A method for quantitative evaluating the enhancement of the rate of Type Ⅱ photosensitized oxidation by D_2O was suggested. The effect of substrate concentration on this process was also discussed.
Humic-like substances(HULIS),a class of macromolecular photosensitizers,are major components of light-absorbing aerosols in the atmosphere.Due to the amphiphilic nature of HULIS,they tend to appear at the air-water in...Humic-like substances(HULIS),a class of macromolecular photosensitizers,are major components of light-absorbing aerosols in the atmosphere.Due to the amphiphilic nature of HULIS,they tend to appear at the air-water interface of atmospheric water.However,there have been limited studies on the photosensitized chemistry of HULIS at the air-water interface owing to the lack of methods with high interface selectivity.Here,a unique field-induced droplet ionization mass spectrometry(FIDI-MS)technique was used to investigate the photosensitized chemistry of several samples at the air-water interface.These samples include commercially available humic acid and the PM_(2.5)sample collected during Beijing′s severe winter haze in December 2016.Ultrahigh-resolution Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS)was also applied to analyze the atomic compositions,the degree of unsaturation and the aromaticity of these samples.Both TypeⅠand TypeⅡphotosensitized oxidation pathways were observed,which were postulated to be dictated by the packing density of the molecules at the air-water interface.These findings reveal that the photosensitization of HULIS at the air-water interface contributes greatly to the formation of atmospheric aerosols,further advancing our understanding of the important roles played by photosensitized chemistry in the atmosphere.展开更多
文摘A method for quantitative evaluating the enhancement of the rate of Type Ⅱ photosensitized oxidation by D_2O was suggested. The effect of substrate concentration on this process was also discussed.
基金the National Natural Science Foundation of China(42221001)the National Natural Science Foundation of China(22325402,22174073)+4 种基金the National Key R&D Program of China(2023YFE0124200)the Natural Science Foundation of Tianjin City(21JCJQJC00010)the Natural Science Foundation of Tianjin City(23ZYJDSS00030)the Nankai Cangzhou Chemistry(NCC)Fund(NCC2022PY05)the Haihe Laboratory of Sustainable Chemical Transformations and the Frontiers Science Center for New Organic Matter at Nankai University(63181206)。
文摘Humic-like substances(HULIS),a class of macromolecular photosensitizers,are major components of light-absorbing aerosols in the atmosphere.Due to the amphiphilic nature of HULIS,they tend to appear at the air-water interface of atmospheric water.However,there have been limited studies on the photosensitized chemistry of HULIS at the air-water interface owing to the lack of methods with high interface selectivity.Here,a unique field-induced droplet ionization mass spectrometry(FIDI-MS)technique was used to investigate the photosensitized chemistry of several samples at the air-water interface.These samples include commercially available humic acid and the PM_(2.5)sample collected during Beijing′s severe winter haze in December 2016.Ultrahigh-resolution Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS)was also applied to analyze the atomic compositions,the degree of unsaturation and the aromaticity of these samples.Both TypeⅠand TypeⅡphotosensitized oxidation pathways were observed,which were postulated to be dictated by the packing density of the molecules at the air-water interface.These findings reveal that the photosensitization of HULIS at the air-water interface contributes greatly to the formation of atmospheric aerosols,further advancing our understanding of the important roles played by photosensitized chemistry in the atmosphere.
