Variation in chemical composition and sources of PM2.5 during the COVID-19 lockdown in Delhi.

The Government of India (GOI) announced a nationwide lockdown starting 25th March 2020 to contain the spread of COVID-19, leading to an unprecedented decline in anthropogenic activities and, in turn, improvements in ambient air quality. This is the first study to focus on highly time-resolved chemical speciation and source apportionment of PM2.5 to assess the impact of the lockdown and subsequent relaxations on the sources of ambient PM2.5 in Delhi, India. The elemental, organic, and black carbon fractions of PM2.5 were measured at the IIT Delhi campus from February 2020 to May 2020. We report source apportionment results using positive matrix factorization (PMF) of organic and elemental fractions of PM2.5 during the different phases of the lockdown. The resolved sources such as vehicular emissions, domestic coal combustion, and semi-volatile oxygenated organic aerosol (SVOOA) were found to decrease by 96%, 95%, and 86%, respectively, during lockdown phase-1 as compared to pre-lockdown. An unforeseen rise in O3 concentrations with declining NOx levels was observed, similar to other parts of the globe, leading to the low-volatility oxygenated organic aerosols (LVOOA) increasing to almost double the pre-lockdown concentrations during the last phase of the lockdown. The effect of the lockdown was found to be less pronounced on other resolved sources like secondary chloride, power plants, dust-related, hydrocarbon-like organic aerosols (HOA), and biomass burning related emissions, which were also swayed by the changing meteorological conditions during the four lockdown phases. The results presented in this study provide a basis for future emission control strategies, quantifying the extent to which constraining certain anthropogenic activities can ameliorate the ambient air. These results have direct relevance to not only Delhi but the entire Indo-Gangetic plain (IGP), citing similar geographical and meteorological conditions common to the region along with overlapping regional emission sources. SUMMARY OF MAIN FINDINGS: We identify sources like vehicular emissions, domestic coal combustion, and semi-volatile oxygenated organic aerosol (SVOOA) to be severely impacted by the lockdown, whereas ozone levels and, in turn, low-volatility oxygenated organic aerosols (LVOOA) rise by more than 95% compared to the pre-lockdown concentrations during the last phase of the lockdown. However, other sources resolved in this study, like secondary chloride, power plants, dust-related, hydrocarbon-like organic aerosols (HOA), and biomass burning related emissions, were mainly driven by the changes in the meteorological conditions rather than the lockdown.

[1]  M. Molina,et al.  Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected , 2006 .

[2]  D. R. Worsnop,et al.  Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols , 2005 .

[3]  K. Badarinath,et al.  Variations in CO, O3 and black carbon aerosol mass concentrations associated with planetary boundary layer (PBL) over tropical urban environment in India , 2009 .

[4]  R. Gehrig,et al.  Chemical composition of PM10 in Switzerland: An analysis for 2008/2009 and changes since 1998/1999 , 2012 .

[5]  Pierre Tulet,et al.  Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City , 2009 .

[6]  A. Tobías,et al.  Changes in air quality during the lockdown in Barcelona (Spain) one month into the SARS-CoV-2 epidemic , 2020, Science of The Total Environment.

[7]  S. Tripathi,et al.  Realtime chemical characterization of post monsoon organic aerosols in a polluted urban city: Sources, composition, and comparison with other seasons. , 2018, Environmental pollution.

[8]  Jaiprakash,et al.  Chemical characterization of PM1.0 aerosol in Delhi and source apportionment using positive matrix factorization , 2016, Environmental Science and Pollution Research.

[9]  A. Weinheimer,et al.  Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO , 2010 .

[10]  Edward Charles Fortner,et al.  Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry , 2009 .

[11]  K. Prather,et al.  Comparison of oil and fuel particle chemical signatures with particle emissions from heavy and light duty vehicles , 2006 .

[12]  B. Finlayson‐Pitts,et al.  Atmospheric Chemistry of Tropospheric Ozone Formation: Scientific and Regulatory Implications , 1993 .

[13]  P. Parekh,et al.  The use of chemical and statistical methods to identify sources of selected elements in ambient air aerosols in Karachi, Pakistan , 1967 .

[14]  A. Gautam,et al.  21-Day Lockdown in India Dramatically Reduced Air Pollution Indices in Lucknow and New Delhi, India , 2020, Bulletin of Environmental Contamination and Toxicology.

[15]  D. R. Worsnop,et al.  Evolution of Organic Aerosols in the Atmosphere , 2009, Science.

[16]  Michelle Gamber,et al.  Does Wuhan Need to be in Lockdown during the Chinese Lunar New Year? , 2020, International journal of environmental research and public health.

[17]  Bhola R. Gurjar,et al.  Traffic induced emission estimates and trends (2000–2005) in megacity Delhi , 2013 .

[18]  F. Cassee,et al.  Inhalation toxicity profiles of particulate matter: a comparison between brake wear with other sources of emission , 2019, Inhalation toxicology.

[19]  P. Paatero Least squares formulation of robust non-negative factor analysis , 1997 .

[20]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics Changes in Organic Aerosol Composition with Aging Inferred from Aerosol Mass Spectra , 2022 .

[21]  J. Peñuelas,et al.  Biomass burning contributions to urban aerosols in a coastal Mediterranean city. , 2012, The Science of the total environment.

[22]  A. P. Dimri,et al.  PM2.5 diminution and haze events over Delhi during the COVID-19 lockdown period: an interplay between the baseline pollution and meteorology , 2020, Scientific Reports.

[23]  Krag A. Petterson,et al.  Field and laboratory evaluation of a high time resolution x-ray fluorescence instrument for determining the elemental composition of ambient aerosols , 2017, Atmospheric Measurement Techniques.

[24]  M. C. Ooi,et al.  Air quality changes during the COVID-19 lockdown over the Yangtze River Delta Region: An insight into the impact of human activity pattern changes on air pollution variation , 2020, Science of The Total Environment.

[25]  Jing-chun Duan,et al.  Atmospheric heavy metals and Arsenic in China: Situation, sources and control policies , 2013 .

[26]  A. Piazzalunga,et al.  High secondary aerosol contribution to particulate pollution during haze events in China , 2014, Nature.

[27]  Jiří Novák,et al.  Source apportionment with uncertainty estimates of fine particulate matter in Ostrava, Czech Republic using Positive Matrix Factorization , 2016 .

[28]  F. E. Mark,et al.  Bromine in waste incineration: partitioning and influence on metal volatilisation. , 2003, Environmental science and pollution research international.

[29]  Vyoma Singla,et al.  Role of organic aerosols in CCN activation and closure over a rural background site in Western Ghats, India , 2017 .

[30]  B. Efron Bootstrap Methods: Another Look at the Jackknife , 1979 .

[31]  B. S. Negi,et al.  Aerosol composition and sources in Urban areas in India , 1967 .

[32]  Juan C. Zavala-Reyes,et al.  Temporary reduction in fine particulate matter due to ‘anthropogenic emissions switch-off’ during COVID-19 lockdown in Indian cities , 2020, Sustainable Cities and Society.

[33]  K. Lehtinen,et al.  Atmospheric submicron aerosol composition and particulate organic nitrate formation in a boreal forestland–urban mixed region , 2014 .

[34]  S. Tripathi,et al.  Real-time measurement and source apportionment of elements in Delhi's atmosphere. , 2020, The Science of the total environment.

[35]  A. Zhang,et al.  Does lockdown reduce air pollution? Evidence from 44 cities in northern China , 2020, Science of The Total Environment.

[36]  Z. H. Khan,et al.  Characterization and source identification of polycyclic aromatic hydrocarbons (PAHs) in the urban environment of Delhi. , 2007, Chemosphere.

[37]  P. Leighton,et al.  Photochemistry of Air Pollution , 1961 .

[38]  Y. Duan,et al.  Study on emission of hazardous trace elements in a 350 MW coal-fired power plant. Part 2. arsenic, chromium, barium, manganese, lead. , 2017, Environmental pollution.

[39]  G. Martini,et al.  Brake wear particle emissions: a review , 2014, Environmental Science and Pollution Research.

[40]  Esko I. Kauppinen,et al.  Aerosol characterisation in medium-speed diesel engines operating with heavy fuel oils , 1999 .

[41]  J. Collett,et al.  Wintertime Residential Biomass Burning in Las Vegas, Nevada; Marker Components and Apportionment Methods , 2016 .

[42]  W. E. Wilson,et al.  A study of sulfur dioxide in photochemical smog. II. Effect of sulfur dioxide on oxidant formation in photochemical smog. , 1972, Journal of the Air Pollution Control Association.

[43]  P. Paatero,et al.  Atmospheric aerosol over Alaska: 2. Elemental composition and sources , 1998 .

[44]  D. Ceburnis,et al.  Characterization of Primary Organic Aerosol from Domestic Wood, Peat, and Coal Burning in Ireland. , 2017, Environmental science & technology.

[45]  A Chandra,et al.  Impact of indian and imported coal on Indian thermal power plants , 2004 .

[46]  Renjian Zhang,et al.  Chemical source profiles of urban fugitive dust PM2.5 samples from 21 cities across China. , 2019, The Science of the total environment.

[47]  Qi Zhang,et al.  An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol , 2011 .

[48]  G. Beig,et al.  COVID-19 lockdown and air quality of SAFAR-India metro cities , 2020, Urban Climate.

[49]  Saraswati,et al.  Source Apportionment of PM2.5 in Delhi, India Using PMF Model , 2016, Bulletin of Environmental Contamination and Toxicology.

[50]  T. Zhao,et al.  Significant changes in the chemical compositions and sources of PM2.5 in Wuhan since the city lockdown as COVID-19 , 2020, Science of The Total Environment.

[51]  Puja Khare,et al.  Elemental characterization and source identification of PM2.5 using multivariate analysis at the suburban site of North-East India , 2010 .

[52]  R. Agha,et al.  World Health Organization declares global emergency: A review of the 2019 novel coronavirus (COVID-19) , 2020, International Journal of Surgery.

[53]  G. Gordon,et al.  Emissions of trace elements from coal fired power plants , 1974 .

[54]  Amit Kumar Srivastava,et al.  Spatial variability of concentrations of gaseous pollutants across the National Capital Region of Delhi, India , 2016 .

[55]  Rakesh Kumar,et al.  Source Apportionment of PM10 by Positive Matrix Factorization in Urban Area of Mumbai, India , 2012, TheScientificWorldJournal.

[56]  Roy M Harrison,et al.  Sources and properties of non-exhaust particulate matter from road traffic: a review. , 2008, The Science of the total environment.

[57]  S. Palanivelraja,et al.  Influence of Temperature, Relative Humidity and Seasonal Variability on Ambient Air Quality in a Coastal Urban Area , 2013 .

[58]  P. Paatero,et al.  Methods for estimating uncertainty in PMF solutions: examples with ambient air and water quality data and guidance on reporting PMF results. , 2015, The Science of the total environment.

[59]  P. Paatero The Multilinear Engine—A Table-Driven, Least Squares Program for Solving Multilinear Problems, Including the n-Way Parallel Factor Analysis Model , 1999 .

[60]  Qi Zhang,et al.  Primary and secondary aerosols in Beijing in winter: sources, variations andprocesses , 2016 .

[61]  Shao-Meng Li,et al.  A new source of oxygenated organic aerosol and oligomers , 2012 .

[62]  R. Prakash,et al.  Profile of selenium in soil and crops in seleniferous area of Punjab, India by neutron activation analysis , 2009 .

[63]  Michael J. Burr,et al.  Source apportionment of fine particulate matter over the Eastern U.S. Part I: source sensitivity simulations using CMAQ with the Brute Force method , 2011 .

[64]  S. Tiwari,et al.  Investigation into relationships among NO, NO2, NOx, O3, and CO at an urban background site in Delhi, India , 2015 .

[65]  C. Buisson,et al.  Near-highway aerosol and gas-phase measurements in a high-diesel environment , 2015 .

[66]  Qi Zhang,et al.  A case study of urban particle acidity and its influence on secondary organic aerosol. , 2007, Environmental science & technology.

[67]  A. Prévôt,et al.  Improved source apportionment of organic aerosols in complex urban air pollution using the multilinear engine (ME-2) , 2017 .

[68]  H. V. Joshi,et al.  Evaluation of the emission characteristics of trace metals from coal and fuel oil fired power plants and their fate during combustion. , 2005, Journal of hazardous materials.

[69]  R. Gautam,et al.  Connecting Crop Productivity, Residue Fires, and Air Quality over Northern India , 2019, Scientific Reports.

[70]  D. Worsnop,et al.  Submicron aerosol source apportionment of wintertime pollution in Paris, France by double positive matrix factorization (PMF 2 ) using an aerosol chemical speciation monitor (ACSM) and a multi-wavelength Aethalometer , 2014 .

[71]  J. Jimenez,et al.  Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data , 2008 .

[72]  J. J. Rodriguez,et al.  Amplified ozone pollution in cities during the COVID-19 lockdown , 2020, Science of The Total Environment.

[73]  J. Apte,et al.  Sources and atmospheric dynamics of organic aerosol in New Delhi, India: insights from receptor modeling , 2019, Atmospheric Chemistry and Physics.

[74]  P. Roy,et al.  SARS-CoV-2 pandemic lockdown: Effects on air quality in the industrialized Gujarat state of India , 2020, Science of The Total Environment.

[75]  I. Obernberger,et al.  Chemical properties of solid biofuels¿significance and impact , 2006 .

[76]  S. Tripathi,et al.  Variations in Black Carbon concentration and sources during COVID-19 lockdown in Delhi , 2020, Chemosphere.

[77]  Sönke Szidat,et al.  Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter. , 2008, Environmental science & technology.

[78]  Roy M. Harrison,et al.  Critical review of receptor modelling for particulate matter: A case study of India , 2012 .

[79]  A K Gupta,et al.  Chemical mass balance source apportionment of PM10 and TSP in residential and industrial sites of an urban region of Kolkata, India. , 2007, Journal of hazardous materials.

[80]  X. Tie,et al.  Water-soluble ions in atmospheric aerosols measured in Xi'an, China: Seasonal variations and sources , 2011 .

[81]  Mike Sutton,et al.  Investigations on the effect of chlorine in lubricating oil and the presence of a diesel oxidation catalyst on PCDD/F releases from an internal combustion engine. , 2007, Chemosphere.

[82]  P. Buseck,et al.  Individual aerosol particles from biomass burning in southern Africa: 2, Compositions and aging of inorganic particles , 2003 .

[83]  Swades Pal,et al.  Effect of lockdown amid COVID-19 pandemic on air quality of the megacity Delhi, India , 2020, Science of The Total Environment.

[84]  P. D. Hien,et al.  Comparative receptor modelling study of TSP, PM2 and PM2−10 in Ho Chi Minh City , 2001 .

[85]  Durga Toshniwal,et al.  Impact of lockdown measures during COVID-19 on air quality– A case study of India , 2020, International journal of environmental health research.

[86]  P. Paatero,et al.  Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values† , 1994 .

[87]  Sangi Lee,et al.  Source apportionment of PM2.5: Comparing PMF and CMB results for four ambient monitoring sites in the southeastern United States , 2008 .

[88]  Krag A. Petterson,et al.  Source apportionment of highly time-resolved elements during a firework episode from a rural freeway site in Switzerland , 2020, Atmospheric Chemistry and Physics.

[89]  J. Seinfeld Air pollution: A half century of progress , 2004 .

[90]  J. Fung,et al.  Characterization of Aerosol Aging Potentials at Suburban Sites in Northern and Southern China Utilizing a Potential Aerosol Mass (Go:PAM) Reactor and an Aerosol Mass Spectrometer , 2019, Journal of Geophysical Research: Atmospheres.

[91]  J. Jimenez,et al.  A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data , 2004 .

[92]  S. Ohta,et al.  A chemical characterization of atmospheric aerosol in Sapporo , 1990 .

[93]  Maria Ascensão Trancoso,et al.  Source apportionment of atmospheric urban aerosol based on weekdays/weekend variability: evaluation of road re-suspended dust contribution , 2006 .

[94]  C. Belis,et al.  ACTRIS ACSM intercomparison - Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments , 2015 .

[95]  G. Pandit,et al.  Chemical Characterization and Source Identification of Particulate Matter at an Urban Site of Navi Mumbai, India , 2011 .

[96]  W. Malm,et al.  Chemical Smoke Marker Emissions During Flaming and Smoldering Phases of Laboratory Open Burning of Wildland Fuels , 2010 .

[97]  J. Jimenez,et al.  Evaluation of Composition-Dependent Collection Efficiencies for the Aerodyne Aerosol Mass Spectrometer using Field Data , 2012 .

[98]  V. Shridhar,et al.  Metallic species in ambient particulate matter at rural and urban location of Delhi. , 2010, Journal of hazardous materials.

[99]  Janae Csavina,et al.  Effect of wind speed and relative humidity on atmospheric dust concentrations in semi-arid climates. , 2014, The Science of the total environment.

[100]  J. Apte,et al.  Submicron aerosol composition in the world's most polluted megacity: the Delhi Aerosol Supersite study , 2019, Atmospheric Chemistry and Physics.

[101]  Donald F. Gatz,et al.  Toxic trace elements in urban air in Illinois , 1990 .

[102]  Qi Zhang,et al.  Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry. , 2005, Environmental science & technology.

[103]  L. Skare,et al.  Formal recycling of e-waste leads to increased exposure to toxic metals: an occupational exposure study from Sweden. , 2014, Environment international.

[104]  J. Warner,et al.  Increased atmospheric ammonia over the world's major agricultural areas detected from space , 2017, Geophysical research letters.

[105]  Michael Hannigan,et al.  Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations. , 2009, Environmental science & technology.

[106]  G. Mills,et al.  Tropospheric ozone and its precursors from the urban to the global scale from air quality to short-lived climate forcer , 2014 .

[107]  I. S. Goldstein,et al.  Organic Chemicals From Biomass , 1981 .