The uptake of 2-methyl-3-buten-2-ol into aqueous mixed solutions of sulfuric acid and hydrogen peroxide.
The uptake of 2-methyl-3-buten-2-ol into aqueous mixed solutions of sulfuric acid and hydrogen peroxide.
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DOI：
10.1039/c0cp00905a
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发表时间：
2011-01
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影响因子：
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通讯作者：
Ze Liu;Maofa Ge;Weigang Wang;S. Yin;Shengrui Tong
中科院分区：
文献类型：
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作者：
Ze Liu;Maofa Ge;Weigang Wang;S. Yin;Shengrui Tong
近年来，多相酸催化氧化异戊二烯及其气相氧化产物制备SOA的研究已被认为是一条很有潜力的途径，但该过程的动力学和化学机理尚不清楚。采用旋转湿壁反应器和差分泵浦单光子电离飞行时间质谱仪（RWW-SPI-TOFMS），研究了2-甲基-3-丁烯-2-醇（MBO）在H2O（2）和H2SO（4）混合水溶液中的吸收行为。首次获得了反应吸收系数（γ），并根据产物信息推测了反应途径。MBO在H（2）SO（4）-H（2）O（2）混合溶液中的反应吸收系数远大于在H（2）SO（4）溶液中的反应吸收系数。乙醛，丙酮和在线产品，其中转化为异戊二烯容易在离线实验的持续时间，建议作为该过程中的产品。在酸性溶液中，羰基产物可以进一步反应，这可能在SOA的形成中起作用。此外，在真实的大气中，在线产物易于转化为异戊二烯，这是公认的生物源SOA的前体。因此，MBO与H（2）O（2）的多相酸催化氧化可能是SOA负载的潜在贡献者。
Multiphase acid-catalyzed oxidation with hydrogen peroxide (H(2)O(2)) has been suggested recently to be a potential route to SOA formation from isoprene and its gas-phase oxidation products, the kinetics and chemical mechanism of this process have not been well-known yet. In this work, the uptake of 2-methyl-3-buten-2-ol (MBO), an important biogenic hydrocarbon and structurally similar to isoprene, into aqueous mixed solutions of H(2)O(2) and sulfuric acid (H(2)SO(4)) was performed using a rotated wetted-wall reactor coupled to a differentially pumped single-photon ionization time of flight mass spectrometer (RWW-SPI-TOFMS). The reactive uptake coefficients (γ) were acquired for the first time and the reaction pathways were deduced according to products information. The reactive uptake coefficients of MBO into H(2)SO(4)-H(2)O(2) mixed solutions are much greater than that into H(2)SO(4) solutions. Acetaldehyde, acetone and an on-line product, which transformed to isoprene readily in the duration of an off-line experiment, were suggested as products in this process. The further reactions of the carbonyl products can occur in acidic solution, which may play a role in SOA formation. Additionally, in real atmosphere the on-line product is apt to transform to isoprene, an acknowledged precursor of biogenic SOA. Thus, the multiphase acid-catalyzed oxidation of MBO with H(2)O(2) might be a potential contributor to SOA loading.