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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Surface-catalyzed chlorine and nitrogen activation: Mechanisms for the heterogeneous formation of ClNO, NO, NO _2, HONO, and N _2O from HNO _3 and HCl on aluminum oxide particle surfaces
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Surface-catalyzed chlorine and nitrogen activation: Mechanisms for the heterogeneous formation of ClNO, NO, NO _2, HONO, and N _2O from HNO _3 and HCl on aluminum oxide particle surfaces

机译：表面催化的氯和氮活化：在氧化铝颗粒表面由HNO _3和HCl异质形成ClNO，NO，NO _2，HONO和N _2O的机理

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摘要

It is well-known that chlorine active species (e.g., Cl _2, ClONO _2, ClONO) can form from heterogeneous reactions between nitrogen oxides and hydrogen chloride on aerosol particle surfaces in the stratosphere. However, less is known about these reactions in the troposphere. In this study, a potential new heterogeneous pathway involving reaction of gaseous HCl and HNO _3 on aluminum oxide particle surfaces, a proxy for mineral dust in the troposphere, is proposed. We combine transmission Fourier transform infrared spectroscopy with X-ray photoelectron spectroscopy to investigate changes in the composition of both gas-phase and surface-bound species during the reaction under different environmental conditions of relative humidity and simulated solar radiation. Exposure of surface nitrate-coated aluminum oxide particles, from prereaction with nitric acid, to gaseous HCl yields several gas-phase products, including ClNO, NO _2, and HNO _3, under dry (RH < 1%) conditions. Under humid more conditions (RH > 20%), NO and N _2O are the only gas products observed. The experimental data suggest that, in the presence of adsorbed water, ClNO is hydrolyzed on the particle surface to yield NO and NO _2, potentially via a HONO intermediate. NO _2 undergoes further hydrolysis via a surface-mediated process, resulting in N _2O as an additional nitrogen-containing product. In the presence of broad-band irradiation (λ > 300 nm) gas-phase products can undergo photochemistry, e.g., ClNO photodissociates to NO and chlorine atoms. The gas-phase product distribution also depends on particle mineralogy (Al _2O _3 vs CaCO _3) and the presence of other coadsorbed gases (e.g., NH _3). These newly identified reaction pathways discussed here involve continuous production of active ozone-depleting chlorine and nitrogen species from stable sinks such as gas-phase HCl and HNO _3 as a result of heterogeneous surface reactions. Given that aluminosilicates represent a major fraction of mineral dust aerosol, aluminum oxide can be used as a model system to begin to understand various aspects of possible reactions on mineral dust aerosol surfaces.
机译：众所周知，平流层中气溶胶颗粒表面上的氮氧化物和氯化氢之间的异质反应可以形成氯活性物质（例如，Cl _2，ClONO _2，ClONO）。但是，对流层中的这些反应知之甚少。在这项研究中，提出了潜在的新的非均质途径，涉及氧化铝颗粒表面上气态HCl和HNO _3的反应，是对流层矿物粉尘的替代物。我们将傅里叶变换红外光谱与X射线光电子能谱相结合，以研究在相对湿度和模拟太阳辐射的不同环境条件下反应过程中气相和表面结合物的组成变化。在干燥（RH <1％）的条件下，表面硝酸盐涂覆的氧化铝颗粒从与硝酸的预反应暴露到气态HCl中，会生成几种气相产物，包括ClNO，NO _2和HNO _3。在更多潮湿条件下（RH> 20％），仅观察到气体产物为NO和N _2O。实验数据表明，在吸附水的存在下，ClNO可能会通过HONO中间体在颗粒表面水解，生成NO和NO _2。 NO _2通过表面介导的过程进一步水解，产生N _2O作为附加的含氮产物。在宽带辐射（λ> 300 nm）的存在下，气相产物可能会经历光化学反应，例如ClNO光解离为NO和氯原子。气相产物的分布还取决于颗粒矿物学（Al _2O _3与CaCO _3）和其他共吸附气体（例如NH _3）的存在。这里讨论的这些新近确定的反应途径涉及由于表面反应不均匀而从稳定的水槽（如气相HCl和HNO_3）连续生产消耗臭氧的活性氯和氮物质。考虑到硅铝酸盐是矿物粉尘气溶胶的主要组成部分，可以将氧化铝用作模型系统，以开始理解矿物粉尘气溶胶表面可能发生反应的各个方面。

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