
Further, the hydrogenation process is included under the catalyst such as platinum, palladium and is heat-treated in hydrogen, or passes through electrochemistry
Reaction is to ReNiO3Carry out proton doping.
Further, the trigger action and trigger energy include: the direct current formed by direct current or alternating voltage or friendship
Power transformation field action, pulse or the effect of continuous photon etc..
Further, the activation can be subject to reality by applying the processes such as external voltage, light triggering, ultrasound triggering
It is existing.
Further, thick by changing material component, crystal structure and crystal orientation, the film of rare-earth Ni-base thin-film material
Stress state, hydrogenation electrode arrangements, device architecture etc. adjust proton activation energy and soft breakdown critical voltage between degree, substrate and film
Value, so that the nonlinear change characteristic to material resistance is adjusted control.
Further, nonlinear resistance prepared by the present invention can be applied to varistor, filtering and rectification, electric signal passes
Sense, overvoltage protection etc., and it is suitable for reducing atmosphere.
The present invention after extensive and in-depth study, by improving preparation process, obtains a kind of based on hydrogenation rare earth nickel
The nonlinear resistance preparation method of based perovskite oxide.Technical concept of the invention is: utilizing hydrogenation rare-earth Ni-base chemical combination
Migration occurs for the proton mixed in object and reduces to cause material with the bonding action of nickel oxygen octahedra under the effect of certain activation energy
Soft breakdown, make instantaneous reduction of the resistance under corresponding trigger condition, realize non-linear resistance variation.Prepared device can be applied
In varistor, filtering and rectification, electric signal sensing, overvoltage protection etc..Compared to conventional oxidations such as zinc oxide, titanium oxide
Object non-linear resistance material, hydrogenation rare-earth Ni-base compound nonlinear resistance are particularly suitable for reducing atmosphere.
Detailed description of the invention
Fig. 1 is that the two-way hydrogenation rare-earth Ni-base oxide perovskite oxide based on strip platinum catalysis electrode is non-linear
Resistance schematic diagram.
Fig. 2 is that the two-way hydrogenation rare-earth Ni-base oxide perovskite oxide based on strip platinum catalysis electrode is non-linear
The I-V characteristic figure of resistance.As can be seen that output electric current sharply increases, resistance when applied positive and negative bi-directional voltage is more than 5V
Device resistance value reduces.
Fig. 3 is that the unidirectional hydrogenation rare-earth Ni-base oxide perovskite oxide based on cylindric platinum catalysis electrode is non-thread
Property resistance schematic diagram.
Fig. 4 is that the unidirectional hydrogenation rare-earth Ni-base oxide perovskite oxide based on cylindric platinum catalysis electrode is non-thread
The I-V characteristic figure of property resistance.As can be seen that output electric current sharply increases, resistance device when applied negative voltage is more than 5V
Resistance value reduces.
Fig. 5 is unidirectional hydrogenation rare-earth Ni-base oxide perovskite oxide nonlinear resistance in dark and visible illumination condition
Under I-V characteristic figure.As can be seen that output electric current sharply increases, and resistance device resistance value subtracts under radiation of visible light triggering
It is small.
Specific embodiment
Unless specific instructions, various raw materials of the invention can be by being commercially available；Or the routine side according to this field
Method is prepared.Unless otherwise defined or described herein, all professional and scientific terms and art technology used herein are ripe
It is identical to practice meaning known to personnel.Furthermore any method similar to or equal to what is recorded and material all can be applied to this
In inventive method.
Other aspects of the present invention are apparent to those skilled in the art due to this disclosure
's.
Present invention will be further explained below with reference to specific examples.It should be understood that these embodiments are merely to illustrate the present invention
Rather than it limits the scope of the invention.In the following examples, the experimental methods for specific conditions are not specified, usually according to conventional strip
Part, or carry out according to the normal condition proposed by manufacturer.
Embodiment 1:
Pt/H-SmNiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 200 nanometers of samarium nickel oxygen (SmNiO3) polycrystal film.Strip metal platinum is prepared in film surface
Catalysis electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 milli of spacing
Rice.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2It is moved back in/He mixed gas in 300 degrees Celsius
Fire 30 minutes carries out hydrogenation treatment.In actual use, using two adjacent platinum catalytic electrodes as signal input output end,
Between application voltage two electrodes of measurement and measure electric current.Fig. 1 illustrates device architecture.Fig. 2 illustrates measurement I-V relation curve,
It can be seen that when applied positive and negative bi-directional voltage is more than 5V, H-SmNiO3In proton be activated cause hydrogen cause insulator phase
Change degree becomes smaller, and output electric current sharply increases, and resistance device resistance value reduces.It is made in the application of practical overvoltage crowbar
Standby Pt/H-SmNiO3Device is used in parallel with protected device, when additional AC or DC voltage is excessive, Pt/H-SmNiO3Device
Part resistance reduces, to realize the purpose of divided current.
Embodiment 2:
Pt/H-SmNiO3/SrRuO3/ Si electricity triggers the preparation and application method of unidirectional nonlinear resistance, specific as follows:
10 millimeters of side length of square silicon lining grows 100 nanometers of strontium rubidium oxygen film hearth electrodes, and 200 nanometers of samarium nickel are grown on hearth electrode
Oxygen (SmNiO3) polycrystal film.Cylindrical metal platinum catalytic electrode is prepared in film surface, electrode size: 50 microns of diameter, thick
100 nanometers；Platinum electrode in permutation presses square two lattice arrangements, and 150 microns of platinum electrode spacing.Platinum catalysis electricity will be deposited with
The samarium nickel oxygen film of pole array is placed in 1%H2It anneals 30 minutes in/He mixed gas in 300 degrees Celsius, carries out hydrogenation treatment.?
In actual use, platinum catalytic electrode applies voltage simultaneously to measurement end as signal input output end using hearth electrode and one by one
Measure electric current.Fig. 1 illustrates device architecture.Fig. 2 illustrates measurement I-V relation curve, it can be seen that bears two-way electricity when applying
When pressure is more than 5V, H-SmNiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electric current sharply increase,
Resistance device resistance value reduces.In the application of practical overvoltage crowbar, prepared Pt/H-SmNiO3/SrRuO3Device with protected
It is used in parallel to protect device, when applied voltage is excessive, Pt/H-SmNiO3Device resistance reduces, to realize the mesh of divided current
's.It is different from embodiment 1, it is easier since proton is migrated to platinum electrode compared to hearth electrode in embodiment 2, thus device has list
To soft breakdown I-V characteristic, in addition to for overvoltage protection, and can connect in electronic device to realize the purpose of rectification.
Embodiment 3:
Pt/H-SmNiO3/SrTiO3Electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length
10 millimeters of square strontium titanates (SrTiO3) 200 nanometers of samarium nickel oxygen (SmNiO of lining growth3) polycrystal film, it is grown by control
Condition makes thin-film material extension coherent growth, i.e., subject to film monocrystal material and be in tensile stress state.In film surface system
Standby strip metal platinum catalytic electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item is parallel to each other in array
Arrangement, 1 millimeter of spacing.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2In/He mixed gas in
300 degrees Celsius are annealed 30 minutes, and hydrogenation treatment is carried out.In actual use, using two adjacent platinum catalytic electrodes as signal
Input/output terminal between application voltage two electrodes of measurement and measures electric current.When applied positive and negative bi-directional voltage is more than 70V, H-
SmNiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electric current sharply increase, resistance device resistance
Value reduces.Compared to the samarium nickel oxygen polycrystalline material in embodiment 1, prepared thin film grain-boundary ratio is substantially reduced in embodiment 3,
The potential barrier overcome needed for proton activation migration greatly improves, therefore device soft breakdown voltage increases.
Embodiment 4:
Pt/H-SmNiO3/LaAlO3Electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length
10 millimeters of square lanthanum alumina (LaAlO3) 200 nanometers of samarium nickel oxygen (SmNiO of lining growth3) polycrystal film, it is grown by control
Condition makes thin-film material identical as substrate high preferred orientation, but symbiosis and epibiosis by edge dislocation relaxation, i.e. film is quasi- monocrystalline material
Material and interfacial stress relaxation.Strip metal platinum catalytic electrode is prepared in film surface, electrode size: 10 millimeters long, wide 0.5 milli
Rice is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 millimeter of spacing.The samarium nickel oxygen of platinum catalytic electrode array will be deposited with
Thin-film material is placed in 1%H2It anneals 30 minutes in/He mixed gas in 300 degrees Celsius, carries out hydrogenation treatment.It is actually using
In, using two adjacent platinum catalytic electrodes as signal input output end, between application voltage two electrodes of measurement and measure electric current.
When applied positive and negative bi-directional voltage is more than 45V, H-SmNiO3In proton be activated cause hydrogen cause insulator phase transition degree become
Small, output electric current sharply increases, and resistance device resistance value reduces.The crystal defect of prepared film is compared to real in embodiment 4
It applies example 3 to increase, therefore the potential barrier overcome needed for proton activation migration decreases, therefore device soft breakdown voltage is relatively real
Example 3 is applied to decrease.
Embodiment 5:
Pt/H-NdNiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 50 nanometers of neodymium nickel oxygen (NdNiO3) polycrystal film.Strip metal platinum is prepared in film surface to urge
Polarizing electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 milli of spacing
Rice.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2It is moved back in/He mixed gas in 300 degrees Celsius
Fire 30 minutes carries out hydrogenation treatment.In actual use, using two adjacent platinum catalytic electrodes as signal input output end,
Between application voltage two electrodes of measurement and measure electric current.When applied positive and negative bi-directional voltage is more than 0.5V, H-NdNiO3In
Proton, which is activated, causes hydrogen that insulator phase transition degree is caused to become smaller, and output electric current sharply increases, and resistance device resistance value reduces.With reality
It applies example 1 to compare, embodiment 5 reduces the soft breakdown voltage of device by changing rare earth element in rare-earth Ni-base compound.
Embodiment 6:
Pt/H-EuNiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 1 micron of europium nickel oxygen (EuNiO3) polycrystal film.Strip metal platinum is prepared in film surface to urge
Polarizing electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 milli of spacing
Rice.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2It is moved back in/He mixed gas in 300 degrees Celsius
Fire 30 minutes carries out hydrogenation treatment.In actual use, using two adjacent platinum catalytic electrodes as signal input output end,
Between application voltage two electrodes of measurement and measure electric current.When applied positive and negative bi-directional voltage is more than 7V, H-EuNiO3In matter
Son, which is activated, causes hydrogen that insulator phase transition degree is caused to become smaller, and output electric current sharply increases, and resistance device resistance value reduces.With implementation
Example 1 is compared, and embodiment 6 improves the soft breakdown voltage of device by changing rare earth element in rare-earth Ni-base compound.
Embodiment 7:
Pt/H-PrNiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 5 nanometers of praseodymium nickel oxygen (PrNiO3) polycrystal film.Strip metal platinum is prepared in film surface to urge
Polarizing electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 milli of spacing
Rice.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2It is moved back in/He mixed gas in 300 degrees Celsius
Fire 30 minutes carries out hydrogenation treatment.In actual use, using two adjacent platinum catalytic electrodes as signal input output end,
Between application voltage two electrodes of measurement and measure electric current.When applied positive and negative bi-directional voltage is more than 0.7V, H-NdNiO3In
Proton, which is activated, causes hydrogen that insulator phase transition degree is caused to become smaller, and output electric current sharply increases, and resistance device resistance value reduces.With reality
It applies example 1 to compare, embodiment 7 reduces the soft breakdown voltage of device by changing rare earth element in rare-earth Ni-base compound.
Embodiment 8:
Pt/H-Sm0.5Eu0.5NiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows:
10 millimeters of side length of square silicon lining grows 1 micron of samarium europium nickel oxygen (Sm0.5Eu0.5NiO3) polycrystal film.In film surface system
Standby strip metal platinum catalytic electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item is parallel to each other in array
Arrangement, 1 millimeter of spacing.The samarium nickel oxygen thin-film material for being deposited with platinum catalytic electrode array is placed in 1%H2In/He mixed gas in
300 degrees Celsius are annealed 30 minutes, and hydrogenation treatment is carried out.In actual use, using two adjacent platinum catalytic electrodes as signal
Input/output terminal between application voltage two electrodes of measurement and measures electric current.When applied positive and negative bi-directional voltage is more than 6V, H-
Sm0.5Eu0.5NiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electric current sharply increase, resistor
Part resistance value reduces.Compared with Example 1, embodiment 8 improves device by changing rare earth element in rare-earth Ni-base compound
Soft breakdown voltage.
Embodiment 9:
Pd/H-Sm0.5Nd0.5NiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows:
10 millimeters of side length of square silicon lining grows 1 micron of samarium neodymium nickel oxygen (Sm0.5Nd0.5NiO3) polycrystal film.In film surface system
Standby strip metal palladium chtalyst electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Palladium item is parallel to each other in array
Arrangement, 1 millimeter of spacing.The samarium nickel oxygen thin-film material for being deposited with palladium chtalyst electrod-array is placed in 1%H2In/He mixed gas in
300 degrees Celsius are annealed 30 minutes, and hydrogenation treatment is carried out.In actual use, using two adjacent platinum catalytic electrodes as signal
Input/output terminal between application voltage two electrodes of measurement and measures electric current.When applied positive and negative bi-directional voltage is more than 2V, H-
Sm0.5Nd0.5NiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electric current sharply increase, resistor
Part resistance value reduces.Compared with Example 1, embodiment 9 improves device by changing rare earth element in rare-earth Ni-base compound
Soft breakdown voltage.
Embodiment 10:
Pt/H-SmNiO3/ Si electricity triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 200 nanometers of samarium nickel oxygen (SmNiO3) polycrystal film.Strip metal platinum is prepared in film surface
Catalysis electrode, electrode size: it is 10 millimeters long, it is 0.5 millimeter wide, it is 100 nanometers thick；Platinum item arrangement parallel to each other in array, 1 milli of spacing
Rice.The samarium nickel oxygen thin-film material aluminium foil for being deposited with platinum catalytic electrode array is wrapped up as quiet in the dilute hydrochloric acid of 0.01mol/L
It sets 30 seconds, completes hydrogenation.In hydrogenation process, the two poles of the earth of samarium nickel oxygen and aluminium foil respectively as primary battery: aluminium betatopic is oxidized,
Proton is spread into samarium nickel oxygen realizes protium doping.In actual use, using two adjacent platinum catalytic electrodes as signal
Input/output terminal between application voltage two electrodes of measurement and measures electric current.Fig. 1 illustrates device architecture.When applied positive and negative double
When being more than 5V to voltage, H-SmNiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electric current sharply
Increase, resistance device resistance value reduces.
Embodiment 11:
Pt/H-SmNiO3/ Si light triggers the preparation and application method of two-way nonlinear resistance, specific as follows: in side length 10
The square silicon lining of millimeter grows 100 nanometers of strontium rubidium oxygen film hearth electrodes, and 100 nanometers of samarium nickel oxygen are grown on hearth electrode
(SmNiO3) polycrystal film.Cylindrical metal platinum catalytic electrode is prepared in film surface, electrode size: 50 microns of diameter, thickness 100
Nanometer；Platinum electrode in permutation presses square two lattice arrangements, and 150 microns of platinum electrode spacing.Platinum catalytic electrode will be deposited with
The samarium nickel oxygen film of array is placed in 1%H2It anneals 30 minutes in/He mixed gas in 300 degrees Celsius, carries out hydrogenation treatment.In reality
Border is in use, platinum catalytic electrode is as signal input output end using hearth electrode and one by one, respectively in dark and visible light illumination
Under the conditions of apply voltage between (100W incandescent light source) measurement end and measure electric current.Fig. 5 illustrates measurement I-V relation curve, can
To find out under visible light illumination, H-SmNiO3In proton be activated cause hydrogen cause insulator phase transition degree become smaller, output electricity
Stream sharply increases, and resistance device resistance value reduces.Embodiment 11 shows in addition to using applied voltage, can also use light source and draws
Play the nonlinear change of prepared hydrogenation rare-earth Ni-base perovskite compound resistance device.
Embodiment 12:
Pt/H-SmNiO3/SrRuO3/ Si light triggers the preparation and application method of unidirectional nonlinear resistance, specific as follows:
10 millimeters of side length of square silicon lining grows 100 nanometers of strontium rubidium oxygen film hearth electrodes, and 100 nanometers of samarium nickel are grown on hearth electrode
Oxygen (SmNiO3) polycrystal film.Cylindrical metal platinum catalytic electrode is prepared in film surface, electrode size: 50 microns of diameter, thick
100 nanometers；Platinum electrode in permutation presses square two lattice arrangements, and 150 microns of platinum electrode spacing.Platinum catalysis electricity will be deposited with
The samarium nickel oxygen film of pole array is placed in 1%H2It anneals 30 minutes in/He mixed gas in 300 degrees Celsius, carries out hydrogenation treatment.?
In actual use, using hearth electrode and a platinum catalytic electrode as signal input output end, received respectively in dark and wavelength for 248
Apply voltage between measurement end under rice ultraviolet laser triggers and measures electric current.Under laser triggering, H-SmNiO3In proton lived
Change causes hydrogen that insulator phase transition degree is caused to become smaller, and output electric current sharply increases, and resistance device resistance value reduces.
The foregoing is merely illustrative of the preferred embodiments of the present invention, the substantial technological content model being not intended to limit the invention
It encloses, substantial technological content of the invention is broadly defined in the scope of the claims of application, any technology that other people complete
Entity or method also or a kind of equivalent change, will if identical with defined in the scope of the claims of application
It is considered as being covered by among the scope of the claims.
Claims (5)
1. a kind of nonlinear resistance preparation method based on hydrogenation rare-earth Ni-base perovskite oxide, which is characterized in that provide dilute
The Ni-based perovskite oxide block of soil or thin-film material prepare hydrogenating catalytic electricity on rare-earth Ni-base perovskite oxide material surface
Pole material array is simultaneously annealed under hydrogen atmosphere or by Electrochemical hydriding process, is realized to rare-earth Ni-base perovskite compound material
The hydrogenation treatment and proton of material are adulterated；
Using two different catalysis electrodes or a catalysis electrode and a hearth electrode as the input/output terminal of electric signal；Work as touching
When hair can be lower than proton activation energy, hydrogenates the proton mixed in rare-earth Ni-base compound and be in the oxygen atom in nickel oxygen octahedra
At bonded state, material is in high resistance state；When triggering can be higher than proton activation energy, hydrogenates and mixed in rare-earth Ni-base compound
Oxygen atom of the proton from nickel oxygen octahedra be activated at bonded state, so that material be made to be in low resistance because of soft breakdown
State realizes the dynamic characteristic of non-linear resistance variation；By the material component, the crystal structure that change rare-earth Ni-base thin-film material
Stress state, hydrogenation electrode arrangements, device architecture adjust proton activation energy between crystal orientation, film thickness, substrate and film
With soft breakdown critical voltage value, so that the nonlinear change characteristic to material resistance is adjusted control；
The crystal structure of the rare-earth Ni-base perovskite oxide material is ABO3Perovskite structure ReNiO3: A i.e. Re be
The combination of Rare Earth Elements Determination or a variety of rare earth elements selects Re=Sm, Re=Nd, Re=Eu, Re=Pr, Re=SmxNd1-x,
0 < x < 1, Re=SmxPr1-x, 0 < x < 1, Re=EuxNd1-x, 0 < x < 1, Re=EuxPr1-x, 0 < x < 1；Nickel element occupies perovskite knot
The position B in structure；
The rare-earth Ni-base perovskite oxide material is thin-film material, and between 1 nanometer to 100 microns, selection exists thickness
The quasi- monocrystalline thin-film material or polycrystalline material of epitaxial growth in single crystalline substrate.
2. a kind of preparation side of nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide as described in claim 1
Method, which is characterized in that the hydrogenation process is included under platinum, palladium catalyst to be heat-treated in hydrogen, or passes through electrochemical reaction
To ReNiO3Carry out proton doping；Electrochemical action selects galvanic interaction.
3. a kind of preparation side of nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide as described in claim 1
Method, which is characterized in that the trigger action and trigger energy includes: the direct current or alternation electricity formed by direct current or alternating voltage
Field action, pulse or the effect of continuous photon.
4. a kind of preparation side of nonlinear resistance based on hydrogenation rare-earth Ni-base perovskite oxide as described in claim 1
Method, which is characterized in that the activation is by applying outer direct current or exchange external voltage, pulse or the triggering of continuous light, ultrasound touching
Hair process is realized.
5. the application method of the nonlinear resistance of the method as described in claim 1 preparation, which is characterized in that prepared non-linear
In terms of resistance is for varistor, filtering and rectification, electric signal sensing, overvoltage protection, and it is suitable for reducing atmosphere.
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