mercury in municipal solid waste in china and its control...

Mercury in Municipal Solid Waste in China and Its Control: A ReviewHefa Cheng* and Yuanan Hu

State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou510640, China

*S Supporting Information

ABSTRACT: Although a potentially significant and preventablesource of environmental pollution, mercury in municipal solidwaste (MSW) has not received adequate attention in China.Discarded mercury-containing products, if not recycled,ultimately release mercury to air, soil, and groundwater, evenafter being properly collected and disposed of in MSWmanagement facilities. This review presents an overview onmercury in MSW and describes the emissions associated withlandfilling, incineration, and composting in China. Besides end-of-pipe technologies for controlling mercury emissions fromMSW management, strategies for controlling mercury in MSWare also discussed, focusing on mercury source reduction andrecycling. Batteries and fluorescent lamps contribute toapproximately three-quarters of mercury in MSW, and are expected to remain as significant sources of mercury in the nearfuture. Reducing or eliminating the mercury contents in household products, particularly batteries and fluorescent lamps, shouldbe the top priority in controlling mercury in MSW, while it is also important to set mercury contents in consumer products atacceptable and achievable levels based on a life-cycle approach. Meanwhile, cost-effective recycling programs should bedeveloped targeting products containing elemental mercury, such as medical thermometers and sphygmomanometers, and wasteproducts with high mercury contents (e.g., button cells) as well.

1. INTRODUCTIONMercury, in both inorganic and organic forms, is a significantpublic health and environmental concern because of its toxic,persistent, and bioaccumulative properties.1 It occurs in threevalence states in nature: elemental (Hg0, boiling point: 356.7°C), monovalent (Hg2

2+), and divalent (Hg2+), with divalentmercury being more stable and common than monovalentmercury in the environment. In particular, divalent mercury canbe associated with organic molecules forming compounds suchas methylmercury (CH3Hg

+), the most toxic and bioaccumu-lative form of mercury.1

Mercury is introduced into the environment both fromnatural sources, including volcanoes, weathering of rocks, forestfires, and soils, and from human activities, with natural andanthropogenic sources contributing approximately equally tothe total atmospheric budget of vapor-phase mercury.2−5 Thetotal global mercury emissions into the atmosphere fromanthropogenic sources, primarily coal and oil combustion,artisanal gold mining, and production of nonferrous metals andcement, are approximately 2000−2300 megagrams (Mg)annually (Figure S1, Supporting Information). The transportof different mercury species emitted into the atmosphere variessignificantly. Oxidized mercury undergoes wet and drydeposition regional to the point of emission with a shortatmospheric lifetime (∼1 week), while the particulate mercurybound to particles is locally and regionally distributed, with asomewhat longer atmospheric lifetime of 1−2 weeks.3,6,7

Elemental mercury, which accounts for ∼95% of atmosphericmercury in general, has a long atmospheric residence time of0.5−2 years before undergoing wet deposition (after beingphoto-oxidized to water-soluble Hg2+ species) and drydeposition.2,3,6 As the distribution of elemental mercury isgoverned by local, regional, and global atmospheric circu-lation,3,4,6 excessive mercury emissions in any given region caninfluence the global mercury deposition.3,5,7−10

Mercury emissions from Asia account for over half of theglobal anthropogenic mercury releases,5,9,11 and a significantincrease in anthropogenic mercury emissions is expected withthe rapid economic and industrial development in Asia if nodrastic control measures are taken.10 Despite the fact thatmercury pollution is a problem with global reach, the technicalcapability, environmental awareness, and socioeconomicstructures vary significantly among different countries, withmost developing countries paying much less attention to theeffective control of mercury emissions compared to thedeveloped ones.10 Because elemental mercury can be long-lived in the atmosphere and transported on intercontinentaland hemispheric scales,4,8 a global approach is necessary toreduce mercury pollution in the long term. A legally binding

Received: July 31, 2011Revised: December 1, 2011Accepted: December 2, 2011Published: December 2, 2011

Critical Review

pubs.acs.org/est

© 2011 American Chemical Society 593 dx.doi.org/10.1021/es2026517 | Environ. Sci. Technol. 2012, 46, 593−605

pubs.acs.org/est

global agreement to reduce the risks to human health and theenvironment from mercury, similar to the StockholmConvention on Persistent Organic Pollutants, is beingnegotiated and is expected to be implemented in the nearfuture.12 Unarguably, successful reduction in mercury releasesfrom China, which is the world’s largest mercury consumer andcontributes approximately a quarter of the global anthropogenicmercury emissions,8,13−16 will be a cornerstone of the globalefforts on reducing mercury pollution.

2. MERCURY IN MUNICIPAL SOLID WASTE (MSW)Nonferrous metal smelting and coal combustion are the majormercury sources in China, accounting for >80% of anthro-

pogenic mercury emissions, with the rest contributed bycement production, mercury mining, household waste burning,and other less significant sources (Figure S2, SupportingInformation). Monitoring data available indicate that atmos-pheric mercury pollution is widespread, while mercurypollution has also occurred in other environmental media inChina (Supporting Information). Industrial sources, such ascoal-fired power plants, cement plants, and MSW incinerators,which are typically located just beyond the fringe of large urbanareas in China, vehicular emissions, and domestic stoves areresponsible for the elevated mercury levels in urban air, whilethe atmosphere in remote areas is mainly impacted by mercurytransported from the industrial sources.17 Overall, the major

Figure 1. Mercury uses in China and mercury contents in MSW. (a) Mercury consumption between 1995 and 2009, and the estimated mercurycontents in MSW from discarded batteries, fluorescent lamps, medical thermometers, and sphygmomanometers. Artisanal gold mining process usinggold−mercury amalgamation has been banned in China since 1996, but was still practiced by some private, illegal mines in remote areas.13−15 Onlymercury use data from the state-owned gold mines are included here, while annual mercury use by small scale gold mines ranges from >500 to 264Mg between 1995 and 2004.31 Mercury use in chemical reagents sharply declined after 2000 because of production bans and the lack of data onsmall-scale production. The mercury content in MSW was calculated by assuming 30% of the batteries and fluorescent lamps manufactured wereconsumed domestically, while 1/3 of the medical thermometers and sphygmomanometers were used domestically with 25% of them being disposedof in MSW. (b) Measured mercury contents in MSW from Chinese cities between 1991 and 2005 (data from 32−43). Geometric mean values areshown when averages are not available.

Environmental Science & Technology Critical Review

dx.doi.org/10.1021/es2026517 | Environ. Sci. Technol. 2012, 46, 593−605594

mercury exposure pathways are consumption of contaminatedfish for residents living in coastal areas and inhalation in citieswith severe atmospheric mercury pollution in China.13,14,18 Forinhabitants of the mercury mining areas in inland China, intakeof rice, rather than fish, has been shown as the major pathwayfor methylmercury exposure.19,20

Municipalities collect, transport, and dispose of discardedmaterials in urban areas that are generated by households andbusinesses, although small amounts of industrial waste andconstruction waste may also end up in the MSW in China.21

Only a few cities in China have introduced waste sorting, whilewaste items with resale values, such as metals and paper, are

highly recycled by the informal recycling sector comprised ofstreet pickers, dump pickers, and itinerant buyers.21,22 A varietyof mercury-containing products, such as batteries, fluorescentlamps, and thermometers, are discarded as household waste,thus the collection, transport, and disposal of MSW cancontribute significantly to mercury emissions. Globally, it isestimated that waste disposal accounts for approximately 8% ofthe total anthropogenic mercury emissions.23 Due to the highmercury contents in MSW and inefficient flue gas cleaning,MSW incineration used to be a major source of atmosphericmercury in developed countries relying heavily on incinerationfor MSW disposal.24,25 In China, MSW incineration was the

Figure 2. Fate of mercury in typical MSW treatment processes: (a) transformation and cycling of mercury within landfills (anaerobic) and composts(typically aerobic); (b) speciation of mercury at different stages of MSW incineration. More than 80% of mercury in the MSW is released into thegas phase during incineration,47 and most of the vaporized elemental mercury reacts with HCl (released from chlorinated plastics and chloride saltsin MSW) in the flue gas to form HgCl2.

6 As the flue gas cools, some Hg0 and Hg2+ condense and adsorb onto the surface of fly ash particles, formingparticulate mercury (Hgp). APCDs can capture some mercury from the flue gas, although their removal efficiencies vary significantly for differentmercury species due to differences in their physical/chemical properties.6,48 Particulate control devices such as fabric bag filters can efficiently removeHgp; Hg

2+ is mostly removed by adsorption or chemical reaction, while Hg0, which is very volatile and not very reactive, is substantially more difficultto remove from the flue gas.



leading sector in mercury emission growth, increasing from 0.6to 10.4 Mg·year−1 over the 1995−2003 period at an annualgrowth rate over 40%.15

With rapid economic growth and unprecedented urban-ization (Figure S3, Supporting Information), MSW disposal hasbecome a major challenge for many Chinese cities.21,22,26−28 Atotal of 157 teragrams (Tg) of MSW was collected from 661middle-size and large cities in 2009.29 Landfilling, incineration,and composting accounted for approximately 80.2%, 18.2%,and 1.6% of the waste disposal capacity, respectively; togetherthey disposed of only 70.6% of the collected MSW in 2009(Table S1, Supporting Information). Due to limited spaceavailable for construction of new landfills, incineration isplaying an increasingly important role in MSW management inChina.21,22,26−28 By 2015, incineration is expected to accountfor over half of the MSW disposal capacity in the easternprovinces, economically more developed regions, and thedensely populated regions, as well as over a quarter of the MSWdisposal capacity in central and western China.22,30

Figure 1a shows the significant changes in mercury usage inChina between 1995 and 2009. Production of caustic soda,polyvinyl chloride, and chemical reagents, and artisanal goldmining consumed large amounts of mercury during this period,depending on market demand and production bans. Theamount of mercury used by the battery industry fell from 582.4Mg in 1995 to 140 Mg in 2009, largely due to thecommendable efforts by the manufacturers to eliminate orreduce mercury from retail batteries. Mercury use by thelighting industry did not follow the dramatic decrease observedfor the battery industry. Instead, it increased slowly from 30.9to 55 Mg over the same period. Medical devices, primarilymedical thermometers and sphygmomanometers, also con-sumed large amounts of mercury, while their mercury use haddecreased from the peak of approximately 270 Mg since 2004due to global mercury reduction efforts. With very littlecollection and recycling, almost all the spent batteries andfluorescent lamps end up in the MSW stream, while significantfractions of medical thermometers and sphygmomanometersare also used in households and are discarded into MSW inChina. The estimated concentrations of mercury in the MSWresulting from disposal of batteries, fluorescent lamps, medicalthermometers, and sphygmomanometers are also shown inFigure 1a. It is estimated that mercury content in MSWcontributed by these domestically used mercury-containingproducts decreased from 1.8 mg·kg−1 in 1995 to 0.5 mg·kg−1 in2009, largely due to the significant reduction in mercurycontents in batteries. Batteries comprised approximately 93% ofthe mercury in MSW in 1995, followed by fluorescent lamps(5%). By 2009, batteries still predominated as the majormercury source, contributing approximately 54% of the totalmercury in MSW, with fluorescent lamps accounting for 21%, aconsiderably larger percentage than in 1995. Figure 1b showsthe mercury concentrations measured in MSW from variouscities in China during the period 1991−2005. Despite thesignificant variability, mercury contents were mostly lower than3 mg·kg−1, which is comparable to those in the MSW fromdeveloped countries.44−46 Some MSW samples exhibited veryhigh mercury levels, probably due to contamination by wasteproducts that contained elemental mercury.39

Although the mercury contents of MSW are generally low inChina, the cumulative amount contained in the large volume ofMSW generated each year can be significant. Assuming anaverage mercury content of 0.5 mg·kg−1, the mercury contained

in the MSW collected from the 661 middle-size and large citiesin 2009 amounted to 78.5 Mg, more than 10% of the annualanthropogenic mercury emissions in China. Control of mercuryemissions from MSW management can be more difficultcompared to industrial point sources as the mercury-containingwastes are generated in individual households and are dispersedin large volumes of household and commercial waste items.Nonetheless, the mercury emissions from MSW managementare not only potentially significant, but also largely preventable.

3. MERCURY EMISSIONS FROM MSW MANAGEMENT3.1. Landfilling. After being buried in landfills, the mercury

contained in a variety of discarded items can still impact thesurrounding soil, groundwater, and even the air throughleachate and gas emissions. Mercury transformation in landfillsis mediated primarily by bacteria, but is also influenced byphysical conditions, such as temperature, pH, and the presenceof oxygen. As illustrated in Figure 2a, most of the mercuryeither precipitates as highly insoluble cinnabar (HgS) or bindsto the abundant organic matter, while the rest can remain aselemental mercury in situ, vaporize into the gas phase, or leachout into groundwater.45,49 Because landfills reduce wastevolume by generating methane with anaerobic bacteria, volatilemethylated mercury compounds also form during MSWdecomposition.50,51 Many studies have demonstrated thatlandfills could serve as a potential atmospheric mercury source(e.g., 40,52−54).Table 1 shows the concentrations of mercury species

detected in leachate, landfill gas, and cover soils from variousMSW landfills in China. Elevated levels of mercury were foundin these media, clearly indicating the releases and emissions ofmercury from mercury-containing waste products buried inlandfills. Mercury concentration in leachate depends on manyfactors, such as the mercury content in the MSW, solution pH,presence of sulfide, and retention by organic and inorganicmaterials in MSW. Such leachate can cause groundwatercontamination from unlined landfills and those with brokenliners. Compared to the mercury in leachate, the mercury inlandfill gas has received little attention in China until recently.Feng and co-workers measured the mercury emissions from thesurface cover of several MSW landfills in China;40,59−62,81 theyobserved that mercury emissions from the landfills were 1−2orders of magnitude greater than those from the backgroundzones and highly correlated with the mercury contents in theupper substrate.62,81 Maximum mercury emissions occurred atthe working face, which decreased significantly after beingcovered by soil or vegetation, while the vent pipes appeared tobe the least significant mercury emission sources.40 Overall,methylated mercury species accounted for <5% of the totalmercury in the landfill gas,40 but posed a significant concernbecause of their extreme toxicity. Pollution of topsoilssurrounding landfill sites also occurred, probably fromdeposition of mercury in the landfill gas.39,40,42

3.2. Composting. MSW composting is typically accom-plished by either aerobic or anaerobic processes, withbreakdown of organic matter taking place much faster in theformer (months vs years). The fate of mercury duringanaerobic composting is similar to that in landfills. In aerobiccomposting, microbiological processes are significantly en-hanced to achieve rapid transformation and degradation oforganic waste under controlled temperature, moisture, andaeration. The main forms of inorganic mercury in aerobic,biologically stabilized solid waste composts are mercuric oxide



Table

1.Mercury

Con

tentsin

Various

Environ

mentalMedia

Associatedwithor

Impacted

byMSW

Managem

entin

China

city/region

year

medium

mercury

content

source

landfill

Guangzhou

1996

leachate

25μg·L−1

55

Guiyang

2005

leachate

0.0794

μg·L−1

42

Shanghai

2003

leachate

1.016μg·L−1

56

Xi’an

1997

leachate

0.025μg·L−1

57

Xiamen

2001

leachate

0.12−0.17

μg·L−1

58

Shanghai

2003

groundwater

inlandfillmonito

ringwells

0.04−0.09

μg·L−1

56

Shanghai

2003

surfacewater

from

riversflowingthrough

thelandfillsite

0.05−0.27

μg·L−1

56

Guiyang

2003

landfillgas

0.5yearafterMSW

beingfilled:

665.5±291.2ng·m

−3fortotalgaseous

mercury,2.06±1.82

ng·m

−3formonom

ethylmercury,

and9.5±

5.2ng·m

−3fordimethylmercury;

1year

afterMSW

burial:25.6±

3.2ng·m

−3fortotalgaseousmercury;

2yearsafterMSW

burial:14.5

±1.8ng·m

−3fortotalgaseousmercury,and

0.18

±0.06

ng·m

−3formonom

ethylmercury

59,60

Wuhan

2004

landfillgas

7.0−

68.9ng·m

−3

61

Guiyang

1989−1995

landfillcoversoil(w

ithtreesgrow

n)0.64

mg·kg

−1

62

Guiyang

1989−2001

landfillcoversoil(notreesgrow

n)6.53

mg·kg

−1

62

Guiyang

1994−2004

landfillcoversoil

3.12−6.53

mg·kg

−1

39,40

Guiyang

2005

landfillcoversoil

0.188±

0.026mg·kg

−1

42

Shanghai

1989−2001

landfillcoversoil

0.018−

0.26

mg·kg

−1

63

Wuhan

1995−2005

landfillcoversoil

0.037−

0.099mg·kg

−1

39,40

compost

Beijing

1999

compost

3.57

mg·kg

−1

64

Beijing

2001

compost

2.59

mg·kg

−1

65

Beijing

2003

compost

0.42−6.06

mg·kg

−1

66

Daqing

2001

compost

1.06

mg·kg

−1

65

Guangzhou

1999

compost

0.43

mg·kg

−1

64

Guiling

2008

compost

0.011−

0.016mg·kg

−1

67

Hefei

2000

compost

0.66−1.36

mg·kg

−1

68

Liuzhou

2001

compost

0.31

mg·kg

−1

65

Shenzhen

1999

compost

0.6−

0.79

mg·kg

−1

69

Yibin

1996

compost

0.0023

mg·kg

−1

70

averageof

22Chinese

cities

1999

compost

9.23

mg·kg

−1

64

fivemajor

regionsin

China

2007

compost

0.48−2.77

mg·kg

−1

71

incineratio

nHangzhou

2006

bottom

ash

0.16

mg·kg

−1formixed

MSW

;0.10

mg·kg

−1forsource

classifiedMSW

72

Shanghai

2003

bottom

ash

0.45

mg·kg

−1

36

Shanghai

2004−2005

bottom

ash

1.9−

4.3mg·kg

−1

73

Shenzhen

2003

bottom

ash

0.28−0.54

mg·kg

−1

36

Chongqing

2005−2006

flyash

8.52

mg·kg

−1

74

Harbin

2004

flyash

3.08

mg·kg

−1

75



(HgO) and soluble complexes such as HgCl2 (Figure 2a),which can be dissolved and mobilized by rainwater percolatingthrough the compost residues.45 Methylmercury can also beproduced under aerobic conditions and by pure cultures ofaerobic microorganisms, although the rate is much slower thanunder anaerobic conditions82 and only a very minor fraction ofmercury in compost products exists in methylated forms.83

The mercury content in compost depends on the presence ofmercury-containing items in the MSW and the extent of wastesorting, thus it can vary significantly. Most compost products inChina contained less than 1 mg·kg−1 mercury (Table 1), whichis relatively low compared to the mercury contents (0.9−20.3mg·kg−1) of those in developed countries.84 This might be dueto the relatively low levels of mercury in the MSW stream ofthese cities and waste separation at the composting facilities.Despite the lack of evidence indicating that mercury in MSWcomposts could pose a risk to human health or theenvironment,84,85 spreading mercury-containing composts toagricultural soils may not be an environmentally sound practicebecause mercury and other heavy metals can accumulate in soilsand be taken up by plants.86

3.3. Incineration. Most mercuric compounds are thermallyunstable at temperatures above 700−800 °C, thus nearly all ofthe mercury occurring in MSW is released to the flue gas uponincineration, with only approximately 4% remaining in thebottom ash.6,87 Figure 2b schematically illustrates the fate ofmercury species at different stages of MSW incineration. Mostof the vaporized mercury condenses on the fly ash as the fluegas cools and is removed by air pollution control devices(APCDs), while a small fraction can escape the flue gascleaning system. Table 1 also summarizes the concentrations ofmercury in bottom ash, fly ash, and flue gas of MSWincinerators, and in the environmental media impacted byMSW incineration. As expected, mercury was significantlyenriched on the fly ash (including APCD residue) compared tothe bottom ash. The fly ash should be buried in hazardouswaste landfills, where the fate of the mercury attached to fly ashparticles is expected to be similar to the case of direct landfillingof the mercury-containing MSW (Supporting Information).Despite flue gas cleaning, mercury concentrations in the stackgas and air surrounding MSW incinerators were elevated. Therelatively high levels of mercury in the surface soils and plantssurrounding incinerators resulted primarily from deposition ofparticulate mercury emitted with the stack gas.79,80

Flue gas cleaning systems comprised of wet scrubber, fabricbag filter with carbon, and/or dry sorbent injection had 75−82% average mercury removal efficiencies worldwide.88 InChina, MSW incinerators are typically equipped with a dry/semidry scrubbing system for removing acidic gases, anactivated carbon injection system for capturing dioxins,followed by a downstream fabric bag filter; such a combinationis quite effective at removing mercury from the flue gas.76,77

Field measurements at two large-scale MSW incinerators inShanghai showed 60−100% mercury removal by the APCDs.73

Monitoring results from 20 representative MSW incinerationfacilities in China indicated that mercury emissions from 90%and 60% of them could meet the standards in China (0.2mg·m−3) and European Union (E.U., 0.05 mg·m−3), respec-tively.89

4. MERCURY SOURCE REDUCTION AND RECYCLINGVarious end-of-pipe technologies can be used to controlmercury emissions from landfills, composts, and incineratorsT

able

1.continued

city/region

year

medium

mercury

content

source

incineratio

nHangzhou

2006

flyash

4.8mg·kg

−1formixed

MSW

;7.7mg·kg

−1forsource

classifiedMSW

72

Shanghai

2003

flyash

44.3mg·kg

−1

36

Shanghai

2004−2005

flyash

4.8−

117.7mg·kg

−1

73

Shenzhen

2003

flyash

69.1−84.6mg·kg

−1

36

Guangzhou

2007−2008

stackfluegas

<500−35

500ng·m

−3

76

Shanghai

2005−2006

stackfluegas

200−

1840

ng·m

−3

77

Shanghai

2004

air(300

mdownw

indof

anincineratio

nfacility)

1020

ng·m

−3

78

Shenzhen

2008

surfacesoil(nearan

incinerator)

0.012−

0.136mg·kg

−1

79

Shenzhen

2008

plantleaves

(200−2000

maw

ayfrom

anincinerator)

0.031−

0.247mg·kg

−1

80



based on the emission characteristics of the respective source.Leachate from modern sanitary landfills is often captured andtreated, and the mercury in the leachate, which is primarilypresent in particulate form, can be easily removed bywastewater treatment systems.56,63 With only 35 landfill gaspower plants in operation in 2010, landfill gas is not capturedor simply flared in the vast majority of landfills (over 440) inChina.90 Therefore, it is important to enhance the capture andtreatment of landfill leachate, while improving landfill gascollection and installing mercury capture devices in landfill gasutilization facilities to minimize mercury emissions fromlandfills. Mercury pollution in composting can be reduced byrequiring separate collection of compostable materials, and byemploying centralized separation technologies to remove heavymetal sources, such as batteries and consumer electronics, atthe composting facilities. MSW sorting has been shown to beeffective at reducing the contamination of compost indeveloped countries.84 Although incinerators are required tocontrol the emissions of mercury and other air pollutants, thecurrent standard (0.2 mg·m−3) on mercury emissions fromMSW incineration in China is much looser than those inEurope and the United States (0.05−0.08 mg·m−3).22,91 A morestringent mercury emission standard (0.05 mg·m−3) for newlyconstructed MSW incinerators in China has been proposedrecently.89 Meanwhile, an effective administrative mechanismon MSW incineration and a strong monitoring capacity shouldalso be developed for verification of the actual mercuryemissions from MSW incineration facilities and theircompliance with the relevant regulations.92

Although end-of-pipe technologies can effectively controlmercury emissions from MSW management, minimization andelimination of mercury in the solid waste is far more desirablecompared to the pollution control strategies.92 This can beachieved by preventing mercury-containing items from enteringMSW and recycling them before sending the waste for disposal,and more preferably, by eliminating nonessential use ofmercury in consumer products.4.1. Batteries. The single most significant source of

mercury in MSW in China is consumer batteries. Significantregulatory efforts have been made to reduce mercury contentsin all types of batteries since the late 1990s, as summarized inTable 2. The then State Environmental Protection Admin-istration issued a technical guideline on disposal and recyclingof waste batteries, reiterating the limits on mercury contents inbatteries in 2003.93 Besides restricting mercury contents inbatteries, some regulations also outlined the obligations ofmanufacturers and importers on collecting and recycling high-mercury-content batteries, and promoted mercury-free andlow-mercury batteries.93,94 As a result of the joint efforts ofgovernment agencies and manufacturers, mercury contents inbatteries and mercury consumption by the battery industry inChina have been drastically reduced (Figure 1a). A newdirective currently under review further aims to reduce themercury consumption of battery industry by 80% (from 140Mg in 2009 to 26 Mg in 2015) through implementingnonmercury production technologies.95 Today, batteries exceptbutton cells produced by the major manufacturers in Chinacontain very low levels of mercury, although batteries made bysome small producers may far exceed the mercury contentlimits (in violation of the relevant regulations).Despite the sharp decline in the use of mercury in consumer

batteries, waste batteries remain a major source of mercury inMSW. The overall recycling rate of batteries in China is less Table

2.PastandCurrent

Regulations

Restricting

Mercury

Use

inBatteries

inChina

year

ofenactm

ent

mercury

contentrequirement

regulatio

n/directive

1995

Batterieswith

>1mg·kg

−1mercury

werenoteligiblefortheChina

Environm

entalLabel.

The

certifiabletechnicalrequirementforenvironm

entallabelingproducts:Mercury-freedrycells

andbatteries(H

JBZ

9-1995);StateEn

vironm

entalProtectio

nAdm

inistration:

Beijing,China,1

995.

1999

Productio

nandtradeof

allmercuric

oxidebatterieswerebanned.

Catalogue

ofoutdated

productioncapacity,technologiesand

productstobe

phased

out(batch1);StateEconomicand

Trade

Com

mission:Beijing,China,1

999.

2001

Productio

nandtradeof

zinc−carbon

batteriesandalkalinebatteriescontaining

>250

mg·kg

−1

mercury

werebanned.

Regulationon

mercury

contentlim

itationforbatteries;China

LightIndustry

Associatio

n:Beijing,China,1

997.

2005

Alkalinebatterieswith

>1mg·kg

−1mercury

werephased

out.

Regulationon

mercury

contentlim

itationforbatteries;China

LightIndustry

Associatio

n:Beijing,China,1

997.

2005

Maximum

allowablemercury

contentlim

itsweresetat1mg·kg

−1forzinc−carbon

batteries,and20

mg·g−

1forzinc−air,alkaline,andsilver

oxidebutton

cells.

Primarybatteries-p

art2:

Physical

andtechnologicalspecifications

(GB8897.2-2005);GeneralAdm

inistrationof

QualitySupervision,

Inspectio

nandQuarantine:

Beijing,China,2

005.

2009

Zinc−

air,alkaline,andsilver

oxidebutton

cells

containing

≤5mg·kg

−1wereclassifiedas

“mercury-

free”batteries,whilethosewith

20mg·g−

1mercury

wereclassifiedas

“mercury-containing”

batteries.

The

limitationofmercury

contentforzinc

silveroxide,zinc

oxygen

andzinc

manganesedioxidebuttonbatteries(G

B24428-2009);GeneralAdm

inistrationof

QualitySupervision,

Inspectio

nandQuarantine:

Beijing,China,

2009.

2010

Zinc−

mercury

batteriesandalkalinebatteriescontaining

>1mg·kg

−1mercury

werebanned.

Catalogue

ofoutdated

productiontechnologiesandproductsto

bephased

out(2010);Ministryof

Industry

and

Inform

ationTechnology:

Beijing,China,2

010.

2015

Alkalinebutton

cells

with

>5mg·kg

−1mercury

will

bephased

out.

Catalogue

ofoutdated

productiontechnologiesandproductsto

bephased

out(2010);Ministryof

Industry

and

Inform

ationTechnology:

Beijing,China,2

010.



than 2%.96 Although environmental groups and activists havecalled for full recycling of batteries in China, the task isdaunting and the cost is prohibitive given the large number ofbatteries discarded each year (approximately 8 billion).Meanwhile, mercury reduction in batteries began in the late1990s and continues today. Most alkaline batteries aremanufactured with “no mercury added”, whereas button cells(except the lithium ion type) still contain relatively high levelsof mercury (up to 20 mg·g−1). Although recycling the batteriescontaining low levels of mercury reduces environmental impactrelative to discarding them, such programs are not cost-effectiveat recovering mercury from the MSW stream.97 Because of themuch smaller sizes and higher mercury contents of button cells,the costs associated with their collection and transport aremuch lower compared to those for other types of consumerbatteries, thus they should be the primary target of batteryrecycling programs. Overall, reduction of mercury input to theMSW stream from batteries can be best achieved by continuingto reduce the mercury contents in all types of batteries throughtechnological innovation, legislation, compliance and enforce-ment efforts, and by recycling the button cells with highmercury contents.4.2. Fluorescent Lamps. As an energy-efficient alternative

to incandescent light bulbs (ILBs), fluorescent lamps havebecome one of the main types of light source in China (FigureS4, Supporting Information). Fluorescent lamps containvarying amounts of mercury, depending on their type, size,and manufacturer. Although export-oriented manufacturersfollow the strict standards set by the U.S. and E.U., compulsoryregulations on mercury contents in fluorescent lamps arelacking in China and reduction of mercury use is largely basedon voluntary efforts of the manufacturers. Fluorescent lampscontaining <10 mg of mercury are certified with the ChinaEnvironmental Label,98,99 but lamps with much higher mercurylevels are common on the market. Mercury consumption by thelighting industry would reach 90 Mg by 2015, and fluorescentlamps would replace batteries as the most significant source ofmercury in MSW, if no changes were made in the mercurycontents in fluorescent lamps and the current manufacturingpractices prevailed. A national standard on mercury content influorescent lamps is currently being drafted, which is expectedto significantly reduce their mercury use and emissions in thenear future.100

Containing mercury in spent fluorescent lamps is achallenging task for MSW management: some of these lampsbreak and release mercury into the atmosphere duringtransport, while the ones that survive the transport mayeventually break during compaction at landfill sites, or duringshredding at incineration or composting facilities.101 Unlikebatteries, there has been no regulation or official recyclingprogram for fluorescent lamps, and the spent lamps are simplydisposed of as general MSW in China. The Ministry ofEnvironmental Protection is drafting a technical guideline onMSW disposal that will require separate collection and disposalof fluorescent lamps along with other hazardous substances.102

However, compared to other mercury-containing wasteproducts, such as batteries, recycling of fluorescent lamps canbe more difficult. Each lamp contains only milligrams ofmercury and must be carefully transported to a facility to avoidbreakage. Recycling of fluorescent lamps, particularly compactfluorescent lamps that have relatively lower mercury contents, isa very expensive way to recapture small quantities of mercury(Supporting Information). Instead, the problem of mercury in

fluorescent lamps can be best prevented through better designand manufacturing practices. Table 3 shows that 1 million 4-

foot linear fluorescent lamps with a high mercury content of48.2 mg could release 38.6 kg of mercury at 20% recycling rate,and 28.9 kg of mercury at 40% recycling, a rate that is expensiveand difficult to achieve. On the other hand, only 8.2 and 5.0 kgof mercury would end up in the MSW stream from these lampswithout any recycling if their mercury contents were reduced to8.2 and 5.0 mg, respectively. Such comparison demonstratesthe profound impact of source reduction via technologyinnovation on the net mercury impact of fluorescent lamps.Significant reductions in the mercury contents in fluorescentlamps remain to be made by the lighting industry in China.Policy measures that provide incentives or require allmanufacturers to achieve “best practice” in lamp design andmanufacturing should be developed.101 Meanwhile, to reduceatmospheric emissions of mercury, spent fluorescent lamps withlow mercury contents should be buried in lined MSW landfillswhile banning their incineration.Although total elimination of mercury from fluorescent

lamps is not possible in the near term,103 their use should beactively encouraged because of the negative net mercuryemissions over their lifetimes. Unlike the case of batteries,banning certain mercury-containing lamps could be moredetrimental to the environment and public health due to thelost energy-savings. Coal-fired power plants generate approx-imately 80% of total electricity and account for 12.7% ofatmospheric mercury emissions in China.16 Fluorescent lampssave up to 75% of energy use compared to ILBs and last up to10 times longer. Substituting ILBs with fluorescent lampsdrastically reduces net mercury emissions, even if they are notproperly disposed of, as the amounts of mercury contained inthe lamps are relatively small compared to the avoided mercuryemissions from electricity generation (Table S2, SupportingInformation). Up to 75% reduction in mercury emissions canbe achieved compared to ILBs with full recycling of themercury contained in fluorescent lamps.104 With their energy-savings, florescence lamps also offer other significant environ-mental benefits, e.g., reduction in CO2 emissions.

105,106

4.3. Mercury-Containing Medical Devices. Medicalthermometers and sphygmomanometers contain mercury thatis measured in grams, in contrast to milligrams of mercuryfound in batteries and fluorescent lamps, and thus represent

Table 3. Total Amounts of Mercury (in kg) That Can BeReleased into the MSW Stream from 1 Million 4-Foot LinearFluorescent Lamps under Different Source Reduction andRecycling Schemes

content of mercury in each 4-foot linear fluorescent lamp

recycling rate (%) 48.2 mga 22.8 mga 11.6 mga 8.2 mga 5.0 mgb

0 48.2 22.8 11.6 8.2 5.020 38.6 18.2 9.3 6.6 4.040 28.9 13.7 7.0 4.9 3.060 19.3 9.1 4.6 3.3 2.080 9.6 4.6 2.3 1.6 1.0

aThe lighting industry in the U.S. reduced the average mercurycontent of 4-foot linear fluorescent lamps from 48.2 mg in 1985 to22.8 mg in 1994, to 11.6 mg in 1999, and to 8.2 mg in 2001.103bCurrent commercial lighting efficiency ordinances in some U.S. citiesrequire 4-foot linear fluorescent lamps with mercury content notexceeding 5 mg.



obvious candidates for exchange and recycling programs.101

China urgently needs to develop official collection, recycling,and replacement programs for elemental mercury-containinghousehold items (e.g., medical thermometers, sphygmoman-ometers, thermometers, and barometers), which have beensuccessfully implemented in many developed countries. Suchprograms are cost-effective at reducing mercury in MSW,because recycling each of these products can recapture as muchmercury as recycling hundreds to thousands of batteries andfluorescent lamps, and the costs associated with their collection,containment, and transport are much lower. As mercury-freesubstitutes for mercury-containing medical devices are available(though some may cost more), programs should be developedto phase out production of the old devices and provideincentives to consumers to adopt these replacements.4.4. Electrical and Electronic Equipment. Mercury is

also found in electrical and electronic equipment at varyinglevels. Production of mercury-containing switches and relayshas been banned in China since 2010,107 while electrical andelectronic household products rarely enter the MSW streamdue to widespread electronic waste recycling activities.108 Inaddition, the contents of mercury (along with other 5 groups ofhazardous substances) in all electronic information products,including many not covered by the Restriction of HazardousSubstances (RoHS) directive of the E.U., have been regulatedsince the enactment of the Chinese version of RoHS regulationon March 1, 2007.109 Overall, the mercury contribution fromelectrical and electronic equipment to MSW is negligible,although the electronic waste recycling practices in Chinashould be effectively regulated to prevent secondarypollution.108 Agricultural chemicals and paints, which pre-viously contained mercury compounds because of theirantimicrobial properties and toxicity, are no longer significant

sources of mercury, either, due to the voluntary phase-out bythe manufacturers and regulatory bans, although the use of suchold products may continue to contribute to mercury pollution.

5. POLICY RECOMMENDATIONSBecause the mercury in MSW originates from a wide range ofdiscarded items, control of mercury pollution via enhancedMSW collection and management would require significantinvestment and effort, while source reduction offers astraightforward and more cost-effective alternative. It is notedthat mercury regulations for imported products and productbans in many developed countries have contributed positivelyto mercury reduction in China. To make their productscompetitive on the global market, Chinese manufacturers hadsignificantly improved their product design and manufacturingpractices, which in turn also led to reductions in mercurycontents of the products on the domestic market. Compre-hensive domestic laws, standards, and regulations that prohibitor restrict mercury-containing products, and corresponding lifecycle management programs for these products, should bedeveloped to reduce mercury sources in household waste.Meanwhile, manufacturers should also be provided withfinancial and technical supports to develop alternatives tomercury-containing products and nonmercury productionprocesses. Such efforts will be rewarded with safer consumerproducts and less burden of mercury emission control in MSWmanagement.The effectiveness and cost of reducing mercury in MSW

stream via recycling or source reduction should be assessed indeveloping policy options. Figure 3 shows the projectedamount of mercury releases to MSW in China by 2015 undervarious mercury control strategies. Obviously, source reductionhas much more significant impact on reducing mercury in

Figure 3. Amount of mercury that can be released from batteries, fluorescent lamps, medical thermometers, and sphygmomanometers discarded intothe MSW stream in China under various control strategies. The 2009 base case represents the conditions that 30% of batteries and fluorescent lampsmanufactured in China are consumed domestically, and 1/3 of medical thermometers and sphygmomanometers produced are used domestically with25% of them being disposed of in MSW. The 2015 scheme 1 assumes no change in production and disposal patterns compared to the base case butwith 25% recycling of batteries and fluorescent lamps and 100% recycling of mercury-containing medical devices. The 2015 scheme 2 assumesmercury use by the battery industry is reduced to 26 Mg,95 and mercury use by the lighting industry increases to 90 Mg (due to market growth),while the production and disposal patterns of mercury-containing medical devices are the same as the base case. The 2015 scheme 3 assumesmercury uses by both battery and lighting industries are reduced by 80% from the 2009 level, while the production and disposal patterns of mercury-containing medical devices are the same as the base case. The 2015 scheme 4 assumes 80% reduction in mercury uses by both battery and lightingindustries, while mercury-containing medical devices are completely banned or recycled.



MSW than recycling, and should be the preferred strategy tokeep most mercury out of MSW and thus the environment. Itshould also be noted that the chemical form of mercury indifferent waste products varies significantly. Spent batteries andfluorescent lamps may contain mercury in both elemental andoxidized forms, while thermometers and sphygmomanometerscontain elemental mercury only and in much larger quantities.Elemental mercury is volatile and much more mobile thanoxidized mercury in landfills and composts, although they mayinterconvert among various forms under suitable conditions.Therefore, the consumer products containing large amounts ofelemental mercury should be the primary target of mercuryrecycling programs.Although phasing out the production of mercury-containing

household products and using alternative mercury-freetechnologies can ultimately eliminate the mercury input toMSW, it is important to set achievable goals on mercuryelimination in consumer products. There are some data onmercury emissions from mercury-containing products duringthe production phase, but data on emissions from other phasesof their life cycle are lacking in most cases. As indicated by theexample of fluorescent lamps, determining the acceptable andachievable level of mercury in consumer products based on alife-cycle approach is more practical than complete banning ofmercury.110

In addition to the mercury reduction efforts by the policymakers, product manufacturers, and MSW managementfacilities, active participation by the general public can helpreduce the use of mercury-containing products and increasetheir recycling.92 The general public are the consumers ofmercury-containing products, and are also responsible fordiscarding them into MSW or recycling them. Proper labelingof mercury-containing products and their disposal requirementscan make them readily identifiable by the consumers and helpminimize their accidental disposal in MSW. Public educationand outreach programs can increase the acceptance of mercury-free products, heighten awareness of the recycling programs,involve more individuals and businesses, and thus help reducethe mercury sources in the MSW stream.111

■ ASSOCIATED CONTENT

*S Supporting InformationAdditional information on anthropogenic mercury emissionsfrom different source categories in the world and in China,overview of mercury pollution in China, MSW generation anddisposal in China, incineration fly ash management, mercurycontents and mercury emissions from ILBs and fluorescentlamps over their lifetimes, production of lighting products inChina, and recycling of fluorescent lamps. This information isavailable free of charge via the Internet at http://pubs.acs.org/.

■ AUTHOR INFORMATION

Corresponding Author*Phone: (+86) 20 8529-0175; fax: (+86) 20 8529-0706; e-mail:[email protected].

■ ACKNOWLEDGMENTS

We are grateful to the anonymous reviewers for helpfulcomments and critiques. This work was partially supported bythe National Natural Science Foundation of China (No.41073079), the SRF for ROCS, SEM, and the “One Hundred

Talents” program of the Chinese Academy of Sciences. This iscontribution IS-1417 from GIGCAS.

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