Abstract

Abstract. Anthropogenic atmospheric emissions of typical toxic heavy metals have caused worldwide concern due to their adverse effects on human health and the ecosystem. By determining the best available representation of time-varying emission factors with S-shape curves, we establish the multiyear comprehensive atmospheric emission inventories of 12 typical toxic heavy metals (Hg, As, Se, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn) from primary anthropogenic activities in China for the period of 1949–2012 for the first time. Further, we allocate the annual emissions of these heavy metals in 2010 at a high spatial resolution of 0.5° × 0.5° grid with ArcGIS methodology and surrogate indexes, such as regional population and gross domestic product (GDP). Our results show that the historical emissions of Hg, As, Se, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn, during the period of 1949–2012, increased by about 22–128 times at an annual average growth rate of 5.1–8.0 %, reaching about 526.9–22 319.6 t in 2012. Nonferrous metal smelting, coal combustion of industrial boilers, brake and tyre wear, and ferrous metal smelting represent the dominant sources of heavy metal emissions. In terms of spatial variation, the majority of emissions are concentrated in relatively developed regions, especially for the northern, eastern, and southern coastal regions. In addition, because of the flourishing nonferrous metal smelting industry, several southwestern and central-southern provinces play a prominent role in some specific toxic heavy metals emissions, like Hg in Guizhou and As in Yunnan. Finally, integrated countermeasures are proposed to minimize the final toxic heavy metals discharge on account of the current and future demand of energy-saving and pollution reduction in China.

Highlights

  • Heavy metals (HMs) is a general collective term which applies to the group of metals (e.g., Hg, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, Zn) and metalloids (e.g., As, Se) with atomic density greater than 4.5 g cm−3

  • Atmospheric emissions of varied HMs from coal combustion are calculated by combining the provincial average concentration of each heavy metal in feed coals, the detailed coal consumption data, and the specific emission factors, which are further classified into subcategories with respect to different boiler configurations and the application rates and removal efficiencies of various air pollutant control devices (APCDs)

  • Ij where E is the atmospheric emissions of each heavy metal; A is the annual production yield of industrial producing processes, volume of municipal solid wastes incineration, or liquid fuel and biofuel consumption etc.; EF is the assumed average emission factors; and j is the emission source classified by source subcategories

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Summary

Introduction

Heavy metals (HMs) is a general collective term which applies to the group of metals (e.g., Hg, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, Zn) and metalloids (e.g., As, Se) with atomic density greater than 4.5 g cm−3 These elements are present in only trace levels in feed coals and raw materials, the huge coal consumption and enormous output of various industrial products have resulted in significant emissions of HMs into the atmosphere. For the first time, we have evaluated the historical trend and spatial distribution characteristics by source categories and provinces of atmospheric emissions of 12 typical HMs (Hg, As, Se, Pb, Cd, Cr, Ni, Sb, Mn, Co, Cu, and Zn) from primary anthropogenic activities during the period of 1949–2012. We classify all sources into two major categories: coal combustion sources and non-coal combustion sources

Methodology of HM emissions from coal combustion sources
Average concentrations of varied HMs in feed coals
HM emission factors from coal combustion sources
Methodology of HM emissions from non-coal combustion sources
Algorithm for determination of dynamic emission factors
Dynamic HM emission factors of nonferrous metal smelting
Dynamic HM emission factors of ferrous metal smelting
Dynamic HM emission factors of non-metallic mineral manufacturing
HM emission factors of biomass burning
HM emission factors of liquid fuels combustion
Dynamic HM emission factors of municipal solid waste incineration
HM emission factors of brake and tyre wear
Activity data
Evaluation of potential uncertainties
Temporal trend of HM emissions by source categories
HM emissions from coal combustion by power plants
HM emissions from coal consumption by industrial boilers
HM emissions from metal smelting and other primary sources
Composition of HM emissions by province and source category in 2010
Spatial variation characteristics of HM emissions
Uncertainty analysis
Proposals for future control policies
Conclusions
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