Study on the Mechanism of Carbon/NO_x Reaction by Using Isotopes

同位素研究碳/NO_x反应机理

• 批准号: 08455369
• 负责人: TOMITA Akira
• 金额: $ 4.29万
• 依托单位: Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 1996
• 资助国家: 日本
• 起止时间: 1996 至 1997
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-08455369/
• 关键词: Carbon; NO_x; N_2O; Reaction mechanism; Coal combustion; Surface species; 流動層燃焼; NO; ガス化

Nitrogen oxide reduction with carbon has been studied as a possible way to eliminate this pollutant involved in the ozone layr depletion, acidic rain falls and global warming. In order to obtain the fundamental reaction pathways occurring in the fluidized bed reactor, we have studied the reaction mechanism between carbon and NO_x and N_2O.The principal technique used was the step response experiments using isotope gases. For example, by switching the reactant gas from ^<15>N^<18>O to ^<14>N^<16>O,we can speculate the behavior of surface ^<15>N species or surfhce ^<18>O species during the reaction with ^<14>N^<16>O.From these experiments, it was clearly concluded that the main N_2 formation during C-NO reaction is the reaction between C (N) and NO.By using a similar technique, we also clarified the reaction mechanism between carbon and N_2O.During the reaction of carbon with a mixture of ^<14>N2^<16>O and ^<15>N_2^<16>O,no formation of ^<14>N^<15>N was observed, suggesting the splitting of N_2 from N_2O without N-N bond breakage.The simulation of these reactions were also studied by using molecular orbital calculation, and we found that the above mechanisms are quite reasonable.

碳还原氮氧化物是消除臭氧层破坏、酸雨福尔斯和全球变暖的一种可能途径。为了获得流化床反应器中发生的基本反应途径，我们研究了碳与NO_x和N_2O之间的反应机理。例如，通过将反应气体从^<15>N^<18>O切换到^<14>N^<16>O，我们可以推测表面^<15>N物种或表面^<18>O物种在与^<14>N^<16>O反应过程中的行为。从这些实验中可以清楚地得出结论，在C-NO反应过程中，N_2的主要生成是C（N）与NO之间的反应。通过使用类似的技术，我们还阐明了碳与N_2O之间的反应机理。在碳与^<14>N_2 ^<16>O和^<15>N_2^<16>O的混合物的反应过程中，没有观察到^<14>N^<15>N的生成，用分子轨道计算方法对N_2与N_2O的反应进行了模拟，发现上述机理是合理的。

项目成果

Ph.Chambrion, Hironori Orikasa, Takeshi Suzuki, Takashi Kyotani and Akira Tomita: "A Study of the C-NO Reaction by Using Isotopically Labeled C and NO" Fuel. 76 (6). 493-498 (1997)

Ph.Chambrion、Hironori Orikasa、Takeshi Suzuki、Takashi Kyotani 和 Akira Tomita：“使用同位素标记的 C 和 NO”燃料进行 C-NO 反应的研究。

Ph.Chambrion ら: "XPS of Nitrogen-Containing Functional Groups Formed dUring the C/NO Reaction" Energy Fuels. 11(3). 681-685 (1997)

Ph. Chambrion 等人：“C/NO 反应期间形成的含氮官能团的 XPS”能源燃料 11(3) (1997)。

Ph.Chambrion, T.Suzuki, Z.-G.Zhang, T.Kyotani and A.Tomita: "XPS of Nitrogen-Contining Functional Groups Formed during the C/NO Reaction" Energy Fuels. 11 (3). 681-685 (1997)

Ph.Chambrion、T.Suzuki、Z.-G.Zhang、T.Kyotani 和 A.Tomita：“C/NO 反应期间形成的含氮官能团的 XPS”能源燃料。

Ph.Chambrion ら: "A Study of the C-NO Reaction by Using Isotopically Labeled C and NO" Fuel. 76(6). 493-498 (1997)

Ph. Chambrion 等人：“使用同位素标记的 C 和 NO 进行 C-NO 反应的研究”Fuel 76(6) (1997)。

Ph.Chambrion ら: "XPS of Nitrogen-Containing Functional Groups Formed during the C/NO Reaction" Enegry Fuals. 11(3). 681-685 (1997)

Ph. Chambrion 等人：“C/NO 反应期间形成的含氮官能团的 XPS”Enegry Fuals 11(3) (1997)。