CN110718629A - Preparation method of transient keratin resistive random access memory - Google Patents
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- 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/011—Manufacture or treatment of multistable switching devices
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- 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 without a potential-jump barrier or surface barrier, 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
- H10N70/245—Multistable switching devices, e.g. memristors based on migration or redistribution of ionic species, e.g. anions, vacancies the species being metal cations, e.g. programmable metallization cells
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- 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 without a potential-jump barrier or surface barrier, and specially adapted for rectifying, amplifying, oscillating or switching
- H10N70/801—Constructional details of multistable switching devices
- H10N70/881—Switching materials
Abstract
The invention discloses a preparation method of a transient keratin resistive random access memory, which is characterized in that soluble keratin powder is dissolved at normal temperature, and low-temperature annealing is carried out for 20-50min after the soluble keratin powder is prepared into a film by spin coating. Then covering with a mask plate, and evaporating and depositing a layer of Ag electrode with the thickness of about 90-120nm on the mask plate. And (3) preparing the transient resistive random access memory device based on human hair keratin. The invention also specifically discloses preparation steps, tests the performance of the keratin material and the electrical performance of the resistive random access device, and proves that the memory device has repeatable and reliable non-volatile memory behavior and multi-level memory effect. The potential resistance switching mechanism is due to the formation and breakage of Ag conductive filaments. The transient characteristic of the device is that the dielectric layer keratin film can be completely dissolved in deionized water within 30 min. The biological transient resistance change device can supplement the limitation of the traditional resistance change device, becomes a novel green and safe resistance change memory device, and is expected to be applied to the aspect of biomedicine.
Description
Technical Field
The invention belongs to the technical field of resistive random access memory devices, and particularly relates to a preparation method of a transient keratin resistive random access memory.
Background
The exploration of the progress of electron transport in biomaterials is a key process for biological energy conversion, which can be realized in solid state devices. The demand for future green data storage and novel electronic technologies has led to the development of natural biomolecule based memory storage devices. Furthermore, the biocompatibility and biodegradability of such biomolecule-based memory devices broaden their application in implantable devices, biomedicine and biosensing, and some biomolecules including proteins, sugars, DNA, RNA and viruses have been shown to have robust resistive switching characteristics, allowing for the substitution of safe and "green" features into next generation memory devices.
Biomaterials extracted from living organisms and used in microelectronic devices have attracted increasing attention to build biocompatible electronic devices. Currently, several organic biomaterials have been studied in the development of bioelectronic devices. Among them, keratin materials exhibit their biodegradability, natural abundance and intrinsic biocompatibility, which have become great hopes for the world of innovative biomaterials. On the other hand, the increasing demand for green information storage in the future has led to the rapid development of natural biomaterial-based storage devices. Among several types of emerging memory technologies, resistive switching memory devices that can switch resistance states between high and low resistance states by applying an electric field have received extensive research interest due to their simple structure
With the concern and importance of society on human health and environmental problems. Biomaterials that are non-toxic, biocompatible, renewable, lightweight, degradable, and capable of being printed on flexible substrates are being considered for a new generation of green resistive memory devices. For example, the biomaterial is applied to the resistive device as chitosan, egg albumen, sericin, fibroin, and the like based on crab shells, which have been explored as described above. In addition, the electronic product based on the degradable and transient characteristic material can be implanted into the body, and the device can disappear in the body after medical diagnosis, so that continuous operations can be further reduced, and the transient electronic equipment is very suitable for the application of the implanted equipment. The method for extracting keratin on the premise mainly comprises a high-temperature high-pressure hydrolysis method, an expansion method, a chemical treatment method, a biotechnology method and the like. At present, research based on a biological material resistive random access memory device is just started, so that technical problems exist in material selection, device preparation and integration.
Disclosure of Invention
Keratin is widely present in wool, hair, feathers, nails and reptile skin, and has excellent biomacromolecule mechanical properties. Keratin is a functional material, and is widely applied to the aspects of biology, medicine, materials and the like in recent years. Keratin from human hair has distinct advantages over other animal sources, namely a realistic source of autologous proteins with a rich supply and for biocompatible electronics. In addition, the soluble human hair keratin can be easily obtained by a mixture of reducing agents under acidic or alkaline conditions. The invention aims to explore feasibility of converting human hair waste into functional protein biological materials and research a preparation method of a keratin-based resistive random access memory device. The method is mainly realized by simple spin coating and evaporation deposition, and the invention provides the following technical scheme: a preparation method of a transient keratin resistive random access memory comprises the following preparation steps:
1) dissolving keratin, and filtering to obtain keratin solution;
2) the prepared keratin solution is baked to form a keratin film through spin coating;
3) carrying out ultrasonic treatment on the FTO/glass transparent conductive substrate, drying by nitrogen and cleaning by ozone;
4) and depositing an Ag electrode on the keratin film by vacuum evaporation to form an Ag/keratin/FTO memory device.
The performance of the keratin film is characterized by Fourier infrared spectroscopy and surface SEM, and the result shows that the film has excellent uniform compactness. And the device has good electrical characteristics, the device has more than 103A reasonable resistance window of OFF/ON ratio of over 104s retention time. More importantly, the keratin film can be dissolved in deionized water within 30min, and the dissolution of the device is accompanied by the disappearance of the electrical properties, showing physical transient characteristics, i.e. the device can be partially or totally physically and/or functionally disappeared when triggered by water.
Preferably, the keratin solution in the step 1) has a mass concentration of 50-70mg/ml, and is prepared by ultrasonically dispersing keratin powder in deionized water at 20-35 ℃ for 10-30min, and filtering with a PTFE filter with a pore size of 0.3-0.5 μm;
preferably, the preparation conditions of 2) are spin-coated on the FTO-coated glass substrate at a spin speed of 2000 rpm for 10 to 30 seconds, respectively, and then baked on a hot plate at 40 to 70 ℃ for 20 to 50min to remove the solvent.
Preferably, the 3) ultrasonic cleaning mode is ultrasonic cleaning for 15-45min in the sequence of detergent water, deionized water, absolute alcohol and isopropanol; the ozone cleaning time is 10-30 min.
Preferably, the 4) Ag electrode deposition thickness is 90-120 nm.
The transient keratin resistive memory device is prepared through a simple spin coating and evaporation deposition method, and the device can show the characteristics of a transient device.
The keratin film characterization adopts surface SEM characterization and Fourier infrared spectrum characterization, and the electrical performance of the transient resistance change device adopts a Keithley-4200 semiconductor analysis and test system for characterization. The device has typical bipolar characteristics and has good repeatability and durability.
Preferably, the keratin comprises the following preparation steps:
(1) washing human hair with sodium dodecyl sulfate solution;
(2) taking thioglycollic acid as hair for deoxidation treatment, so as to destroy cystine bonds and form a reduction solution;
(3) retaining the reducing solution by filtration, extracting the crude fraction of keratin with an alkaline solution, a second extraction with deionized water;
(4) combining the extracts;
(5) the solution was pH adjusted and concentrated on the dialysis system, then lyophilized and stored.
The protein powder prepared by this method can be dissolved in water to form a keratin solution, and the solution has slight viscosity in light yellow color. The soluble keratin has rapid dissolution property, can promote mitosis of epidermal cells, can be used for preparing biological materials or medicines for promoting proliferation or migration of cells, and plays a role in hemostasis and wound healing.
Preferably, the concentration of the (1) sodium dodecyl sulfate is 0.2-0.7% (w/v), and the preparation temperature is 20-35 ℃; the dosage of the thioglycolic acid (2) is 0.2-0.6M, and the pH value is 7.5-8.5, and the treatment lasts for 12-20 h; the alkali solution (3) is 90-110mMtris, and the extraction time is 1-4 h; the merging and extracting conditions of (4) are as follows: centrifuging at 4000-7000rpm at 2-6 deg.C for 30-60min, and dialyzing with ultrafiltration membrane; the pH value of the solution (5) is 7-8, and the concentration multiple on a dialysis system is 20-30 times
The beneficial effects of the invention are as follows:
(1) the keratin has the potential to be used as a resistive memory device, the keratin is synthesized by a reduction method, and the resistive memory device based on the keratin film is obtained by simple spin coating and evaporation deposition, wherein the switching mechanism is the formation and the fracture of Ag conductive filaments caused by redox reaction.
(2) For non-volatile memory applications, the device achieves a resistance window greater than 103Sum of OFF/ON ratio of more than 104s retention time.
(3) The physical transient properties of the keratin-based resistive switching memory devices were demonstrated using soluble keratin films in DI water within 30 min.
(4) The potential of the low-cost and biodegradable keratin resistive random access memory in transient electronic and green safe storage application is shown.
Drawings
In order to make the object, technical scheme and beneficial effect of the invention more clear, the invention provides the following drawings for explanation:
fig. 1 is a method for manufacturing a keratin resistive memory device.
Fig. 2 is a microscopic topography of a keratin film.
FIG. 3 is a Fourier transform infrared spectrum of a keratin film.
Fig. 4 is a cross-sectional structure of a keratin resistance change device.
FIG. 5(a) is an I-V characteristic curve of an Ag/keratin/FTO memory device in semilogarithmic coordinates; (b) corresponding resistance-voltage (R-V) curves are shown.
Fig. 6 (a) durability of keratin-based storage device 80+ voltage consecutive scans; (b) endurance of 100 switching cycles of the keratin-based memory device reset process.
Fig. 7 is a retention characteristic of a keratin-based storage device.
Fig. 8 is a physical transient characteristic of the resistive memory device.
FIG. 9 shows an I-V characteristic curve testing apparatus and an I-V characteristic curve diagram.
Detailed Description
The technical solutions in the embodiments of the present invention are clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the scope of the present invention.
The keratin is extracted as follows:
(1) washing human hair with sodium dodecyl sulfate solution;
(2) taking thioglycollic acid as hair for deoxidation treatment, so as to destroy cystine bonds and form a reduction solution;
(3) retaining the reducing solution by filtration, extracting the crude fraction of keratin with an alkaline solution, a second extraction with deionized water;
(4) combining the extracts;
(5) the solution was pH adjusted and concentrated on the dialysis system, then lyophilized and stored.
The transient keratin resistive random access memory device is prepared by the following method:
1) as shown in fig. 1, human hair is reduced to produce water-soluble keratin powder;
2) dissolving 60mg of keratin in 1ml of deionized water, performing ultrasonic treatment until the keratin is completely dissolved, spin-coating the solution on the upper layer of a cleaned FTO film, and performing low-temperature annealing at 60 ℃;
3) taking the keratin film prepared in the step 2), carrying out evaporation deposition of an Ag electrode on the upper surface of the keratin film, and finally preparing the keratin film-based resistive random access memory device.
The keratin film prepared at normal temperature is subjected to shape characterization as shown in figure 2, and from the micro shape of the keratin film, the compact and uniform keratin film is uniformly distributed on the FTO layer, which shows that the film has good uniform compactness. The keratin film was characterized by fourier infrared spectroscopy (FTIR) to obtain a spectrum for each functional group separately.
As shown in FIG. 3, the map shows characteristic absorption bands of peptide bonds (-CONH-). The bands produced by the oscillation of the peptide bond are called amides a, I, II, III. Occurs at 3400-3300cm-1The region is called the amide A band, which is generated by the stretching vibration of N-H. The amide I band falls at 1690-1600cm-1The range of (1) is caused by C ═ O stretching vibration. 1660cm-1The strong absorption band at (a) is connected to the alpha-helix. The amide II band falling at 1575-1480cm-1 is due to C-N stretching and N-H bending vibration. The amide III band occurs at 1300-1230cm-1Insofar, this is due to stretching of CN and CO, bending vibration of NH and O ═ CN. The device was cut to more clearly view the profile of the cross section of the device.
As shown in fig. 4, the corresponding sandwich structure is clearly seen, red from bottom to top is a glass layer, yellow is an FTO electrode layer, about 500nm thick, green is a keratin layer, about 180nm thick, the top dark green is an Ag electrode layer, about 100nm thick.
And performing electrical property characterization on the prepared resistive random access device, and connecting a tungsten probe of the top Ag electrode to the bottom FTO electrode to provide voltage scanning when the FTO electrode is grounded.
FIG. 5(a) shows the I-V characteristics of an Ag/keratin/FTO memory device on a semi-logarithmic scale. It shows that the Ag/keratin/FTO memory device shows typical bipolar resistance switching characteristics through a loop of 0V → -3V → 0V → 3V → 0V dc voltage sweep. A corresponding resistance-voltage (R-V) curve is shown in fig. 5 (b). It has clockwise lagging R-V switching function from low resistance state to high resistance state. The result shows that the OFF/ON ratio of the device is greater than 103Can easily distinguish between high and low resistance states.
The devices were subjected to endurance and retention characteristics tests as shown in fig. 6 and 7. Fig. 6 (a) shows endurance of the memory device under 80+ voltage continuous scans, and in order to evaluate the potential of the keratin-based memory device, endurance characteristics of 100 switching cycles of the set-reset process are read using a read voltage of 0.2V as shown in (b), which means robust reliability of memory device performance, i.e., the device has the capability of repeated read and write, which is a standard for measuring the performance of the resistive switching memory device. FIG. 7 shows a retention characteristic performance test of a keratin-based memory device, in which the resistance change characteristics of the device can be continuously cycled for 100 or more times and has a characteristic of about 104Retention characteristics over s time.
To investigate the physical transient properties of the devices, the prepared keratin films were immersed in deionized water. As shown in fig. 8, the keratin film is newly melted into deionized water with the lapse of time by the immersion in water. Meanwhile, the transient resistance change device characteristic is shown along with the disappearance of the electrical performance of the device.
Finally, it is noted that the above-mentioned preferred embodiments illustrate rather than limit the invention, and that, although the invention has been described in detail with reference to the above-mentioned preferred embodiments, it will be understood by those skilled in the art that various changes in form and detail may be made therein without departing from the scope of the invention as defined by the appended claims.
Claims (7)
1. A preparation method of a transient keratin resistive random access memory comprises the following preparation steps:
1) dissolving keratin, and filtering to obtain keratin solution;
2) the prepared keratin solution is baked to form a keratin film through spin coating;
3) carrying out ultrasonic treatment on the FTO/glass transparent conductive substrate, drying by nitrogen and cleaning by ozone;
4) and depositing an Ag electrode on the keratin film by vacuum evaporation to form an Ag/keratin/FTO memory device.
2. The method for preparing the transient keratin resistive random access memory according to claim 1, wherein the method comprises the following steps: the keratin solution in the step 1) has the mass concentration of 50-70mg/ml, and is prepared by ultrasonically dispersing keratin powder in deionized water for 10-30min at the temperature of 20-35 ℃ and filtering the solution by a PTFE filter with the pore diameter of 0.3-0.5 mu m.
3. The method for preparing the transient keratin resistive random access memory according to claim 1, wherein the method comprises the following steps: the 2) preparation conditions were spin-coating on the FTO-coated glass substrates at a spin speed of 2000 rpm for 10-30s, respectively, and then baking on a hot plate at 40-70 ℃ for 20-50min to remove the solvent.
4. The method for preparing the transient keratin resistive random access memory according to claim 1, wherein the method comprises the following steps: the 3) ultrasonic cleaning mode is ultrasonic cleaning for 15-45min in the sequence of liquid detergent, deionized water, absolute alcohol and isopropanol; the ozone cleaning time is 10-30 min.
5. The method for preparing the transient keratin resistive random access memory according to claim 1, wherein the method comprises the following steps: the deposition thickness of the 4) Ag electrode is 90-120 nm.
6. The method for preparing the transient keratin resistive random access memory according to claim 1, wherein the method comprises the following steps: the keratin comprises the following preparation steps:
(1) washing human hair with sodium dodecyl sulfate solution;
(2) taking thioglycollic acid as hair for deoxidation treatment, so as to destroy cystine bonds and form a reduction solution;
(3) retaining the reducing solution by filtration, extracting the crude fraction of keratin with an alkaline solution, a second extraction with deionized water;
(4) combining the extracts;
(5) the solution was pH adjusted and concentrated on the dialysis system, then lyophilized and stored.
7. The method of claim 1, wherein: the concentration of the sodium dodecyl sulfate (1) is 0.2-0.7% (w/v), and the preparation temperature is 20-35 ℃; the dosage of the thioglycolic acid (2) is 0.2-0.6M, and the pH is 7.5-8.5 for treatment for 12-20 h; the alkali solution in the step (3) is 90-110mM tris, and the extraction time is 1-4 h; the merging and extracting conditions of (4) are as follows: centrifuging at 4000-7000rpm at 2-6 deg.C for 30-60min, and dialyzing with ultrafiltration membrane; the pH value of the solution (5) is 7-8, and the concentration multiple on a dialysis system is 20-30 times.
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Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0454600A1 (en) * | 1990-04-25 | 1991-10-30 | Aesculap-Icp Sa | Product based on modified keratin, its preparation and use, especially in human or veterinary medicine |
KR101157105B1 (en) * | 2011-02-14 | 2012-06-22 | 동국대학교 산학협력단 | Nonvolatile memory device using the resistive switching of graphene oxide and the fabrication method thereof |
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Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0454600A1 (en) * | 1990-04-25 | 1991-10-30 | Aesculap-Icp Sa | Product based on modified keratin, its preparation and use, especially in human or veterinary medicine |
KR101157105B1 (en) * | 2011-02-14 | 2012-06-22 | 동국대학교 산학협력단 | Nonvolatile memory device using the resistive switching of graphene oxide and the fabrication method thereof |
Non-Patent Citations (1)
Title |
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QIQI LIN等: ""Human hair keratin for physically transient resistive switching memory devices"" * |
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