1. 大气非均相反应中复合效应的研究进展

1.1. 首次发现了共存的NOx可以极大地促进SO₂和亚硫酸盐向硫酸盐的转化，揭示了NO₂和矿质氧化物共同催化活化分子氧，并促进硫酸盐的形成(JPCA, 2008, 112, 6630; PCCP, 2012, 14(5), 1668; PCCP, 2013, 15, 19196);

1.2. 进一步证实了SO₂可以极大促进NO₂在MgO表面转化为HONO，该过程可能是大气中HONO的潜在来源(EST, 2017, 51, 3767);

1.3. 系统研究了SO₂和NH₃在矿质氧化物表面非均相反应过程中的相互促进作用机制，揭示了这一过程是大气中硫酸盐和铵盐形成的重要途径(PCCP, 2016, 18 (2), 956; JPCA 2018, 122 (30), 6311; ESNano, 2019, 6, 2749 (HOT Article)；AE, 2019, 208: 133);

1.4. 液相反应中共存NH₃促进SO₂溶解，离子强度改变NO₂氧化SO₂的速率常数，进而加速硫酸盐形成（EP, 2019, 252, 236);

1.5. 北京地区冬季强霾期间的监测数据分析结果表明，成霾期间共存矿质颗粒物和高浓度NOx是促进SO₂转化为硫酸盐的关键因素。复合污染条件下，SO₂的环境容量下降，导致硫酸盐快速增长致霾(SR, 2014(4): 04172；EP, 2018, 233, 662)。

2. 颗粒物吸湿性及吸湿过程中的复合效应研究进展

2.1. 建立了基于压力平衡法的水蒸气吸附仪(JPCA, 2010, 114, 4232)和吸湿性差分电迁移率分析仪HTDMA(ACS Earth and Space Chemistry, 2019, 3(7), 1216)，结合原位红外光谱和拉曼光谱等手段，研究了非均相反应对颗粒物吸湿性的促进作用及其机制(PCCP, 2012, 14 (23), 8403; JES, 2010, 22 (4), 555; 2012, 24(1), 62);

2.2. 揭示了多相过程中的复合效应改变大气中硫酸盐的赋存形式，是大气中二次石膏形成的关键机制(PCCP, 2013, 15, 19196);

2.3. 发现了有机-无机混合颗粒物吸湿过程中存在液相反应，阐明了弱酸置换强酸的内在机制 (EST, 2013, 47(18), 10381; AE, 2012, 50, 97; 2013, 69, 281; 2019, 200, 34)。

3. 黑碳表面的非均相过程研究进展

3.1. 在不同燃氧比条件下制备了甲苯、正己烷和癸烷燃烧的黑碳样品。基于组成和吸湿性表征，发现正己烷和癸烷黑碳的亲水性随燃氧比减小而增大，平均粒径 和有机碳含量随燃氧比减小而降低，黑碳的聚集形态不受燃氧比影响。基于红外 光谱和拉曼光谱的分析，发现亲水性官能团主要位于黑碳结构中的石墨层边缘和 表面石墨层。(JPCA, 2012, 116, 4129)

3.2. 利用原位拉曼光谱研究 O3 与黑碳的非均相反应，发现O3老化导致黑碳微晶有序度降低，无序碳和无定型碳为臭氧化反应活性位点。 O3老化使得黒碳表面含氧官能团含量升高，光照可以进一步增强O3对黒碳的老化。(PCCP, 2010, 12, 10896; JPC, 2012, 137, 084507; PCCP, 2016, 18, 24401)

3.3. 发现 NO2 摄取系数和 HONO 产率随燃氧比减小而减小，有机碳(OC) 是 NO2 老化过程中的主要活性组分。光照可以进一步增强老化作用，并证明黒碳表面含氮物种的光解是大气中HONO的一个重要来源。(EST, 2013, 47, 3174; AE, 2013, 64, 270)

3.4. 发现可见光可激发分子 O2 与黑碳的非均相化学反应，导致黑碳表面生成各种含氧官能团，有机碳(OC)是参与老化反应的主要活性组分。(PNAS, 2012, 109, 21250)

3.5. 发现黒碳可以催化O₂氧化SO₂向硫酸盐的转化，并通过理论计算揭示了其催化反应机理。分子O₂可以在黒碳表面的醚键位点(C-O-C)常温下裂解为环氧基，环氧基进而实现对SO₂的直接氧化。 (AE, 2016, 142, 383; PCCP, 2016, 18, 31691; AE, 2017, 152, 465; ACS Catal, 2018, 8, 3825)

相关论文:

53) Biwu Chu, Yali Wang, Weiwei Yang, Jinzhu Ma, Qingxin Ma*, Peng Zhang, Yongchun Liu, Hong He, “Effects of NO₂ and C₃H₆ on the heterogeneous oxidation of SO₂ on TiO₂ in the presence or absence of UV-Vis irradiation.” Atmos. Chem. Phys., 19, (2019) 14777-14790.

52) Shuping Zhang, Jia Xing*, Golam Sarwar, Yanli Ge, Hong He, Fengkui Duan, Yan Zhao, Kebin He, Lidan Zhu, Biwu Chu*, “Parameterization of heterogeneous reaction of SO₂ to sulfate on dust with coexistence of NH₃ and NO₂ under different humidity conditions”, Atmos. Environ., 208, (2019) 133-140.

51) Qingxin Ma, Cheng Zhong, Chang Liu, Jun Liu, Jinzhu Ma, Lingyan Wu, Hong He*, “A comprehensive study about the hygroscopic behavior of mixtures of oxalic acid and nitrate salts: Implication for the occurrence of atmospheric metal oxalate complex”, ACS Earth. Space Chem., 3, (2019) 1216-1225.

50) Qingxin Ma*, Ling Wang, Biwu Chu, Jinzhu Ma, Hong He*, “Contrary role of H₂O and O₂ in the kinetics of heterogeneous photochemical reactions of SO₂ on TiO₂”, J. Phys. Chem. A., 123, (2019) 1311-1318.

49) Qingxin Ma, Chang Liu, Jinzhu Ma, Biwu Chu, Hong He*, “A laboratory study on the hygroscopic behavior of H₂C₂O₄-containing mixed particles”, Atmos. Environ., 200, (2019) 34-39.

48) Tianzeng Chen, Biwu Chu*, Yanli Ge, Shuping Zhang, Qingxin Ma, Hong He, Shao-Meng Li, “Enhancement of aqueous sulfate formation by the coexistence of NO₂/NH₃ under high ionic strengths in aerosol water”, Environ. Pollut., 252, (2019), 236-244.

47) 王铃，马庆鑫^*，贺泓，“光照对SO₂在矿质氧化物表面非均相反应的影响”，环境科学，38 (3), (2018) 1-2.

46) Weiwei Yang, Qinxin Ma*, Yongchun Liu, Jinzhu Ma, Biwu Chu, Ling Wang, Hong He, “Role of NH₃ in the heterogeneous formation of secondary inorganic aerosols on mineral oxides”, J. Phys. Chem. A, 122, (2018) 6311-6320.

45) Guangzhi He, Jinzhu Ma,Hong He^*, “Role of carbonaceous aerosols in catalyzing sulfate formation”, ACS. Catal., 8, (2018) 3825-3832.

44) Jinzhu Ma, Biwu Chu, Jun Liu, Yongchun Liu, Hongxing Zhang,Hong He^*, “NO_X promotion of SO₂ conversion to sulfate: An important mechanism for the occurrence of heavy haze during winter in Beijing”, Environ. Pollut., 233, (2018) 662-669.

43) Chang Liu, Qingxin Ma,Hong He^*, Guangzhi He, Jinzhu Ma, Yongchun Liu, Ying Wu, “Structure-activity relationship of surface hydroxyl groups during NO₂ adsorption and transformation on TiO₂ nanoparticles”, Environ. Sci. Nano., 4, (2017) 2388-2394.

42) Qingxin Ma*, Tao Wang*, Chang Liu, Hong He, Zhe Wang, Weihan Wang, Yutong Liang, “SO₂ initiates the efficient conversion of NO₂ to HONO on MgO surface”, Environ. Sci. Technol., 51, (2017) 3767-3775.

41) Weiwei Yang, Jianghao Zhang, Qingxin Ma^*, Yan Zhao, Yongchun Liu, Hong He*, “Heterogeneous reaction of SO₂ on manganese oxides: the effect of crystal structure and relative humidity”, Sci. Rep., 7, (2017) 4550.

40) Chong Han, Yongchun Liu, Hong He*, “Heterogeneous reaction of NO₂ with soot at different relative humidity”, Environ. Sci. Pollut. Res., 24, (2017) 21248-21255.

39) Yan Zhao, Yongchun Liu^*, Jinzhu Ma, Qingxin Ma, Hong He*, “Heterogeneous reaction of SO₂ with soot: the roles of relative humidity and combustion conditions in sulfuric acid formation”, Atmos. Environ., 152, (2017) 465-476.

38) Guangzhi He, Hong He*, “DFT studies on the heterogeneous oxidation of SO₂ by oxygen functional groups on grapheme”, Phys. Chem. Chem. Phys., 18, (2016) 31691-31697.

37) Yan Zhao, Qingxin Ma, Yongchun Liu, Hong He*, “Influence of sulfur in fuel on the properties of diffusion flame soot”, Atmos. Environ., 142, (2016) 383-392.

36) Chong Han, Yongchun Liu, Hong He*, “The photoenhanced aging process of soot by the heterogeneous ozonization reaction”, Phys. Chem. Chem. Phys., 18, (2016) 24401-24407.

35) Weiwei Yang , Hong He* , Qingxin Ma , Jinzhu Ma , Yongchun Liu , Pengfei Liu, Yujing Mu, “Synergistic formation of sulfate and ammonium resulting from reaction between SO₂ and NH₃ on typical mineral dust”, Phys. Chem. Chem. Phys., 18, (2016) 956-964.

34) Biwu Chu, Tengyu Liu, Xiao Zhang, Yongchun Liu, Qingxin Ma, Jinzhu Ma, Hong He*, Xinming Wang, Junhua Li, Jiming Hao, “Secondary aerosol formation and oxidation capacity in photooxidation in the presence of Al₂O₃ seed particles and SO₂”, Sci. China-Chem., 58 (9), (2015) 1426-1434.

33) 马庆鑫，马金珠，楚碧武，刘永春，赖承钺，贺泓*，“矿质和黑碳颗粒物表面大气非均相反应研究进展”, 科学通报，60(2)，(2015)122-136.

32) Yongchun Liu, Chong Han, Jinzhu Ma, Xiaolei Bao, Hong He*, “Influence of relative humidity on heterogeneous kinetics of NO₂ on kaolin and hematite”,   Phys. Chem. Chem. Phys., 17, (2015) 19424-19431.

31) Chengyue Lai, Yongchun Liu*, Jinzhu Ma, Qingxin Ma, Biwu Chu, and Hong He*, “Heterogeneous kinetics of cis-pinonic acid with hydroxyl radical under different environmental conditions”, J. Phys. Chem. A, 119, (2015) 6583-6593.

30) Chengyue Lai, Yongchun Liu*, Jinzhu Ma, Qingxin Ma, Hong He*, “Laboratory study on OH-initiated degradation kinetics of dehydroabietic acid”, Phys. Chem. Chem. Phys., 17, (2015) 10953-10962.

29) Chengyue Lai, Yongchun Liu*, Jinzhu Ma, Qingxin Ma, Hong He*, “Degradation kinetics of levoglucosan initiated by hydroxyl radical under different environmental conditions”, Atmos. Environ., 91, (2014) 32-39.

28) Biwu Chu, Kun Wang, Hideto Takekawa, Junhua Li, Wei Zhou, Jingkun Jiang, Qingxin Ma, Hong He, Jinming Hao*, “Hygroscopicity of particles generated from photooxidation of α-pinene under different oxidation conditions in the presence of sulfate seed aerosols”, J. Environ. Sci., 26, (2014) 129-139.

27) Hong He*, Yuesi Wang*, Qingxin Ma, Jinzhu Ma, Biwu Chu, Dongsheng Ji, Guiqian Tang, Chang Liu, Hongxing Zhang, Jiming Hao, “Mineral dust and NOx promote the conversion of SO₂ to sulfate in heavy pollution days”, Sci. Rep., 4, (2014) 04172. 

26) Qingxin Ma, Hong He*, Yongchun Liu, Chang Liu, Vicki H. Grassian, “Heterogeneous and multiphase formation pathways of gypsum in the atmosphere”, Phys. Chem. Chem. Phys., 15, (2013) 19196-19204.

25) Qingxin Ma, Jinzhu Ma, Chang Liu, Chengyue Lai, Hong He*, “Laboratory study on the hygroscopicbehavior of external and internal C₂−C₄ dicarboxylic Acid−NaCl mixtures”, Environ. Sci. Technol., 47, (2013) 10381-10388.

24) Qingxin Ma, Hong He*, Chang Liu, “Hygroscopic properties of oxalic acid and atmospherically relevant oxalates”, Atmos. Environ., 69, (2013) 281-288.

23) Chong Han, Yongchun Liu, Hong He*, “Role of Organic Carbon in     Heterogeneous Reaction of NO₂ with Soot”, Environ. Sci. Technol., 47, (2013) 3174-3181.

22) Jinzhu Ma, Yongchun Liu, Chong Han, Qingxin Ma, Chang Liu, Hong He*, “Review of heterogeneous photochemical reactions of NOy on aerosol – A possible daytime source of nitrous acid (HONO) in the atmosphere”, J. Environ. Sci., 25, (2013) 326-334.

21) Jinzhu Ma, Yongchun Liu, Qingxin Ma, Chang Liu, Hong He*，“Heterogeneous photochemical reaction of ozone with anthracene adsorbed on mineral dust”,  Atmos. Environ., 72, (2013) 165-170.

20) Chong Han, Yongchun Liu*, Hong He*, “Heterogeneous photochemical aging of soot by NO₂ under simulated sunlight”, Atmos. Environ., 64, (2013) 270-276.

19) Chong Han, Yongchun Liu*, Jinzhu Ma, Hong He*, “Key role of organic carbon in the sunlight enhanced atmospheric aging of soot by O₂”, Proc. Nat. Acad. Sci. USA., 109(52), (2012) 21250-21255.

18) Yongchun Liu, Qingxin Ma, Hong He*, “Heterogeneous Uptake of Amines by Citric Acid and Humic Acid”, Environ. Sci. Technol., 46, (2012) 11112-11118.

17) Chong Han, Yongchun Liu*, Jinzhu Ma, Hong He*, “Effect of soot microstructure on its ozonization reactivity”, J. Chem. Phys., 137, (2012) 084507.

16) Yongchun Liu, Chong Han, Chang Liu, Jinzhu Ma, Qingxin Ma, Hong He*, “Differences in the reactivity of ammonium salts with methylamine”, Atmos. Chem. Phys., 12, (2012) 4855-4865.

15) Qingxin Ma, Yongchun Liu, Chang Liu, Hong He*, “Heterogeneous reaction of acetic acid on MgO, a-Al₂O₃, and CaCO₃ and the effect on the hygroscopic behaviour of these particles”, Phys. Chem. Chem. Phys., 14, (2012) 8403-8409.  

 

14）Chong Han, Yongchun Liu*, Chang Liu, Jinzhu Ma, Hong He*, “Influence of combustion conditions on hydrophilic properties and microstructure of flame soot”, J. Phys. Chem. A, 116, (2012) 4129-4136.

13) Qingxin Ma, Yongchu Liu, Chang Liu, Jinzhu Ma, Hong He*, “A case study of Asian dust storm particles: Chemical composition, reactivity to SO₂ and hygroscopic properties”, J. Environ. Sci, 24, (2012) 62-71. 

12) Qingxin Ma, Hong He*, “Synergistic effect in the humidifying process of atmospheric relevant calcium nitrate, calcite and oxalic acid mixtures”, Atmos. Environ., 50, (2012) 97-102.

11) Chang Liu, Qingxin Ma, Yongchun Liu, Jinzhu Ma, Hong He*, “Synergistic reaction between SO₂ and NO₂ on mineral oxides: a potential formation pathway of sulfate aerosol. Phys. Chem. Chem. Phys., 14, (2012) 1668-1676.   

10) 马金珠、刘永春、马庆鑫、刘畅、贺泓*, “大气非均相反应及其环境效应”, 环境化学, 30, (2011) 97-119.

9) Jinzhu Ma, Yongchun Liu, Hong He*, “Heterogeneous reactions between NO₂ and anthracene adsorbed on SiO₂ and MgO ”, Atmos. Environ., 45, (2011) 917-924.

8) Jinzhu Ma, Yongchun Liu, Hong He*, “Degradation kinetics of anthracene by ozone on mineral oxides”, Atmos. Environ., 44, (2010) 4446-4453.    

   

7) Yongchun Liu, Chang Liu, Jinzhu Ma, Qingxin Ma, Hong He*, “Structural and hygroscopic changes of soot during heterogeneous reaction with O₃”, Phys. Chem. Chem. Phys., 12, (2010) 10896-10903.

6) Qingxin Ma, Yongchun Liu, Chang Liu, Jinzhu Ma, Hong He*, “A comprehensive characterisation of Asian dust storm particles: chemical composition, reactivity to SO₂, and hygroscopic property”, Atmos. Chem. Phys. Discuss., 10, (2010) 8899-8925.

5) Qingxin Ma, Hong He*，Yongchun Liu, “In situ DRIFTS study of hygroscopic  behavior of mineral aerosol ”, J. Environ. Sci., 22, (2010) 555-560.

4)Qingxin Ma, Yongchun Liu, Hong He*, “The utilization of physisorption analyzer for studying the hygroscopic properties of atmospheric relevant particles”, J. Phys. Chem. A, 114, (2010) 4232-4237.

3) Yongchun Liu, Qingxin Ma, Hong He*, “Comparative study of the effect of water on the heterogeneous reactions of carbonyl sulfide on the surface of α-Al₂O₃ and MgO” , Atmos. Chem. Phys., 9, (2009) 6273-6286.

2) 贺泓*, 刘永春，曲久辉, “环境微界面过程的原位和在线研究方法”, 环境科学学报,29, (2009) 11-20.

1) Qingxin Ma, Yingchun Liu, Hong He*, “Synergistic effect between NO₂ and SO₂ in their adsorption and reaction on γ-Alumina”, J. Phys. Chem. A, 112, (2008) 6630-6635.

1. 主要实验设施

1.1. 30m³室内烟雾箱系统

烟雾箱系统作为研究和评价光化学反应机理的有效手段，对认识和解决局地、区域和全球尺度的大气污染问题发挥着重要作用。中国科学院生态环境研究中心(RCEES-CAS)30m³室内烟雾箱采用“箱中箱”的设计思路，主要由零空气发生系统、特氟龙膜反应器、光源系统、温度控制系统、进样与控制系统和检测系统构成。反应器设计为3.0m×2.5m×4.0m的长方体，比表面积为1.97m^-1，由125μm厚的Teflon膜焊接缝合而成。采用120盏365nm的紫外灯作为主要光源，最大NO₂光解速率为0.55min^-1，主要用于研究复合污染条件下O₃和二次气溶胶的生成机制。

1.2. 氧化流动管实验观测系统

颗粒物生成潜势反应器（PAM）由Kang首次提出并应用，原理是通过光解进入反应器的臭氧，然后在反应器腔内产生比实际大气高几百倍甚至几千倍的OH·浓度，故而能在非常短的停留时间（几十秒到几分钟）模拟相当于在实际大气环境下几天甚至几周的VOCs氧化过程。研究组设计搭建了由两个体积均为15 L的不锈钢圆筒组成的孪生氧化流动管反应器（OFR），主要用来研究SOA的生成和老化过程以及实际环境大气SOA生成潜势的变化趋势与影响因素(JES, 2016, 39, 52-61)。

2. 复合污染条件对SOA生成的影响

2.1. 矿质颗粒物种子对SOA生成的影响

对矿质颗粒物影响光化学反应SOA生成的研究表明， Al₂O₃种子SOA产率影响不明显，但显著影响SOA粒径分布。高浓度Al₂O₃种子有可能使颗粒物粒数浓度明显增大，而粒径明显减小，进而增大颗粒物的大气寿命，加剧其人体健康风险，并改变其消光特性(AE, 2013, 77: 781, Sci. China-Earth Sci., 2015, 58(2), 245)。复合污染条件下，矿质颗粒物表面污染物之间的协同效应可能通过改变大气氧化能力进而改变二次颗粒物生成对前体物的敏感性，例如Al₂O₃种子存在条件下，高NOx条件下SOA的生成可能高于低NOx条件(Sci. China-Chem., 2015, 58(9), 1426)。

2.2. 金属离子影响SOA气溶胶相老化过程

发现含铁硫酸盐存在条件下，其表面液相中的铁离子与过氧化物种发生类似Fenton反应，在气溶胶相产生活性氧物种，导致部分SOA组分的挥发性升高，重新分配到气相，从而减少SOA产量，并使得SOA的氧化程度升高 (AE, 2012, 55, 26, EP, 2014, 193: 88)。这两种效应的相对重要性和不同体系生成的SOA本身的化学特性密切相关(SR, 2017, 7: 40311)。这些研究结果有助于解释实验室模拟中SOA氧化程度普遍低于外场观测数据的现象。同时发现无机气溶胶种子还会影响反应生成的SOA的吸湿性，进而影响其致霾能力(JES, 2014, 26 (1): 129)。

2.3. 共存无机气体对SOA生成的影响

课题组开展了大气二次颗粒物生成中无机和有机致霾前体物的复合效应研究。发现二氧化硫和氨气等无机污染气体对二次无机颗粒物和二次有机气溶胶（SOA）生成均有重要贡献，贫氨条件下，SO₂主要通过生成酸性气溶胶进而通过酸催化作用促进低聚物的形成提高SOA产率，而富氨条件下，SO₂和NH₃可显著增加SOA中含氮有机物和有机硫酸脂的生成，同时促进小分子高级氧化产物的摄取，进而导致SOA氧化态的增加。针对单一VOCs组分(如单环芳烃类)、特征排放源（如机动车蒸发排放源）以及含氧VOCs (如生物质标记物甲氧基苯酚类和烯醚烯酯等中间态含氧VOCs)的研究中都发现了SO₂和NH₃对SOA生成的协同促进作用(ACP, 2016, 16(22), 14219; ACP, 2019, 19, 8063; EST, 2019, 53 (15), 8845; ACP, 2019, 19, 2687; ACP, 2019, 19, 2001; AE, 2019, 207, 30)。复合污染条件下一些排放源对我国大气中SOA的贡献不容忽视(如机动车蒸发排放源SOA生成贡献达0.49±0.04 Tg yr^-1) (AE, 2019, 201, 101; ACP, 2019, 19, 8063)。

3. SOA生成中的氧化机制研究

3.1. 在低前体物浓度条件下，VOCs光氧化过程的中间气相产物会提前转化为高级氧化产物，SOA产率明显高于高浓度条件。这可能是目前模式研究中普遍低估SOA环境浓度的原因之一(JES, 2019, 79, 256)。

3.2. 在复合污染条件下，含氧VOCs氧化过程中有机硫酸酯的形成和小分子高级氧化产物的摄取被证明是导致SOA氧化态随SO₂浓度升高而增加的关键原因。此外，大气环境中烯烃臭氧化形成的克里奇中间体(sCI)与水和SO₂的竞争性反应也可以显著影响SOA产率及其组成(EST, 2019, 53 (15), 8845；ACP, 2019, 19, 2687)。

4. SOA外场观测研究

4.1. 利用OFR实验观测系统对城市环境空气的SOA生成潜势的研究表明，北京城市SOA生成潜势远高于其他发达国家，且随环境中的PM_2.5浓度增加而显著增加。一般情况下，北京城市大气SOA生成达到最大时对应的老化时间在3天左右；但重污染条件下，有机气溶胶难以因过度氧化而出现浓度下降，从而出现长时间地持续生成(JES, 2016, 39, 52, EST, 2018, 52 (12): 6834)。

4.2. 北京南郊夏季的外场观测结果表明，有机气溶胶（OA）是细颗粒物的主要组分，其元素日变化特征和氧化程度受光化学过程和液相化学过程共同影响，其中SOA的贡献占主导地位且随污染程度的增加而增加(Chemosphere, 2020, 247, 125918）。

相关论文:

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