Abstract

Abstract. Long-term measurements from satellites and surface stations have demonstrated a decreasing trend of tropospheric carbon monoxide (CO) in the Northern Hemisphere over the past decade. Likely explanations for this decrease include changes in anthropogenic, fires, and/or biogenic emissions or changes in the primary chemical sink hydroxyl radical (OH). Using remotely sensed CO measurements from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument, in situ methyl chloroform (MCF) measurements from the World Data Centre for Greenhouse Gases (WDCGG) and the adjoint of the GEOS-Chem model, we estimate the change in global CO emissions from 2001 to 2015. We show that the loss rate of MCF varied by 0.2 % in the past 15 years, indicating that changes in global OH distributions do not explain the recent decrease in CO. Our two-step inversion approach for estimating CO emissions is intended to mitigate the effect of bias errors in the MOPITT data as well as model errors in transport and chemistry, which are the primary factors contributing to the uncertainties when quantifying CO emissions using these remotely sensed data. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, and unchanged anthropogenic CO emissions from Europe since 2008. We find decreasing trends of biomass burning CO emissions from boreal North America, boreal Asia and South America, but little change over Africa. In contrast to prior results, we find that a positive trend in CO emissions is likely for India and southeast Asia.

Highlights

  • Tropospheric carbon monoxide (CO) is a product of incomplete combustion and a byproduct of the oxidation of hydrocarbons

  • Miyazaki et al (2015) demonstrated that assimilation of Tropospheric Emission Spectrometer (TES) O3, Ozone Monitoring Instrument (OMI) NO2 and Measurement of Pollution in the Troposphere (MOPITT) CO can provide a better description of tropospheric OH

  • The objective of this work is to investigate the dominant reasons for the observed variation of global tropospheric CO over the past 15 years

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Summary

Introduction

Tropospheric CO is a product of incomplete combustion and a byproduct of the oxidation of hydrocarbons. It plays a key role in atmospheric chemistry because it is the main sink for OH and an important precursor for tropospheric ozone (O3). Recent studies have demonstrated significant change in tropospheric CO abundance in the past decade. Using Atmospheric Infrared Sounder (AIRS) CO measurements, Warner et al (2013) indicated that the Northern Hemispheric CO mixing ratio decreased by 1.28 ppb yr−1 in the period of 2003–2012. Worden et al (2013a) demonstrated that Northern Hemispheric CO column measurements from MOPITT show a decrease of ∼ 0.92 % yr−1 in the period of 2000– 2011. The reason for the large variation of tropospheric CO abundance is still unclear; for example, Strode et al (2016) found decreases in modeled CO abundance over North America and Published by Copernicus Publications on behalf of the European Geosciences Union

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