Effects of high RH on α-pinene SOA phase partitioning
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1 Effets f hgh RH n α-pnene SA phase parttnng Götebrg summer shl 26/06/2008 Nenne Prsle PhD student Chemstry, CCAR, Unv. Cpenhagen, Denmark nlp@kem.ku.dk 26/06/2008 Götebrg, Nenne Prsle 1 Mtvatn Current atmspher mdels annt aunt fr bserved rgan aersl mass. Identfy mehansms that ntrbute t nreasng predted sendary rgan aersl (SA) mass. The nfluene f humdty n SA gas-partle phase parttnng s ne suh ptental effet. 26/06/2008 Götebrg, Nenne Prsle 2/28 1
2 utlne parttnng thery» why expet a humdty effet n SA phase parttnng? the experments prelmnary results» what dd we bserve?» future wrk/hallenges my ther PhD prjet» surfatant parttnng n atvatng lud drplets 26/06/2008 Götebrg, Nenne Prsle 3/28 The expermental system rg rg H 2 2 (G) 3 rgan prduts [H 2 ] (P) rg H 2!!! rgans and water parttn nt a sngle ndensed phase 2
3 SA phase parttnng referene: Prest and Dnahue (EST 2006) the effetve gas phase saturatn mass nentratn *» related t the partal pressure f a spees n slutn» the saturatn vapr pressure f the pure lqud spees, wth the prpertes the spees psesses n a gven slutn the parttnng effent ξ» rat f the mass nentratn f a spees n slutn t the ttal mass nentratn n gas phase and slutn 26/06/2008 Götebrg, Nenne Prsle 5/28 Effetve gas phase saturatn nentratn, * 0 p = p γ χ Rault s law, G p = W, P *, P RT W = χ, P W 0, G p, Pγ W = RT, P, P deal gas law mass fratn n slutn effetve gas phase saturatn mass nentratn 26/06/2008 Götebrg, Nenne Prsle 6/28 3
4 * depends n SA mpstn * depends n the partle mpstn» atvty effent» mean mlar weght * = p 0, P γ W RT mpstn hange => * hange f» atvty effent hange» mean mlar weght hange χ χ : ' *'' *' '' γ W = γ W '' ' '' ' 26/06/2008 Götebrg, Nenne Prsle 7/28 Parttnng effent, ξ A 1 = 1+ ξ * = A ξ 26/06/2008 Götebrg, Nenne Prsle 8/28 4
5 RH effet n SA phase parttnng nreasng RH => SA hygrsp grwth f water and rgans mx n slutn» nrease absrbng A» derease W avg => derease * (f pseud-deal) bth wll nrease ξ => nrease resultng A 1 ξ = 1+ * A A W,, ξ, *, ξ, A * wet shft A 26/06/2008 Götebrg, Nenne Prsle 9/28 * wet shft - depends n ntal A larger effet f * wet shft smaller A (dry) r C RG µg m -3 A ~70% RH > 80% experments 26/06/2008 Götebrg, Nenne Prsle 10/28 5
6 Expermental setup purfed ar H 2 ar heater heated nlet 2) RH ramp 5% - 85% α-pnene aetntrle RH meter purfed ar 12 m 3 Tefln reatr SMPS purfed ar 2-butanl T ntrlled AMS purfed ar dffusn drer PTRMS atmzers AS slutn 1) make SA 3 generatr 2 Expermental setup purfed ar ar heater H 2 heated nlet α-pnene aetntrle RH meter purfed ar 12 m 3 Tefln reatr SMPS purfed ar 2-butanl T ntrlled AMS purfed ar dffusn drer PTRMS atmzers AS slutn 3 generatr 2 6
7 Hygrsp grwth max RH ~85% partles take up water at RH ~65% RH ~65% DRH(pure AS) = 80% 26/06/2008 Götebrg, Nenne Prsle 13/28 Aersl mass mpstn tmeseres (AMS) Mass Cnentratn (µg m -3 ) AS α-pnene RH ramp RH~65% Water Ammnum Ntrate Sulphate rgans Chlrde ttal aersl mass - wall lss ntamnatn? lletn effeny 0 11: :00 13:00 14:00 15:00 16:00 17:00 Date and Tme 26/06/2008 Götebrg, Nenne Prsle 14/28 7
8 bserved SA mass grwth +20% -nludng ntamnatn? 26/06/2008 Götebrg, Nenne Prsle 15/28 Predted SA mass grwth referenes: Prest and Dnahue (EST 2006) Chang and Pankw (apd 2008) We bserved: A ~20% fr A ~15 µg m -3 at RH ~85% +25% Cnsstent wet shft : *(dry)/*(wet) ~1.5 ±0.5 26/06/2008 Götebrg, Nenne Prsle 16/28 8
9 bserved SA water ntent frm hygrsp grwth α-pnene SA dameter GF=1.08 at RH=85% [Varutbangkul et al., ACP 2006, 2367] rrespnds t aersl χ(h 2 )=0.75 rrespnds t derease n W avg frm W SA by fatr 3 26/06/2008 Götebrg, Nenne Prsle 17/28 Humdty effet n SA mass? at mst (nl. ntamnatn), we bserved an a-pnene SA mass grwth f ~20%» we dd nt see a large RH effet n SA mass the bserved SA mass grwth s nsstent wth a * wet shft f ~1.5» ths s abut half the * wet shft expeted frm the effet f pure SA hygrsp grwth n A W avg there may be an addtnal γ-effet n *:» pseud-dealty nt vald assumptn» γ rg nreasng wth water uptake (n surprse) 26/06/2008 Götebrg, Nenne Prsle 18/28 9
10 Partle phase separatn expermental evdene (P rg ) rg H 2 W avg effet smaller fr gven ttal water uptake f aqueus phase separates frm absrbng rgan phase (P Aq ) rg H 2 rg rg H 2 2 (G) 26/06/2008 Götebrg, Nenne Prsle 19/28 Future wrk ntamnatn rretn => better nstran SA grwth phase separatn: water ntent f absrbng rgan phase atvty effents: AIM mdel nludng rgans experments w. ther terpenes/mxed terpenes 26/06/2008 Götebrg, Nenne Prsle 20/28 10
11 Take-hme message #1 The predted effet f RH n SA gas-partle phase parttnng s hghly dependent n the assumed dry SA vlatlty dstrbutn. 26/06/2008 Götebrg, Nenne Prsle 21/28 Take-hme message #2 If the partle phase separates nt dstnt rgan and aqueus phases, the effet f a gven ttal water uptake nt the aersl phase n SA gas-partle phase parttnng wll be muh less than f the water and rgans parttn nt a sngle absrbng rgan aersl phase. 26/06/2008 Götebrg, Nenne Prsle 22/28 11
12 Surfatants n lud drplet atvatn lud drplet atvatn: Köhler thery surfatant parttnng n an aqueus drplet results and future wrk 26/06/2008 Götebrg, Nenne Prsle 23/28 Clud drplet atvatn Köhler equatn S= pw 4ν σ = aw exp w 0 pw RTd S atvatn rtal pnt (S,d) atvated drplet d>d d 26/06/2008 Götebrg, Nenne Prsle 24/28 12
13 Surfatant parttnng => greater predted S and S Srjamaa et al. (ap 2004) H 3 C surfatants derease σ fatty ad sdum salts: sdum laurate - preferentally nentrate n the surfae» surfae-bulk parttnng mrsp drplets have large surfae area-t-bulk vlume rat smaller equlbrum surfae area and bulk vlume nentratns Na + S = p p w 0 w = a w 4ν wσ exp RTd a w lwered less σ lwered less 26/06/2008 Götebrg, Nenne Prsle 25/28 Prsle et al. (Tellus B 2008) d 13
14 Take-hme message #3 If the surfatant prpertes are aunted fr n predtng lud drplet atvatn, the effet f surfatant parttnng between the drplet bulk and surfae must be aunted fr n bth Kelvn and Rault terms f the Köhler equatn, else partle rtal supersaturatns are nsderably underestmated. 26/06/2008 Götebrg, Nenne Prsle 27/28 Thank yu see yu at EAC2008! Aknwledgements are due:» Prfs. Nel Dnahue and Spyrs Pands (CMU)» Gab Engelhart (CMU)» Prf. Ar Laaksnen (FMI)» Rkka Srjamaa (Unv. Kup), Tm Raatkanen (FMI)» CCAR, BACCI & EUCAARI 26/06/2008 Götebrg, Nenne Prsle 28/28 14
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