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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Interaction of Nitrous Acid with Polycrystalline Ice: Adsorption on the Surface and Diffusion into the Bulk
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Interaction of Nitrous Acid with Polycrystalline Ice: Adsorption on the Surface and Diffusion into the Bulk

机译：亚硝酸与多晶冰的相互作用：表面吸附和扩散进入大块

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The thermodynamic and kinetic constants needed to model the interactions of nitrous acid (HONO) with ice were measured. The experiments were done in a packed ice bed flow tube at temperatures between 213 and 253 K and at HONO gas phase concentrations between 0.4 and 137 ppbv. The experiments were performed using radioactively labeled HO~(13)NO molecules. The use of the short-lived isotope ~(13)N (t_(1/2) ≈ 10 min) enabled in situ monitoring of the migration of HO~(13)NO in the flow tube. The measurements showed that the interactions do not only occur through adsorption but also via diffusion into polycrystalline ice. A method is suggested to disentangle the bulk and the surface processes. Using this method, the temperature dependence of the linear partition coefficient was found to be K_(lin.C.HONO)= 7.4 × 10~(-11) exp(5.4 × 10~3/T) in units of m. The enthalpy and entropy of adsorption of HONO on ice were ΔH_(ads,HONO) = -45(±20) kJ mol~(-1) and ΔS~0_(ads,HONO) = -17(±89) J mol~(-1) K~(-1), respectively for the standard conditions A_(std)/V_(std) = 1.7 × 10~9 m~(-1). The time dependent uptake into the bulk was expressed using H*_(cc,HONO)(D_(b,HONO))~(1/2), the product of the dimensionless effective Henry's law constant and the square root of the effective diffusion constant in the bulk of the polycrystalline ice matrix. H*_(cc,HONO)(D_(b,HONO))~(-1/2) was evaluated to 1.6(±69%) × 10~(-2) m s~(-1/2). The results are discussed in the context of HONO partitioning in snowpacks.
机译：测量了模拟亚硝酸（HONO）与冰的相互作用所需的热力学和动力学常数。实验在填充冰床流管中进行，温度介于213和253 K之间，HONO气相浓度介于0.4和137 ppbv之间。实验是使用放射性标记的HO〜（13）NO分子进行的。使用短寿命同位素〜（13）N（t_（1/2）≈10分钟）可以原位监测流管中HO〜（13）NO的迁移。测量表明，相互作用不仅通过吸附发生，而且通过扩散到多晶冰中发生。建议使用一种方法来解散主体和表面过程。使用该方法，发现线性分配系数的温度依赖性为K_（lin.C.HONO）= 7.4×10〜（-11）exp（5.4×10〜3 / T），单位为m。 HONO在冰上的吸附焓和熵为ΔH_（ads，HONO）= -45（±20）kJ mol〜（-1）和ΔS〜0_（ads，HONO）= -17（±89）J mol〜对于标准条件A_（std）/ V_（std）= 1.7×10〜9 m〜（-1），分别为（-1）K〜（-1）。时间依赖性吸收到主体中的表达式为H * _（cc，HONO）（D_（b，HONO））〜（1/2），即无量纲有效亨利定律常数与有效扩散的平方根的乘积在多晶冰基质的主体中保持恒定。 H * _（cc，HONO）（D_（b，HONO））〜（-1/2）评估为1.6（±69％）×10〜（-2）m s〜（-1/2）。在雪堆中的HONO分区中讨论了结果。

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