多壁碳纳米管的掺杂及其气敏特性研究
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摘要
碳纳米管具有丰富的孔隙结构、大的比表面积和很高的表面能,是一种具有广阔应用前景的气敏材料。论文对多壁碳纳米管的掺杂处理及其对甲醛和二甲苯这两种有机挥发物的气敏特性进行了初步的研究。
室温下,碳纳米管被认为是p型掺杂的半导体,基于多壁碳纳米管的传感器气敏膜吸附了还原性的有机气体分子后,碳管表面的空穴载流子会减少,从而导致气敏膜的导电性能减弱。在恒定的电压下,通过检测传感器的电流的变化对其电导的变化量进行衡量。传感器电导的变化与所吸附的待测气体的浓度成一定的比例关系,气体浓度越大,电流降幅也随之增大。
室温下,多壁碳纳米管对甲醛和二甲苯两种气体显示出良好的灵敏度和选择性,且响应非常稳定。在此基础上,对多壁碳纳米管进行了超声掺杂阳离子,化学还原掺杂Pd,电化学还原掺杂Pd,以及直接用缩合剂在多壁碳纳米管表面修饰十二胺等处理,并测试了掺杂前后多壁碳纳米管对甲醛和二甲苯的气敏响应的变化。不同方法改性后的多壁碳管对于两种待测气体的灵敏度和选择性均有一定变化。掺杂的金属粒子的大小和均匀程度对传感器的响应影响较大。化学还原镀钯处理后传感器的气敏性能提升最为明显,且对两种气体的选择性增强。
为了进一步提高传感器的选择性,对多壁碳纳米管进行了多重掺杂的处理。对化学还原镀钯后的多壁碳纳米管继续进行电化学镀钯处理,并测试碳管的气敏性能；将十二胺修饰的多壁碳纳米管涂布于定向碳纳米管阵列表面,作为具有立体结构的复合气敏材料。这两种方法制备的碳纳米管复合气敏材料对待测气体均显示出良好的选择性,证明多重掺杂是非常有潜力的一种提升多壁碳纳米管选择性气敏响应的制备方法。
掺杂不同的纳米颗粒后,多壁碳纳米管表面与吸附的气体分子之间的电荷转移会因为纳米颗粒的催化作用而发生改变。化学还原镀钯后,Pd粒子可以强化二甲苯分子与碳管之间的电荷交换,从而大幅度的提升碳管对其的气敏响应；修饰了十二胺的多壁碳纳米管则由于长烃链的空间阻隔作用,对二甲苯的气敏响应不显著,而对小分子的甲醛显示出较高的灵敏度和选择性。论文对基于多壁碳纳米管的气体传感器掺杂前后灵敏度和选择性的改变进行了初步的理论分析和计算。
Carbon nanotube has porous microstructure with high surface area and energy, which makes it a promising gas sensing material. In this dissertation, the preparation and characteristic of gas sensor based on doping multi-wall carbon nanotubes (MWNTs) for formaldehyde and xylene detection were discussed.
Carbon nanotube was thought to be p-type semiconductor at room temperature. After adsorption of reducing gas, the density of the hole carrier will decrease, leading to a weakening conductibility of the sensing membrane. With a constant voltage, change of the conductance could be calculated by the change of current. The electrical conductivity of the dried carbon nanotubes film decreased when the electrode was exposed to formaldehyde and xylene. And there was a good linear correlation between the decreasing amplitude and the gas concentration.
MWNT showed highly sensitivity and selectivity during gas detection at room temperature. Cation-doped MWNTs, Pd modified MWNTs, electric plating MWNTs and lauryl amine modified MWNTs were all prepared and detected. The size and uniformity of the doped metal grain were found important to the doping effects. Notable lifting was found to the sensitivity of Pd loaded MWNTs, which also shows intensifying selectivity to xylene.
Multiple doping processing to MWNTs was performed to lift the selectivity of the gas sensor. MWCNTs loaded with palladium by reduction method were then electric plated before used as sensing material. And lauryl amine modified MWNTs were used as doping agent to the highly-ordered carbon nanotubes arrays. Sensing membrane was then fabricated by the complexes of MWNTs and highly-ordered carbon nanotubes arrays. Sensors based on Multiple doping MWNTs show better selectivity, which suggests that Multiple doping processing could be a promising treating method to lift the selectivity of gas sensors.
Doping with different metal particles, charge transmission between the MWNTs and gas could be impacted by their catalysis function. Pd nano-particles loaded by reduction method generated dramatic sensing response to xylene by strengthening the charge delivery between xylene and MWNTs. Lauryl amine modified MWNTs exhibit outstanding sensitivity and selectivity to formaldehyde with long hydrocarbon chain which could obstruct the adsorption of xylene. Preliminary theoretical analysis and calculation were carried out in the dissertation to study the sensing characteristic of the doping MWNTs.
室温下,碳纳米管被认为是p型掺杂的半导体,基于多壁碳纳米管的传感器气敏膜吸附了还原性的有机气体分子后,碳管表面的空穴载流子会减少,从而导致气敏膜的导电性能减弱。在恒定的电压下,通过检测传感器的电流的变化对其电导的变化量进行衡量。传感器电导的变化与所吸附的待测气体的浓度成一定的比例关系,气体浓度越大,电流降幅也随之增大。
室温下,多壁碳纳米管对甲醛和二甲苯两种气体显示出良好的灵敏度和选择性,且响应非常稳定。在此基础上,对多壁碳纳米管进行了超声掺杂阳离子,化学还原掺杂Pd,电化学还原掺杂Pd,以及直接用缩合剂在多壁碳纳米管表面修饰十二胺等处理,并测试了掺杂前后多壁碳纳米管对甲醛和二甲苯的气敏响应的变化。不同方法改性后的多壁碳管对于两种待测气体的灵敏度和选择性均有一定变化。掺杂的金属粒子的大小和均匀程度对传感器的响应影响较大。化学还原镀钯处理后传感器的气敏性能提升最为明显,且对两种气体的选择性增强。
为了进一步提高传感器的选择性,对多壁碳纳米管进行了多重掺杂的处理。对化学还原镀钯后的多壁碳纳米管继续进行电化学镀钯处理,并测试碳管的气敏性能；将十二胺修饰的多壁碳纳米管涂布于定向碳纳米管阵列表面,作为具有立体结构的复合气敏材料。这两种方法制备的碳纳米管复合气敏材料对待测气体均显示出良好的选择性,证明多重掺杂是非常有潜力的一种提升多壁碳纳米管选择性气敏响应的制备方法。
掺杂不同的纳米颗粒后,多壁碳纳米管表面与吸附的气体分子之间的电荷转移会因为纳米颗粒的催化作用而发生改变。化学还原镀钯后,Pd粒子可以强化二甲苯分子与碳管之间的电荷交换,从而大幅度的提升碳管对其的气敏响应；修饰了十二胺的多壁碳纳米管则由于长烃链的空间阻隔作用,对二甲苯的气敏响应不显著,而对小分子的甲醛显示出较高的灵敏度和选择性。论文对基于多壁碳纳米管的气体传感器掺杂前后灵敏度和选择性的改变进行了初步的理论分析和计算。
Carbon nanotube has porous microstructure with high surface area and energy, which makes it a promising gas sensing material. In this dissertation, the preparation and characteristic of gas sensor based on doping multi-wall carbon nanotubes (MWNTs) for formaldehyde and xylene detection were discussed.
Carbon nanotube was thought to be p-type semiconductor at room temperature. After adsorption of reducing gas, the density of the hole carrier will decrease, leading to a weakening conductibility of the sensing membrane. With a constant voltage, change of the conductance could be calculated by the change of current. The electrical conductivity of the dried carbon nanotubes film decreased when the electrode was exposed to formaldehyde and xylene. And there was a good linear correlation between the decreasing amplitude and the gas concentration.
MWNT showed highly sensitivity and selectivity during gas detection at room temperature. Cation-doped MWNTs, Pd modified MWNTs, electric plating MWNTs and lauryl amine modified MWNTs were all prepared and detected. The size and uniformity of the doped metal grain were found important to the doping effects. Notable lifting was found to the sensitivity of Pd loaded MWNTs, which also shows intensifying selectivity to xylene.
Multiple doping processing to MWNTs was performed to lift the selectivity of the gas sensor. MWCNTs loaded with palladium by reduction method were then electric plated before used as sensing material. And lauryl amine modified MWNTs were used as doping agent to the highly-ordered carbon nanotubes arrays. Sensing membrane was then fabricated by the complexes of MWNTs and highly-ordered carbon nanotubes arrays. Sensors based on Multiple doping MWNTs show better selectivity, which suggests that Multiple doping processing could be a promising treating method to lift the selectivity of gas sensors.
Doping with different metal particles, charge transmission between the MWNTs and gas could be impacted by their catalysis function. Pd nano-particles loaded by reduction method generated dramatic sensing response to xylene by strengthening the charge delivery between xylene and MWNTs. Lauryl amine modified MWNTs exhibit outstanding sensitivity and selectivity to formaldehyde with long hydrocarbon chain which could obstruct the adsorption of xylene. Preliminary theoretical analysis and calculation were carried out in the dissertation to study the sensing characteristic of the doping MWNTs.
引文
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