光谱解析低温等离子体中O_2，N_2，CO_2的活性中间体及其环境化学行为
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摘要
低温等离子体技术在处理密闭舱室中低浓度、大气量、多品种有机污染物和分解CO2制氧气方面具有特殊的优势,但仍然面临着难以解决的问题:抑制有害副产物的生成和提高反应的选择性。要解决这些问题需要系统研究等离子体化学反应机理,需要搞清放电体系中各种气体组份的变化特征以及相互作用规律。
本文以低温等离子体处理密闭舱室有机污染物时最常用的空气分子O2、N2、N2/O2、CO2等为放电体系,以大气压介质阻挡放电为等离子体产生方式,以放电时各种活性基团产生的发射光谱为主要研究手段,研究放电过程中产生的活性基团的类型、能量特征、化学活性、浓度变化规律和相互之间的化学反应过程。
研究表明:
1、氧气介质阻挡放电时产生的活性基团主要是各种能量在9.15~15.78 eV之间的激发态氧原子、激发态氧分子和能量高于15 eV的氧分子离子,当氧气中含有少量水蒸气时还会产生OH自由基和能量更高的激发态O+离子;这些活性物种的形成涉及氧气分子的激发、离解和电离等多种过程,氧分子激发产生的亚稳态及离解产生的氧原子是导致氧气电离激发和一系列高激发态氧原子生成的主要因素,这些活性基团是氧化分解气态有机污染物时最主要的氧化剂和能量来源;
2、氮气放电时活性物种主要是能量在6至11 eV的不同激发态氮气分子及少量的N2+、NO和激发态N原子,增大放电频率能减少基态和激发态的NO浓度;
3、N2/O2混合放电时,随着氧气含量的增加,五重态氮分子和NO迅速减少,而高能量、高活性的的浓度明显增大,同时电子温度也明显升高,因此,N2/O2混合气体提供的更多高能量活性基团和高能量电子有利于提高处理污染物的效率;
4、CO2放电时活性基团主要是激发态CO、CO2+以及O原子,在常压介质阻挡放电这种温和的实验条件下,CO2分子也能够分解为CO、C和O2;
5、量子化学计算表明,CO2在放电中存在三种分解途径,其中三重态分解途径能垒最低,是低能量放电体系中最可能的分解途径。
Although low temperature plasma has great advantage in treating gaseous organic pollutants, which are low in concentration, great in quantity, numerous in varieties, and oxygen generating by decomposing CO2. Some solved difficultly problems are still existing. They are how to inhibit harmful byproducts and enhance selectivity of reactions. There are some subjects, such as the mechanism of plasma chemical reaction, the change laws of gas components, and the rule of reactions of active species.
The main purposes in this thesis are going to study the varieties, energy characteristics, chemical activity, the change laws in concentration, and chemical reactions of active species generated in discharges. The main researches are arranged following.
1. The active species in oxygen dielectric barrier discharge mainly were excited oxygen atoms (9.15~15.78 eV), excited oxygen molecules and oxygen molecular ions (>15 eV). The OH Free Radical and more energic oxygen ions O+ exist in damp oxygen DBD. It has been affirmed that the oxygen atom dissociated from molecule one is the dominant species to producing a serial of higher excited state of oxygen atom and the ionized oxygen molecules.
2. The active species in DBD of oxygen mainly were various excited nitrogen molecules (6~11 eV) and a spot of N2+, NO, excited nitrogen atoms. The concentration of NO was decreased by increasing the dischare frequency.
3. In DBD of the N2/O2 mixture, with increasing concentration of oxygen, the quintuple states nitrogen molecules and NO were decreasing quickly, and the concentration of was increased obviously, and the electron temperature was ncreased markedly. Therefore, the many more energic active species and energic electron generated in N2/O2 discharge were beneficial to enhance the efficiency of treating pollutants.
4. The active species in DBD of CO2 mainly were excited CO, CO2+ and O. Carbon dioxide can be decomposed into carbon monoxide, oxygen and carbon in DBD that is a gentle discharge.
5. The results of Quantum Chemistry Calculation showed that the triplet states decomposing path was the most possible in low energy discharge systems.
本文以低温等离子体处理密闭舱室有机污染物时最常用的空气分子O2、N2、N2/O2、CO2等为放电体系,以大气压介质阻挡放电为等离子体产生方式,以放电时各种活性基团产生的发射光谱为主要研究手段,研究放电过程中产生的活性基团的类型、能量特征、化学活性、浓度变化规律和相互之间的化学反应过程。
研究表明:
1、氧气介质阻挡放电时产生的活性基团主要是各种能量在9.15~15.78 eV之间的激发态氧原子、激发态氧分子和能量高于15 eV的氧分子离子,当氧气中含有少量水蒸气时还会产生OH自由基和能量更高的激发态O+离子;这些活性物种的形成涉及氧气分子的激发、离解和电离等多种过程,氧分子激发产生的亚稳态及离解产生的氧原子是导致氧气电离激发和一系列高激发态氧原子生成的主要因素,这些活性基团是氧化分解气态有机污染物时最主要的氧化剂和能量来源;
2、氮气放电时活性物种主要是能量在6至11 eV的不同激发态氮气分子及少量的N2+、NO和激发态N原子,增大放电频率能减少基态和激发态的NO浓度;
3、N2/O2混合放电时,随着氧气含量的增加,五重态氮分子和NO迅速减少,而高能量、高活性的的浓度明显增大,同时电子温度也明显升高,因此,N2/O2混合气体提供的更多高能量活性基团和高能量电子有利于提高处理污染物的效率;
4、CO2放电时活性基团主要是激发态CO、CO2+以及O原子,在常压介质阻挡放电这种温和的实验条件下,CO2分子也能够分解为CO、C和O2;
5、量子化学计算表明,CO2在放电中存在三种分解途径,其中三重态分解途径能垒最低,是低能量放电体系中最可能的分解途径。
Although low temperature plasma has great advantage in treating gaseous organic pollutants, which are low in concentration, great in quantity, numerous in varieties, and oxygen generating by decomposing CO2. Some solved difficultly problems are still existing. They are how to inhibit harmful byproducts and enhance selectivity of reactions. There are some subjects, such as the mechanism of plasma chemical reaction, the change laws of gas components, and the rule of reactions of active species.
The main purposes in this thesis are going to study the varieties, energy characteristics, chemical activity, the change laws in concentration, and chemical reactions of active species generated in discharges. The main researches are arranged following.
1. The active species in oxygen dielectric barrier discharge mainly were excited oxygen atoms (9.15~15.78 eV), excited oxygen molecules and oxygen molecular ions (>15 eV). The OH Free Radical and more energic oxygen ions O+ exist in damp oxygen DBD. It has been affirmed that the oxygen atom dissociated from molecule one is the dominant species to producing a serial of higher excited state of oxygen atom and the ionized oxygen molecules.
2. The active species in DBD of oxygen mainly were various excited nitrogen molecules (6~11 eV) and a spot of N2+, NO, excited nitrogen atoms. The concentration of NO was decreased by increasing the dischare frequency.
3. In DBD of the N2/O2 mixture, with increasing concentration of oxygen, the quintuple states nitrogen molecules and NO were decreasing quickly, and the concentration of was increased obviously, and the electron temperature was ncreased markedly. Therefore, the many more energic active species and energic electron generated in N2/O2 discharge were beneficial to enhance the efficiency of treating pollutants.
4. The active species in DBD of CO2 mainly were excited CO, CO2+ and O. Carbon dioxide can be decomposed into carbon monoxide, oxygen and carbon in DBD that is a gentle discharge.
5. The results of Quantum Chemistry Calculation showed that the triplet states decomposing path was the most possible in low energy discharge systems.
引文
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