温度对NO_(2)参与非均相反应生成硫酸盐颗粒物的影响研究  

Effect of temperature on the participation of NO_(2)in heterogeneous reaction to form sulfate particulate matter

作　　者：杨子墨 何翔[1,2,3] 王双喜 杨超群 陈星雨 YANG Zimo;HE Xiang;WANG Shuangxi;YANG Chaoqun;CHEN Xingyu(College of Ecology and Environment,Xinjiang University,Urumqi 830017;Key Laboratory of Oasis Ecology,Urumqi 830017;Xinjiang Jinghe Observation and Research Station of Temperate Desert Ecosystem,Ministry of Education,Urumqi 830017)

机构地区：[1]新疆大学生态与环境学院,乌鲁木齐830017 [2]绿洲生态教育部重点实验室,乌鲁木齐830017 [3]新疆精河温带荒漠生态系统教育部野外科学观测研究站,乌鲁木齐830017

出　　处：《环境科学学报》2025年第1期461-469,共9页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.22366035);新疆维吾尔自治区自然科学基金(No.2022D01C387);大学生创新训练计划资助项目(No.202310755079)。

摘　　要：采用原位漫反射傅里叶变换光谱技术研究了SO_(2)/NO_(2)在α-Fe_(2)O_(3)颗粒物表面的非均相反应,探究了温度对NO_(2)参与非均相反应生成硫酸盐颗粒物的影响.结果表明,硫酸盐(1259、1159、1069 cm^(-1))和硝酸盐(1603、1414、1335 cm^(-1))的特征峰在颗粒物表面生成.NO_(2)促进了吸附态SO_(2)生成硫酸盐,而N_(2)O_(4)是生成硫酸盐的关键氧化剂.随着温度由253 K增加到298 K,SO_(2)/NO_(2)在α-Fe_(2)O_(3)颗粒物表面的反应速率降低了65%左右,同时反应初始阶段的摄取系数由(4.88±0.07)×10^(-7)降低到(3.42±0.04)×10^(-7).表明温度的变化对SO_(2)/NO_(2)在α-Fe_(2)O_(3)颗粒物表面的非均相反应具有显著影响,并且在低温条件下,α-Fe_(2)O_(3)颗粒物对反应初始阶段SO_(2)具有更大的摄取能力,有助于解释冬季硫酸盐颗粒物的爆发性增长的现象.Heterogeneous reactions of SO_(2)/NO_(2)on the surface ofα-Fe_(2)O_(3)particles were investigated by in situ diffuse reflection Fourier transform spectroscopy.The influence of temperature on the formation of sulfate particles by NO_(2)participating in heterogeneous reactions was investigated.The results showed that characteristic peaks of sulfate(1259,1159,1069 cm^(-1))and nitrate(1603,1414,1335 cm^(-1))were formed on the surface of the particles.NO_(2)promoted the formation of sulfate from adsorbed SO_(2),while surface N_(2)O_(4)was the key oxidant for sulfate formation.As the temperature increased from 253 K to 298 K,the reaction rate of heterogeneous reaction decreased by about 65%,and the initial uptake coefficient decreased from(4.88±0.07)×10^(-7)to(3.42±0.04)×10^(-7).The results showed that the temperature change exhibited a significant effect on the heterogeneous reaction of SO_(2)/NO_(2)on the surface ofα-Fe_(2)O_(3)particles,α-Fe_(2)O_(3)particles exhibited a greater uptake of SO_(2)at the initial stage of the reaction and at low temperature,which helped to explain the explosive growth of sulfate particles in winter.

关 键 词：非均相反应 温度 NO_(2) α-Fe_(2)O_(3)颗粒物 硫酸盐 

分 类 号：X513[环境科学与工程—环境工程]