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CN1694207A - Method for preparing silver/carbon nanotube field emission cold cathode at low temperature - Google Patents

Method for preparing silver/carbon nanotube field emission cold cathode at low temperature Download PDF

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Publication number
CN1694207A
CN1694207A CN 200510013650 CN200510013650A CN1694207A CN 1694207 A CN1694207 A CN 1694207A CN 200510013650 CN200510013650 CN 200510013650 CN 200510013650 A CN200510013650 A CN 200510013650A CN 1694207 A CN1694207 A CN 1694207A
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China
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cathode
field emission
silver
tube
carbon nanotube
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CN 200510013650
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Chinese (zh)
Inventor
李海燕
张之圣
胡明
崔屾
吴裕功
王秀宇
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Tianjin University
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Tianjin University
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Abstract

The invention discloses a method for preparing silver/carbon nanometer tube field transmitting cold-cathode at low temp. This method includes mixing the nanometer silver tube and the carbon nanometer tube according to the mass ratio mixing the mixture in acetone, the ethyl alcohol, normal heptane and normal butyl alcohol solution, dispersing by the mechanical agitation and the supersonic wave forming spray size. Manufacturing field transmitting cold-cathode copper bottom electrode on glass, quartz, silicon substrate by magnetic suputtering method hyperthermic sintering in bake over, removing the mask, making the silver/carbon nanometer tube field transmitting cold-cathode. The advantages are good electric conductivity and strong adhesive the carbon nanometer tube may fully exposed on the surface of field transmitting cold-cathode.

Description

The method of preparing silver/carbon nanotube field transmitting cold-cathode at low temp
Technical field
The present invention relates to a kind of method, just belong to the technology that sintering prepares field emission cold-cathode by unordered made of carbon nanotubes field emission cold-cathode.
Background technology
Carbon nano-tube field emission display has vast market and good application prospects because of having low, the advantages such as brightness is big, resolution is high, response speed is fast, power consumption is little, good stability of the electric field of unlatching in the flat panel display field.Along with the continuous development of made of carbon nanotubes technology, more company and R﹠D institution are engaged in the development work of carbon nanotube field emission plane display.Main at present employing disordered carbon nanotube or carbon nano pipe array prepare field emission cold-cathode, because of screen effect problem between the caking property of carbon nano pipe array and substrate, the carbon nano-tube also is not well solved, the development of carbon nano pipe array Field Emission Display is subjected to certain limitation.And unordered made of carbon nanotubes is simple, output is big, cost is low, be fit to commercially produce, Korea S Samsung adopts conductive epoxy resin to mix with carbon nano-tube, method with silk screen printing prepares carbon nanotube field transmitting cold-cathode, and then produces the carbon nanotube field emission plane display suitable with the cathode-ray tube display performance; In addition, domestic scientific research personnel adopts method high temperature such as silver slurry or metal powder fusion preparation carbon nanotube field transmitting cold-cathode down.Adopt epoxy resin (mixing the conductivity that metallic particles increases resin sometimes) to have low, the easy shortcoming such as aging, poor reliability of conductivity, because carbon nano-tube usually is embedded in the epoxy resin influence emission effciency as binding agent.It is less to adopt conductive silver paste and metal powder fusion method to prepare the contact resistance of carbon nanotube field transmitting cold-cathode, but needs higher sintering temperature (500-1200 ℃), and the destructible carbon nano-tube also is unfavorable for the integrated of device; Because the particle diameter of metallic particles such as silver is (more than tens of microns) greatly, make the surface irregularity of field emission cold-cathode, influence the even distribution of carbon nano-tube, and then the control of an influence emission effciency and pixel.
Summary of the invention
The purpose of this invention is to provide a kind of method of utilizing nano-Ag particles to prepare carbon nanotube field transmitting cold-cathode, adopt this method can significantly improve conductivity and caking property between carbon nano-tube and the substrate, carbon nano-tube can be exposed to the field emission cold-cathode surface fully; Low preparation temperature can make carbon nano-tube field emission display spare and semiconductor technology compatibility, has quickened carbon nano-tube field emission display spare commercialization process.
The present invention is realized that by the following technical programs a kind of method of preparing silver/carbon nanotube field transmitting cold-cathode at low temp is characterized in that comprising following process:
1) nano-Ag particles of particle diameter 5-30nm and the carbon nano-tube of diameter 20-100nm are pressed mass ratio 10: 1-1: 3 mix, this mixture is added (4-5) by volume: (2-4): (1-3): (0.5-3) in the acetone of Hun Heing, ethanol, normal heptane and the butanol solution, adopt mechanical agitation and ultrasonic wave to combine and disperse, form the spraying slurry.
2) adopt magnetron sputtering method on glass, quartz, silicon base, to prepare the copper hearth electrode of field emission cold-cathode.
3) utilize mask to spray slurry on hearth electrode, carry out the temperature programming sintering then in baking oven, programming rate 0.1-2 ℃/min, sintering temperature arrives 140-200 ℃, and more than the insulation 1h.
4) remove mask, make the silver/carbon nanotube field transmitting cold-cathode of thickness 0.5-3 μ m.
Beneficial effect of the present invention is: adopt nano-Ag particles and carbon nano-tube to be mixed with field emission cold-cathode, promptly have caking property by force, the advantage that conducts electricity very well, its side's resistance can reach 0.007 Ω/below the.Because silver-colored particle grain size is less than the diameter of carbon nano-tube, under settlement action, the top of carbon nano-tube is exposed at the field emission cold-cathode surface, forms transmitting terminal, and the quality by nano-Ag particles and carbon nano-tube is than may command cold-cathode field emission.Because the volatility of acetone, ethanol, normal heptane and n-butanol is different, in the process that the carbon nano-tube cold cathode is shaped, it is smooth that its surface can keep.The more important thing is,, can utilize conventional semiconductor technology and printed circuit technology to produce the carbon nanotube field emission plane display, will promote commercially producing of carbon nanotube field emission plane display greatly because sintering temperature is low.
Description of drawings
Fig. 1 the present invention prepares carbon nanotube field transmitting cold-cathode method flow block diagram
High-resolution transmission electron microscope (HRTEM) photo of Fig. 2 silver nano-grain
The carbon nano-tube root is embedded in the TEM photo in the silverskin behind Fig. 3 sintering
Fig. 4 nano-Ag particles and carbon nano-tube are scanning electron microscopy (SEM) photo of the field emission cold-cathode surface topography of preparation in 5: 1 o'clock by mass ratio
Fig. 5 nano-Ag particles and carbon nano-tube by mass ratio be preparation in 2: 1 o'clock the SEM photo of field emission cold-cathode surface topography
Fig. 6 bottom nano-Ag particles and carbon nano-tube are 10: 1 o'clock by mass ratio, and second layer nano-Ag particles and carbon nano-tube are the SEM photo of the field emission cold-cathode surface topography of preparation in 1: 1 o'clock by mass ratio
Embodiment
Multi-walled carbon nano-tubes with silver nano-grain and catalystic pyrolysis preparation is that example illustrates how to implement the present invention, the invention is not restricted to these embodiment.
Embodiment 1 (as shown in Figure 1)
The nano-Ag particles of particle diameter 5-30nm and the carbon nano-tube of diameter 20-100nm are pressed mass ratio mixing in 5: 1, mixture is joined by 5: 4: 2: in the acetone of 1 mixed, ethanol, normal heptane and the butanol solution, the mode that adopts mechanical agitation and ultrasonic wave to combine is disperseed, and forms the spraying slurry.Adopting glass, quartz or silicon is substrate, and it is comprised that sulfuric acid carries out pickling, after deionized water is cleaned, cleans with acetone again, after the oven dry, will adopt magnetron sputtering method to prepare the copper hearth electrode of field emission cold-cathode in substrate.Utilize mask to spray slurry on hearth electrode, carry out the temperature programming sintering then in baking oven, 0.5 ℃/min of programming rate arrives 185 ℃ of sintering temperatures, and insulation 1.5h.Make the silver/carbon nanotube field transmitting cold-cathode of the about 1.5 μ m of average thickness behind the removal mask, carbon nano-tube bottom and substrate well bond together.The cold cathode surface topography as shown in Figure 4, cold cathode surface side resistance about 0.007 Ω/.Field emission experiment result shows that the carbon nanotube field transmitting cold-cathode emitting performance of this method preparation is better, and an emission and threshold field intensity are respectively 8mAcm -2, 4.8V μ m -1
Embodiment 2
Present embodiment is similar to embodiment 1, difference is that the mass ratio of nano-Ag particles and carbon nano-tube is 2: 1 in the step 1, and the sintering temperature that changes in the step 3 is 160 ℃, the cold cathode surface topography as shown in Figure 5, cold cathode surface side resistance about 0.009 Ω/, an emission and threshold field intensity are respectively 29mAcm -2, 4.3V μ m -1
Embodiment 3
Present embodiment is similar to embodiment 1, difference is that step 3 spraying earlier is 10: 1 slurry with the mass ratio of nano-Ag particles and carbon nano-tube, after drying by the fire 0.5h under slowly being warming up to 100 ℃, the mass ratio that sprays nano-Ag particles and carbon nano-tube again is 2: 1 a slurry, the cold cathode surface topography as shown in Figure 6 when sintering temperature was 200 ℃, cold cathode surface side resistance about 0.008 Ω/, an emission and threshold field intensity are respectively 31mAcm -2, 3.9V μ m -1
Embodiment 4
Present embodiment is similar to embodiment 1, difference is that the mass ratio of nano-Ag particles and carbon nano-tube is 1: 1 in the step 1, and the sintering temperature that changes in the step 3 is 140 ℃, and cold cathode surface side hinders about 0.037 Ω/, and field emission and threshold field intensity are respectively 19mAcm -2, 5.2V μ m -1

Claims (1)

1.一种低温下制备银/碳纳米管场发射冷阴极的方法,其特征在于包括以下过程:1. a method for preparing silver/carbon nanotube field emission cold cathodes at a low temperature is characterized in that comprising the following processes: 1)将粒径5-30nm的纳米银颗粒和直径20-100nm的碳纳米管按质量比10∶1-1∶3混合,将该混合物加入按体积比(4-5)∶(2-4)∶(1-3)∶(0.5-3)混合的丙酮、乙醇、正庚烷和正丁醇溶液中,采用机械搅拌和超声波相结合进行分散,形成喷涂浆料;1) Mix nano-silver particles with a particle diameter of 5-30nm and carbon nanotubes with a diameter of 20-100nm in a mass ratio of 10:1-1:3, and add the mixture in a volume ratio of (4-5):(2-4 ): (1-3): (0.5-3) In the mixed acetone, ethanol, n-heptane and n-butanol solutions, mechanical stirring and ultrasonic waves are used to disperse to form a spray slurry; 2)采用磁控溅射法在玻璃、石英、硅基底上制备场发射冷阴极的铜底电极;2) Prepare the copper bottom electrode of the field emission cold cathode on the glass, quartz and silicon substrates by magnetron sputtering; 3)利用掩膜在底电极上喷涂浆料,然后在烘箱内进行程序升温烧结,升温速度0.1-2℃/min,烧结温度到达140-200℃,并保温1h以上;3) Use a mask to spray the slurry on the bottom electrode, and then perform temperature-programmed sintering in an oven at a heating rate of 0.1-2°C/min, and the sintering temperature reaches 140-200°C, and keep it warm for more than 1 hour; 4)去除掩膜,制成厚度0.5-3μm的银/碳纳米管场发射冷阴极。4) Remove the mask to make a silver/carbon nanotube field emission cold cathode with a thickness of 0.5-3 μm.
CN 200510013650 2005-06-01 2005-06-01 Method for preparing silver/carbon nanotube field emission cold cathode at low temperature Pending CN1694207A (en)

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7887878B2 (en) 2006-12-07 2011-02-15 Electronics And Telecommunications Research Institute Method of manufacturing a fine-patternable, carbon nano-tube emitter with high reliabilty
CN103871802A (en) * 2012-12-15 2014-06-18 中国科学院深圳先进技术研究院 Carbon nanotube composite thin film field emission cathode preparation method
CN106745365A (en) * 2016-12-05 2017-05-31 南京悠谷知识产权服务有限公司 A kind of water purification material and preparation method thereof
CN111128635A (en) * 2019-12-24 2020-05-08 中国工程物理研究院应用电子学研究所 High-current repetition frequency carbon nanotube reinforced silver cold cathode and preparation method thereof

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7887878B2 (en) 2006-12-07 2011-02-15 Electronics And Telecommunications Research Institute Method of manufacturing a fine-patternable, carbon nano-tube emitter with high reliabilty
CN103871802A (en) * 2012-12-15 2014-06-18 中国科学院深圳先进技术研究院 Carbon nanotube composite thin film field emission cathode preparation method
CN103871802B (en) * 2012-12-15 2016-09-07 中国科学院深圳先进技术研究院 The preparation method of carbon nano-tube coextruded film field-transmitting cathode
CN106745365A (en) * 2016-12-05 2017-05-31 南京悠谷知识产权服务有限公司 A kind of water purification material and preparation method thereof
CN111128635A (en) * 2019-12-24 2020-05-08 中国工程物理研究院应用电子学研究所 High-current repetition frequency carbon nanotube reinforced silver cold cathode and preparation method thereof
CN111128635B (en) * 2019-12-24 2023-04-07 中国工程物理研究院应用电子学研究所 High-current repetition frequency carbon nanotube reinforced silver cold cathode and preparation method thereof

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