聚苯胺/半导体金属氧化物基光敏材料的制备及其光电器件的设计
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摘要
半导体纳米材料具有独特的光电特性，在各种光电功能器件方面（如光探测器，光开关，太阳能电池等）有着广泛的应用前景。探索并开发新的光敏性半导体材料，设计并制造新的光电子器件成为当前的研究热点之一。本论文中，以导电聚苯胺和金属氧化物半导体纳米材料为研究对象，利用固相法，水热法，界面法，静电纺丝法等，制备出优化的半导体材料或其复合结构，研究并讨论了其光敏性。并且利用N型金属氧化物和P型聚苯胺之间形成的P-N结特性，设计了N-P-N结构的光探测器。主要工作如下：
1.通过一步固相反应，将高锰酸钾用苯胺单体进行还原，我们得到了二氧化锰/聚苯胺复合材料，并且第一次报道了二氧化锰纳米复合材料的光敏性,这为我们提供了一个制备紫外光敏材料的新方法。紫外光敏性的产生归因于聚苯胺的相关能级与二氧化锰的价带和导带相匹配，在电子传递过程中，聚苯胺起到了一个桥梁的作用，可以帮助二氧化锰传递电子，这样使更多的电子可以从二氧化锰的价带转移到导带。
2.通过简单的固相反应，我们将氧化铋和氧化钒利用聚苯胺进行表面功能化，从而第一次实现了氧化铋和氧化钒的紫外和可见光响应。这表明，通过将金属氧化物表面功能化上具有很强光吸收能力，并且能级与金属氧化物相匹配的聚合物以后，金属氧化物的紫外或可见光电流响应可以被诱导，使其从无到有。
3.我们设计了一个相对独立的紫外光探测器，该三明治结构的光探测器由一层P型聚苯胺纳米纤维（PANI）、两层N型氧化锌纳米棒（ZnO）所组成，与其他光探测器不同的是，它不需要任何额外的偏压只需要紫外光即可工作。光电流的产生受到两个相反的P-N异质结所控制，在零伏的偏压下，我们可以获得高的光电流（1.4×10~(-5)A）和高的光敏度（>10~5），定义为（I光照-I黑暗）/I光照。
4.我们报道了一个新型的三明治结构的光探测器，该光探测器由一层氧化锌纳米棒，一层聚苯胺纳米网，一层染料修饰的氧化锌纳米棒组成。在没有任何额外偏压的作用下，该光探测器仅仅依靠由P-N结所形成的内电场就可以工作。并且当从同一个方向分别照射紫外和可见光时，该光探测器可以产生相反的光电流响应。
5.利用TiO_2和聚苯胺的能级匹配，通过简单的方法，我们制造了TiO_2/聚苯胺核壳结构纳米纤维。当纤维在没有氧气存在的条件下被紫外光照射时，光电导增加，这与之前报道过的UV光敏材料的光敏现象类似。然而，当核壳结构纳米纤维在充满氧气的环境下测试时，我们看到了不同于其他光敏材料的现象。在其他报道中，在UV光照下产生电子空穴对，最终会增加光敏材料的光电导。而在我们的实验中，纤维的光电导会随着紫外灯的开启而减小，这是由于TiO_2吸附越多的氧气，TiO_2核和聚苯胺壳之间的P-N结的耗尽区就越厚造成的。
Semiconductor nanomaterial has wide application prospects in various photoelectronicfunctional devices such as photodetectors, photoswitches and solar cells owing to itsdistinctive and outstanding photoelectric characteristics. To explore and develop newphotosensitive semiconductor materials, to design and fabricate new photoelectric deviceshave attracted a great deal of research interest. This dissertation focused on conductingpolyaniline and metal oxide semiconductor nanomaterials. The optimal semiconductornanomaterials and their composites were prepared by solid-state reaction, hydrothermalmethod, interfacial polymerization, electrospinning technique, and the photosensitive propertyof them was investigated and discussed. Using the P-N junction between N-type metal oxideand P-type polyaniline, the N-P-N structural photodetectors were designed and the mainachievements were summarized as follows:
1. We present a facile synthesis of manganese oxide (MnO_2) nanocomposite with ultraviolet(UV) photosensitive characteristic by a solid-state reaction based on the reduction ofpotassium permanganate (KMnO4) by aniline, which provides a new family and moreselectivity for UV photosensitive nanomaterials in the future. The UV photosensitivemechanism are attributed that the energy level of polyaniline lie in the band gap of the MnO_2and serve as a bridge to transport the photogenerated electrons in MnO_2, then more electronscan be transport from vanlence band to conductor band in MnO_2.
2. We have developed a method, surface-functionalization with well-matched energy level,to induce ultraviolet (UV) or visible (Vis) photoresponse of semiconductor material film fromnot only weak to strong but also nothing to something. By this way, UV and Visphotoresponses of two metal oxides, Bi_2O_3and V_2O_5, have been realized for the first time byfunctionalizing them with polyaniline (PANI).
3. We demonstrate a relatively independent UV photodetector which is composed of onelayer of p-type PANI nanowires and two layers of n-type ZnO nanorods. Different to otherUV photoelectronic nanodevices, it doesn’t need any external power source except UV lightwhen it works. High photocurrent (~1.4×10~(-5)A) and photosensitivity (>10~5), defined as(Iphoto-Idark)/Idark, at zero bias have been obtained, which can be attributed to the design of thetwo opposite p–n heterojunctions in the UV photodetectors.
4. We have designed and fabricated a novel photodetector that is composed ofsandwich-structured n-type zinc oxide nanorods arrays, p-type polyaniline thin film, anddye-modified n-type ZnO nanorods arrays. When the photodetector is alternatively illuminated by ultraviolet and visible light from the same direction, it outputs alternatingcurrent.
5. The TiO_2/polyaniline (PANI) core-shell nanofibers with unique ultraviolet photoresponse(UV) were designed and fabricated. When the core-shell nanofibers were performed in nooxygen (O_2) and full of O_2environment under UV illumination respectively, the increase anddecrease of photoconduction were observed. The mechanism of the opposite photocurrentresponse of the core-shell materials was investigated in detail, which indicated that thedecrease of the photoconduction in O_2was caused by the increasement of the thickness for thedepletion zone.
1.通过一步固相反应，将高锰酸钾用苯胺单体进行还原，我们得到了二氧化锰/聚苯胺复合材料，并且第一次报道了二氧化锰纳米复合材料的光敏性,这为我们提供了一个制备紫外光敏材料的新方法。紫外光敏性的产生归因于聚苯胺的相关能级与二氧化锰的价带和导带相匹配，在电子传递过程中，聚苯胺起到了一个桥梁的作用，可以帮助二氧化锰传递电子，这样使更多的电子可以从二氧化锰的价带转移到导带。
2.通过简单的固相反应，我们将氧化铋和氧化钒利用聚苯胺进行表面功能化，从而第一次实现了氧化铋和氧化钒的紫外和可见光响应。这表明，通过将金属氧化物表面功能化上具有很强光吸收能力，并且能级与金属氧化物相匹配的聚合物以后，金属氧化物的紫外或可见光电流响应可以被诱导，使其从无到有。
3.我们设计了一个相对独立的紫外光探测器，该三明治结构的光探测器由一层P型聚苯胺纳米纤维（PANI）、两层N型氧化锌纳米棒（ZnO）所组成，与其他光探测器不同的是，它不需要任何额外的偏压只需要紫外光即可工作。光电流的产生受到两个相反的P-N异质结所控制，在零伏的偏压下，我们可以获得高的光电流（1.4×10~(-5)A）和高的光敏度（>10~5），定义为（I光照-I黑暗）/I光照。
4.我们报道了一个新型的三明治结构的光探测器，该光探测器由一层氧化锌纳米棒，一层聚苯胺纳米网，一层染料修饰的氧化锌纳米棒组成。在没有任何额外偏压的作用下，该光探测器仅仅依靠由P-N结所形成的内电场就可以工作。并且当从同一个方向分别照射紫外和可见光时，该光探测器可以产生相反的光电流响应。
5.利用TiO_2和聚苯胺的能级匹配，通过简单的方法，我们制造了TiO_2/聚苯胺核壳结构纳米纤维。当纤维在没有氧气存在的条件下被紫外光照射时，光电导增加，这与之前报道过的UV光敏材料的光敏现象类似。然而，当核壳结构纳米纤维在充满氧气的环境下测试时，我们看到了不同于其他光敏材料的现象。在其他报道中，在UV光照下产生电子空穴对，最终会增加光敏材料的光电导。而在我们的实验中，纤维的光电导会随着紫外灯的开启而减小，这是由于TiO_2吸附越多的氧气，TiO_2核和聚苯胺壳之间的P-N结的耗尽区就越厚造成的。
Semiconductor nanomaterial has wide application prospects in various photoelectronicfunctional devices such as photodetectors, photoswitches and solar cells owing to itsdistinctive and outstanding photoelectric characteristics. To explore and develop newphotosensitive semiconductor materials, to design and fabricate new photoelectric deviceshave attracted a great deal of research interest. This dissertation focused on conductingpolyaniline and metal oxide semiconductor nanomaterials. The optimal semiconductornanomaterials and their composites were prepared by solid-state reaction, hydrothermalmethod, interfacial polymerization, electrospinning technique, and the photosensitive propertyof them was investigated and discussed. Using the P-N junction between N-type metal oxideand P-type polyaniline, the N-P-N structural photodetectors were designed and the mainachievements were summarized as follows:
1. We present a facile synthesis of manganese oxide (MnO_2) nanocomposite with ultraviolet(UV) photosensitive characteristic by a solid-state reaction based on the reduction ofpotassium permanganate (KMnO4) by aniline, which provides a new family and moreselectivity for UV photosensitive nanomaterials in the future. The UV photosensitivemechanism are attributed that the energy level of polyaniline lie in the band gap of the MnO_2and serve as a bridge to transport the photogenerated electrons in MnO_2, then more electronscan be transport from vanlence band to conductor band in MnO_2.
2. We have developed a method, surface-functionalization with well-matched energy level,to induce ultraviolet (UV) or visible (Vis) photoresponse of semiconductor material film fromnot only weak to strong but also nothing to something. By this way, UV and Visphotoresponses of two metal oxides, Bi_2O_3and V_2O_5, have been realized for the first time byfunctionalizing them with polyaniline (PANI).
3. We demonstrate a relatively independent UV photodetector which is composed of onelayer of p-type PANI nanowires and two layers of n-type ZnO nanorods. Different to otherUV photoelectronic nanodevices, it doesn’t need any external power source except UV lightwhen it works. High photocurrent (~1.4×10~(-5)A) and photosensitivity (>10~5), defined as(Iphoto-Idark)/Idark, at zero bias have been obtained, which can be attributed to the design of thetwo opposite p–n heterojunctions in the UV photodetectors.
4. We have designed and fabricated a novel photodetector that is composed ofsandwich-structured n-type zinc oxide nanorods arrays, p-type polyaniline thin film, anddye-modified n-type ZnO nanorods arrays. When the photodetector is alternatively illuminated by ultraviolet and visible light from the same direction, it outputs alternatingcurrent.
5. The TiO_2/polyaniline (PANI) core-shell nanofibers with unique ultraviolet photoresponse(UV) were designed and fabricated. When the core-shell nanofibers were performed in nooxygen (O_2) and full of O_2environment under UV illumination respectively, the increase anddecrease of photoconduction were observed. The mechanism of the opposite photocurrentresponse of the core-shell materials was investigated in detail, which indicated that thedecrease of the photoconduction in O_2was caused by the increasement of the thickness for thedepletion zone.
引文
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