The heterogeneous loss of HO_(2)radicals onto ambient aerosols plays an important role in tropospheric chemistry.However,sparse investigation of the dominating parameters controlling the HO_(2)uptake coefficients onto...The heterogeneous loss of HO_(2)radicals onto ambient aerosols plays an important role in tropospheric chemistry.However,sparse investigation of the dominating parameters controlling the HO_(2)uptake coefficients onto ambient aerosols(γHO_(2))has largely hindered the application of the measuredγHO_(2)to the global spatial prediction.Here we induced an offine method using LFP-LIF technique to measure the kinetics of HO_(2)uptake onto ambient aerosols collected in summertime and wintertime in Yokohama city,a regional urban site near Tokyo,Japan.By controlling the dominating parameters which infuenceγHO_(2),we were able to investigate the detailed HO_(2)uptake mechanism.We characterized the chemical composition of the collected ambient aerosols,including organics,inorganics,transition metals ions,etc.and modeledγHO_(2)using different mechanisms.Results show thatγHO_(2)increased with the increase in RH,and the aerosol states(“dry”or wet/aqueous)have large effects onγHO_(2).With fixed RH and aerosol chemical composition,γHO_(2)was highly dependent on pH and inversely correlated with[HO_(2)]_0.By combing the measuredγHO_(2)values with the modeled ones,we found that both the HO_(2)self-reaction and transition metal-catalyzed reactions should be accounted for to yield a single parameterization to predictγHO_(2),and different chemical compositions may have collective effects onγHO_(2).Results may serve for extending theγHO_(2)values measured at one observation site to different environmental conditions,which will help us to achieve more accurate modeling results concerning secondary pollutant formation(i.e.,ozone).展开更多
基金supported by the Key-Area Research and Development Program of Guangdong Province (No.2020B1111360003)the Japan Society for the Promotion of Science (JSPS,No.16H06305)the Natural Science Foundation of Guangdong Province (No.2020A1515110526)。
文摘The heterogeneous loss of HO_(2)radicals onto ambient aerosols plays an important role in tropospheric chemistry.However,sparse investigation of the dominating parameters controlling the HO_(2)uptake coefficients onto ambient aerosols(γHO_(2))has largely hindered the application of the measuredγHO_(2)to the global spatial prediction.Here we induced an offine method using LFP-LIF technique to measure the kinetics of HO_(2)uptake onto ambient aerosols collected in summertime and wintertime in Yokohama city,a regional urban site near Tokyo,Japan.By controlling the dominating parameters which infuenceγHO_(2),we were able to investigate the detailed HO_(2)uptake mechanism.We characterized the chemical composition of the collected ambient aerosols,including organics,inorganics,transition metals ions,etc.and modeledγHO_(2)using different mechanisms.Results show thatγHO_(2)increased with the increase in RH,and the aerosol states(“dry”or wet/aqueous)have large effects onγHO_(2).With fixed RH and aerosol chemical composition,γHO_(2)was highly dependent on pH and inversely correlated with[HO_(2)]_0.By combing the measuredγHO_(2)values with the modeled ones,we found that both the HO_(2)self-reaction and transition metal-catalyzed reactions should be accounted for to yield a single parameterization to predictγHO_(2),and different chemical compositions may have collective effects onγHO_(2).Results may serve for extending theγHO_(2)values measured at one observation site to different environmental conditions,which will help us to achieve more accurate modeling results concerning secondary pollutant formation(i.e.,ozone).
