Photolysis of Particulate Nitrate: a Daytime HONO Source and a Re-NOx-ification Pathway in the Troposphere (TROPospheic HONO: TROPHONO) A Component of.

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Presentation transcript:

Photolysis of Particulate Nitrate: a Daytime HONO Source and a Re-NOx-ification Pathway in the Troposphere (TROPospheic HONO: TROPHONO) A Component of NOMADSS (Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources and Sinks) Field Campaign Xianliang Zhou (Wadsworth Center and SUNY Albany) Jochen Stutz (University of California, Los Angeles)

Objective Objective: To investigate the role of particulate nitrate photolysis in the cycling of reactive nitrogen species in the troposphere, focusing on HONO as an intermediate product. Hypothesis 1 Hypothesis 1: Photolysis of particulate nitrate in aerosol particles, and, to a lesser extent, NO 2 conversion on organic aerosol, are major sources of HONO in the low-NOx troposphere above the surface boundary layer. Hypothesis 2: Hypothesis 2: Photolysis of particulate nitrate in aerosol particles represents an important pathway to recycle HNO 3 /nitrate back to photochemically reactive NO x (re-NOx-ification) in the troposphere.

 Substantial daytime HONO exists in the upper atmospheric boundary layer and free troposphere  require a strong daytime HONO source in the air column.  Photolysis of particulate nitrate (pNO 3 ) in aerosol is fast, with a lifetime of ~1.4 hr for pNO 3, with HONO as a dominant product (HONO/NO 2 = 3 - 9) Supporting Evidences

Potential impact of p-NO 3 photolysis on tropospheric photochemistry

1. Daytime horizontal transects and vertical profiling over land and ocean: To establish daytime distributions of HONO and its production rate, and their relationships with pNO 3, NO x, pOrganics, aerosols, and O 3 in different air masses. 2. Daytime HONO production in urban plumes: To study daytime HONO production in the urban plumes as a function of photochemical ages, and to establish the maximum HONO contribution from the NO x precursor. 3. Nighttime HONO accumulation/early morning decay: To study nighttime accumulation and morning hour decay of HONO. The HONO formation rates during the day and the night will be compared. 4. Bulk aerosol sampling: To collect aerosol samples for laboratory pNO 3 photolysis experiments. Flight Strategy/Experimental Designs

horizontal transects and vertical profiles *

HONO system Aqueous scrubbing Azo dye derivatization Long-Path Absorption Photometric (LPAP) detection of azo dye Detection limit ~1 pptv 90% response time ~1 min

Ambient air H2O SA/NE D H2O MFC SA/NED Valve/sampler box Relays HONO system

HONO data from two HONO systems

Ambient air MFC Valve/sampler box Relays Cd reductor NH 4 Cl buffer SA/NE D HNO 3 system Aqueous scrubbing NO 3 - to NO 2 - conversion on Cd-reductor Azo dye derivatization Long-Path Absorption Photometric (LPAP) detection of azo dye Detection limit ~20 pptv 90% response time ~1 min

PNO 3 system Aqueous scrubbing NO 3 - to NO 2 - conversion on Cd-reductor Azo dye derivatization Long-Path Absorption Photometric (LPAP) detection of azo dye Detection limit ~20 pptv 90% response time ~1 min Ambient air SA/NE D MFC Valve/sampler box Relays Cd reductor NH 4 Cl buffer

Ambient air MFC Valve/sampler box Relays H 2 O/AcN P-Organics system Aqueous scrubbing Long-Path Absorption measurement a 300 nm