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碳烟与气态和吸附态NO_2反应的不同机制

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摘要 在K/MgAlO催化剂上测试了气态及吸附态NO2与碳烟(soot)的反应,结合原位红外表征和第一性原理计算确认了反应中间物,对两类反应的差异进行了机理解析.结果表明,吸附态NO2的活性弱于气态NO2.吸附态NO2以硝酸盐的形式参与反应,导致出现了2个红外特征峰2234和2110 cm-1,分别归属为K位上的氰酸离子和MgAlO载体上的氰离子.此外,气态NO2的反应中间物异氰酸离子也得到证实.吸附态NO2(即硝酸盐)的反应受到K+静电场的束缚,倾向于形成氰酸离子,氰酸离子易裂解成氰离子迁移到载体上;气态NO2与碳烟反应则倾向于形成相对稳定的异氰酸离子.吸附态NO2较弱的低温活性可归因于K+静电场的束缚.
出处 《科学通报》 EI CAS CSCD 北大核心 2014年第26期2604-2608,共5页 Chinese Science Bulletin
基金 国家自然科学基金(21307142 21077043 21107030 21277060) 中国博士后科学基金(2013M531490) 浙江省博士后择优项目(BSH1302053)资助
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