Liu Qifan, Wang Yidan, Wu Lingyan, Jing Bo, Tong Shengrui, Wang Weigang, Ge Maofa
Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
J Environ Sci (China). 2017 Mar;53:107-112. doi: 10.1016/j.jes.2016.03.027. Epub 2016 Jun 7.
In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust (ATD) has been investigated within a temperature range of 255-315K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient (γ) of acrylic acid on ATD decreases from (4.02±0.12)×10 to (1.73±0.05)×10 with a temperature increase from 255 to 315K. According to the temperature dependence of uptake coefficients, the enthalpy (ΔH) and entropy (ΔS) of uptake processes were determined to be -(9.60±0.38) KJ/mol and -(121.55±1.33) J·K/mol, respectively. The activation energy for desorption (E) was calculated to be (14.57±0.60) KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.
在本研究中,使用克努森池反应器在255 - 315K的温度范围内研究了丙烯酸在亚利桑那测试粉尘(ATD)上的非均相摄取的温度依赖性。结合漫反射红外傅里叶变换光谱(DRIFTS)实验,发现丙烯酸可通过表面羟基吸附在ATD上,并在颗粒表面转化为羧酸盐。动力学研究表明,随着温度从255K升高到315K,丙烯酸在ATD上的初始真实摄取系数(γ)从(4.02±0.12)×10降至(1.73±0.05)×10。根据摄取系数的温度依赖性,摄取过程的焓(ΔH)和熵(ΔS)分别确定为-(9.60±0.38) kJ/mol和-(121.55±1.33) J·K/mol。解吸活化能(E)计算为(14.57±0.60) kJ/mol。这些结果表明,丙烯酸在ATD表面的非均相摄取对温度敏感。在ATD上的非均相摄取会影响大气中丙烯酸的浓度,尤其是在低温下。