Machine learning and theoretical analysis release the non-linear relationship among ozone,secondary organic aerosol and volatile organic compounds

Fine particulate matter(PM_(2.5))and ozone(O_(3))pollutions are prevalent air quality issues in China.Volatile organic compounds(VOCs)have significant impact on the formation of O_(3)and secondary organic aerosols(SOA)contributing PM_(2.5).Herein,we investigated 54 VOCs,O_(3)and SOA in Tianjin from June 2017 to May 2019 to explore the non-linear relationship among O_(3),SOA and VOCs.The monthly patterns of VOCs and SOA concentrations were characterized by peak values during October to March and reached a minimum from April to September,but the observed O_(3)was exactly the opposite.Machine learning methods resolved the importance of individual VOCs on O_(3)and SOA that alkenes(mainly ethylene,propylene,and isoprene)have the highest importance to O_(3)formation;alkanes(C_(n),n≥6)and aromatics were the main source of SOA formation.Machine learning methods revealed and emphasized the importance of photochemical consumptions of VOCs to O_(3)and SOA formation.Ozone formation potential(OFP)and secondary organic aerosol formation potential(SOAFP)calculated by consumed VOCs quantitatively indicated that more than 80%of the consumed VOCs were alkenes which dominated the O_(3)formation,and the importance of consumed aromatics and alkenes to SOAFP were 40.84%and 56.65%,respectively.Therein,isoprene contributed the most to OFP at 41.45%regardless of the season,while aromatics(58.27%)contributed the most to SOAFP in winter.Collectively,our findings can provide scientific evidence on policymaking for VOCs controls on seasonal scales to achieve effective reduction in both SOA and O_(3).

Mixing states and secondary formation processes of organic nitrogen-containing single particles in Guangzhou,China

Organic nitrogen(ON)compounds play a significant role in the light absorption of brown carbon and the formation of organic aerosols,however,the mixing state,secondary formation processes,and influencing factors of ON compounds are still unclear.This paper reports on the mixing state of ON-containing particles based on measurements obtained using a highperformance single particle aerosol mass spectrometer in January 2020 in Guangzhou.The ON-containing particles accounted for 21% of the total detected single particles,and the particle count and number fraction of the ON-containing particles were two times higher at night than during the day.The prominent increase in the content of ON-containing particles with the enhancement of NO_xmainly occurred at night,and accompanied by high relative humidity and nitrate,which were associated with heterogeneous reactions between organics and gaseous NO_(x)and/or NO_(3)radical.The synchronous decreases in ON-containing particles and the mass absorption coefficient of water-soluble extracts at 365 nm in the afternoon may be associated with photo-bleaching of the ON species in the particles.In addition,the positive matrix factorization analysis found five factors dominated the formation processes of ON particles,and the nitrate factor(33%)mainly contributed to the production of ON particles at night.The results of this study provide unique insights into the mixing states and secondary formation processes of the ON-containing particles.

Detection of polycyclic aromatic hydrocarbons using a high performance-single particle aerosol mass spectrometer

The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and nitro-PAHs;yet there is still few effective technology to achieve this type of detection.In this study,11 types of PAH and nitro-PAH standard sampleswere analyzed using a high performance-single particle aerosolmass spectrometer(HP-SPAMS)in lab studies.The identification principles‘parent ions’and‘mass-to-charge(m/z)=77’of each compound were obtained in this study.It was found that different laser energies did not affect the identification of the parent ions.The comparative experiments of ambient atmospheric particles,cooking and biomass burning emitted particles with and without the addition of PAHs were conducted and ruled out the interferences from primary and secondary organics on the identification of PAHs.Besides,the reliability of the characteristic ions extraction method was evaluated through the comparative study of similarity algorithm and deep learning algorithm.In addition,the real PAH-containing particles from vehicle exhaust emissions and ambient particles were also analyzed.This study improves the ability of single particle mass spectrometry technology to detect PAHs and nitro-PAHs,and HP-SPAMS was superior to SPAMS for detecting single particles containing PAHs and nitro-PAHs.This study provides support for subsequent ambient observations to identify the characteristic spectrum of single particles containing PAHs and nitro-PAHs.

Stepless shape morphing polymer

To change the situation of shape memory polymers(SMPs)that can only remember very few shapes and enable discretional morphing for practical application,the authors report a reversible stepless multiple SMP derived from ultrahigh molecular weight polyethylene(UHMWPE).As the crystals of semicrystalline polymers are assembled by those with slightly different melting temperatures,and each type of crystal can remember a single shape,the crystalline region of UHMWPE is allowed to remember plenty of temporary shapes after programming.Changing the temperature of the programmed polymer within the melting/crystallization temperature ranges would lead to releasing/recovery of the memorized temporary shapes.Accordingly,multiple shape memory effects can be easily realized without an elaborate design of material structure and training process in advance as before.The temperaturedependent adjustability of the analog capacitor and soft lens with embedded programmed UHMWPE as actuators,characterized by the continuous/random/proportional responsivity,further reveals the utilization prospects of the controllable reversible stepless discretionary morphing effect.Moreover,the maximum work density of the programmed UHMWPE is found to be 210 kJ/m_(3),which is more than 10 times of piezoelectric ceramics,so that it can serve as a proof-of-concept mechanical driver for reversibly pumping of ethanediol-droplet upon heating/cooling.

Enhanced mixing state of black carbon with nitrate in single particles during haze periods in Zhengzhou, China

Black carbon(BC)plays an important role in air quality and climate change,which is closely associated with its mixing state and chemical compositions.In this work the mixing state of BC-containing single particles was investigated to explore the evolution process of ambient BC particles using a single particle aerosol mass spectrometer(SPAMS)in March 2018 in Zhengzhou,China.The BC-containing particles accounted for 61.4%of total detected ambient single particles and were classified into five types including BC-nitrate(BC-N,52.3%)as the most abundant species,followed by BC-nitrate-sulfate(BC-NS,22.4%),BCOC(16.8%),BC-fresh(BC-F,4.5%)and BC-sulfate particles(BC-S,4.0%).With enhancement of the ambient nitrate concentration,the relative peak area(RPA)of nitrate in BC-N and BC–NS particles both increased,yet only the number fraction(N_(f))of BC–N particles increased while the N_(f) of BC-NS particles decreased,suggesting that the enhanced mixing state of BC with nitrate was mainly due to the increase in the ambient nitrate mass concentration.In addition,the Nfof BC-N decreased from 65.3%to 28.4%as the absorbing Angstrom exponents(AAE)of e BC increased from 0.75 to 1.45,which indicated the reduction of light absorption ability of aged BC particles with the enhanced formation of BC-N particles.The results of this work indicated a change in the mixing state of BC particles due to the dominance of nitrate in PM_(2.5),which also influenced the optical properties of aged BC particles.