C3d Science Nanoparticle emissions from residential wood combustation 2019, chapter introduction background conclusion (geanonimiseerd)

Low

MW

Decrease in oxygen caused PAH levels to increase and bind to NPs Image: high temperature combustion produced carbon aggregations with turbostratic Pellet Stoves

7-30

Boilers

single particles having a single nuclei and temperature combustion produced carbon dominated spherical particles 67,681

nm

Steady Cordwood

structure; low showed

state

lowest

concentrations of NPs

nm; but as small as 12nm to as large as 400 nm Highest concentrations seen during start up Advanced boilers produced smaller particles and lower concentrations than traditional boilers PAHs higher in older boiler technology 60-130 nm (no bark pellets) 220 nm (bark pellets) No obvious trend was observed between full and intermittent output in terms of particle size, only

31,581

60-180

Pellet Boilers

increase in

mass

9,18,31,56,61,691 a

very

slight

concentration.

Particles

were likely inorganic salts Steady state: 25-75 nm; lowest particle concentrations Modulating: 65 nm Smolder: 160-200nm; highest particle concentrations Lower excess air values led to lower particle counts

Chip Boilers

21,56,63,701

and

larger particles, however

another

found

group

greater

concentrations with increased oxygen SEM & TEM images indicated different

types of particles; agglomerates of spherical compact particles, perfectly spherical representing coal fly ash or irregular shaped crystalline platelets. Efficient was typically salts and crystalline while intermediate was a variety of soot agglomerates and ash; smolder was large agglomerates of soot PAHs bound to NPs lowest during efficient burns and highest during smoldering conditions Fireplaces and Masonry

Heaters

10-20

nm;

70-250

nm

100-326

50-65

be agglomerates owed range assumed cooling Start-up had highest concentrations; steady state had lowest Decrease in oxygen corresponded to decrease in NPs Newer technology stoves seemed to produce more NPs Agglomerates with individual particles spherical in shape Normal combustion showed spherical and irregular shapes while smoldering combustion showed Some

the

[2,55,71-73]

nm

start-up

diameters

whereas

a

presences

of heavy

organic compounds

were

characterized

conditions

fireplaces;

mary

air intake

generation’

from the front and the other

group in Finland

with

primary

was

a

more

looked

at

periods in a conusing birch cordwood at 7% study showed a higher particle emission number measured in a dilution tunnel by the ELPI and FMPS during the normal combustion and less than half the particle emission number during smoldering state with geometric mean diameters of 56 and 65 nm by FMPS and ELPI measurements, respectively, for normal combustion, and 118 and 160 nm values for smoldering combustion [55]. Surprisingly for cordwood combustion, the repeatability was good. Even if all operating parameters are kept constant, manual fed cordwood appliances are very variable [58]. The study found the average particle number size distribution for normal com-

compact ‘next

and

the PM

and

gaseous

both normal

and

smoldering wood

combustion

masonry heater made of soapstone moisture content. The results from the

secondary air intake. Measurements were taken from a dilution tunnel using a gravimetric based filter measurement and ELPI. Surprisingly, the study found the opposite trend of most, in that the older technology was more favorable to less particulates but ultimately showed agreement that more NPs were produced in the newer technology. The study found the next generation fireplace produced much higher particle emission numbers for than the conventional fireplace; specifically, for the reduced conditions, the emission numbers were 50 times greater in the more modern fireplace than the older conventional unit [73]. While 80% and 60% (total number of particles) of the total PM consisted of particles with a diameter less than 100 nm, for the new and old fireplaces, respectively, it only contributed to a very small extent of the total mass of the aerosol; 5.5-5.8% and 2.6-0.3% for the new and old fireplaces, respectively during normal and reduced operations [73]. Another

fireplace (4kW)

well

ventional

content) during normal and reduced operation from two difone a conventional fireplace (13 kW} with only pri-

ferent

as

from

had

A group in France looked at the mass and number distributions of wood combustion particles emitted from beech cordwood (12% moisture

irregular and

more

structures

salts but

flaming phase smoldering

to

by small larger particle diameters. Number concentrations were greatest during the start-up phases and especially for cold start-up phases but were lower for smoldering phases. particle

and

to

nm

sintered-like

found

170

1m;

during smoldering

bustion

to

duce

bimodal

a

be unimodal

at

distribution

nm

and

with

peaks

65

the smolder at

70

and

combustion 250

nm

to

pro-

[55]. In ad-

dition, SEM and TEM analysis from the hot stack showed both spherical and irregular shaped particles making up larger agglomerates and fine ash particles remained as separate particles. Normal combustion showed spherical and irregular shapes while smoldering combustion showed more irregular and sintered-like structures. The elemental analysis showed single particles were composed mainly of carbon, but also contained K, S, Zn, and less commonly O, Ca, Fe, Mg, Cl, P and Na were found [55]. Similar to studies mentioned above, particle material volatized under the beam indicating the presence of heavy organic compounds. The group was able to suggest the shifting of particle size during the different combustion conditions seemed to be determined by the amount of condensed organic vapor in the flue gas [55].

emissions

524

(geanonimiseerd)

Renewable and Sustainable

In addition to the work done

by Lamberg

et al.

[9]

on

pellet boiler,

a

the

the

old-type

wood

boiler

could

be

Energy Reviews 103 (2019) 515-528

reduced

if it

connected

was

to

a

group also studied three conventional masonry heaters and one modern masonry heater made of soapstone. All masonry heaters burned birch logs with a low moisture content (10-13% on a dry basis). The

storage tank, similar to advanced modern units, higher quality fuel (lower moisture content} was used, or if fuel amount was decreased and

explored continuous combustion, steady-state periods, cyclic operation, and ignition phases. Overall, GMD sizes ranged from 63 nm to 142nm. The largest diameters were found during incomplete combustion phases and also produced bimodal number and size distributions; the ignition phase also produced a larger GMD [9]. Similar to the pellet boiler discussed above, the most abundant PAHs were pyrene and fluoranthene in addition to phenanthrene and cyclopentalc,dlpyrene

found

for

the amount

small

of the masonry

one

sions

(PAH/PM;)

reasonably

were

low with

a

heaters.

Total

higher

than

PAH that

of

from

emissions the

pellet

PM;

boiler

old-type

decrease

still

‘This literature review

revealed two

research

reports

only

exhaust

sources

with NP

emissions in RWC.

articles and

limited

earlier review papers

and about

reports. An earlier review by Kumar

information

NP

on

emissions

[74]; the authors reported only The

two

from

et

cordwood boilers

still holds

non-vehicles

studies

associated

information

had much

amounts

true

[10]. The

advanced

have

study

pellet systems rivaled oil burners but low efficiencies, high PM emissions,

the International submicron

affordable

for

commented

Energy Agency

particles but residential

such

devices

were

[27]. Another

use

on

very review

using ESPs to expensive and suggested the

review shows

the

combustion

particle

automatic

fuel

to

Several

sizes

was

achieved

the amount

tained

[22]. Very few studies have looked

to

nm

which

chamber.

This

[58]. This

a

[2,56,63,78].

combustion

condition

opshift

Perhaps which

NPs

at

the microstructure of NPs

and greater showed

late reactive

this could also

substances

[65,82].

Ideally, a NP with a low mobility is desired to reduce inhalation or atmospheric risks. Ultimately, it is important to understand the rate of environmentally induced changes and how the migration of particles changes their properties [76]. Understanding the aggregation behavior under both atmospheric and aquatic conditions may help further predict their potential interactions with the ambient environment [26]. Mavrocordatos et al. [18] investigated the affect salt content within the particles play and found their morphology was significantly affected in aqueous environments. Perhaps if a sufficient amount of information was gathered on NPs soot emissions from RWC which included explicit details on fuel type, operating parameters, and sampling conditions, manufacturers and operators could be informed with a ‘best practices’ procedure. As shown in many of the studies reviewed herein, NPs account for a substantial amount of the particle emissions associated with biomass combustion. However, standards enforced by regulatory agencies are mass concentration based, focusing on size ranges less than or equal to 10 um (total PM; PM) or less than or equal to 2.5 um (PMa.5). Due to

makes

reproducibility very larger variation than statement compliments the

have

to

a

as

provide important information on the NPs reactivity. The microstructure of NPs can give information about particle formation, condensation, coagulation [65,80,811 and the ability to accumubut

opthe nature of wood- how it burns and

size distributions feed boilers

burn two

of harmful

favor

indicated formed and

produced. Incomplete combustion, smoldering, and transition conditions are known to favor PAH and black carbon production. Further, when temperatures are low, PAHs can condense or adsorb onto particles [77]. Smaller NPs are known to carry larger PAH molecules and are difficult to remove, while larger more coarse particles carry lower molecular weight PAHs [77]. Likewise, Ghiassi et al. found the most reactive soot had an amorphous nanostructure which was composed of short individual layer planes with no orientation relative to each other [79]. The laboratory study by Hata el al. indicated biomass type and the heating rate had a significant effect on the water soluble OC fraction and the smaller the NP, the more water soluble OC the particle con-

emissions

than

to

above

particles were

reduces

nm

be used

studies

less

years later. Table 3 below summarizes from the papers above. In addition, cold and in-efficient burns exist and there may be

220

could

ratio.

reached,

sensors

fewer concentrations of NPs less than 140

larger than

the air

lambda

current

eight

collected

not

that this

posite trends [58]. This is owed ifficult and

The

control devices may of PM emission concentrations as well as reduce of harmful PAHs produced, they tend to be expensive. In

timal oxygen levels were towards larger particle

be associated with health

of NPs

falls within

charge.

the amount

modulate

which contain particle fracimpacts in local areas [56]. As reported by Tom et al. [75], the majority of published studies were associated with laboratory experiments and field performance measurements were lacking. There is a significant need to characterize the particle types in biomass smoke, since the regional and global climate effects of aerosols from biomass burning depend so strongly on particle properties [17]. However, manually fed cordwood stoves and boilers have a tendency to vary in their burn conditions even if fueled exactly the same way. Schmatloch and Brenn directly observed this when fueling a cordwood furnace and trying to reproduce the size distribution in particles; burn one

full

cost competitive, or boilers must use proper combustion designs and adequate air pollution control technology [54]. Therefore, there is a need to develop cost sensitive, yet effective, submicron PM reduction technologies. One interesting technology discussed in a review by Lim et al. [77], is the use of a miniature pipe bundle heat exchanger (a technology used in the automobile industry) where particles migrate to the lower temperature surfaces and deposit on the tube walls to remove particles from the flue gas. Other options may also include better combustion designs or controls, such as lambda probes. Lambda probes can detect the oxygen levels and effectively

review identified and reviewed

current

starts, modulation periods, an underestimation of real-life can

a

chamber

more studies that explicitly or implicitly provide information regarding NP emission data from RWC. However, measuring and quantifying the presence of NP in emissions, and how these emissions vary based on fuel, appliance type, and combustion period are not always well investigated making correlations hard to draw. The second major review by Bolling et al. (2009) pointed out there has been a lot of work done in steady-state operating conditions but there is limited data on particles from conventional cordwood boilers, modern wood stoves,

tions that

of

gaseous compounds [311]. advanced systems that employ multiple

reduce

also

al.

many

the

instead

easiest way to control emissions is to use a high quality fuel with low ash content, low moisture, and constant piece size whose options may

eighty

statement

finding

boilers would

2006, not

and modern

wood

While

Discussion

7.

loaded

were

and unoxidized

of 0.15-2.8%.

range

of fuel

tion devices to oil burners

emis-

but

batches

poorer combustion conditions increased the amount of particles smaller than 100 nm. Finally, the group compared the wood combus-

group

a

findings by Gaegauf et al. [56]. This also makes it difficult to compare particle size distribution among studies. To complicate matters, Baer indicates that nanoparticles are inadequately characterized since they change with time and can be altered or damaged during analysis [76], so precautions must be taken to not bias research. Some key factors which may cause some uncertainty are sampling locations, sampling temperatures, and dilution ratios [74]. Ozgen et al. point out that the variability of the results concerning the number emissions and the size istribution during different stages of the wood burning cycle suggests that emissions are strongly connected to the combustion conditions lepending on the appliance design and operation [72]. The study by Johansson et al. [31] emissions from pellet boilers were closer to those of an oil burner while old-type wood boilers had the highest. An important piece from the study was that emissions from 525

(geanonimiseerd) NPs

small

the

nano

Renewable and Sustainable

appropriate for particles in they contribute very little to the overall mass. However, they contribute significantly to the overall number of the airborne particles present [11,83] and, potential adverse health effects posed by NPs may go unknown [19]. Lim et al. [77], reported that dilution sampling affects particle emissions by promoting size, current measures may

and

ultrafine

size fraction

be

not

efficient and “cleaner”

more

since

follow.

However,

with

systems,

more

being decreased; causing

one

to

in released

increase

an

efficient

Energy Reviews 103 (2019) 515-528

boiler

argue what

systems PAH is

more

NPs

may

levels

are

NPs

important

or

PAHSs?

represented by particle number measurements. Torvela et al. investigated the intermittent period when switching from one condition to another, finding the properties of the PM emissions varied significantly even within a short period suggesting that an eva-

distribution of batch-wise fired appliances (wood stoves) significantly during a burn cycle, while wood log and continuous fed boilers showed a fairly constant particle size distribution. These differences are likely to influence the biological effects induced by wood smoke particles and therefore it has been recommended to explore how combustion conditions influence the particle properties, their possible health risks, and reactivity within the environment. Although a

luation

and adverse health effects based on average values can be misleading [21]. Further, Lamberg et al. particle property concluded from their study that PM; mass does not reflect all of the

lot of work

variation

In addition, NP emission data from wood burning processes under real-world operating conditions are lacking. More data are needed

nucleation

but

ticles which

from

results in

in the formation of ultrafine

increase

an

Particle

varied

par-

better

are

of environmental

affecting possible

combustion

From

toxic

properties of fine particles originating

[9].

the

Gaegauf et al. [56] study in particular, the highest consuspended particles (TSP) (mg/m®) correlated nicely to the highest total number of nanoparticles ( < 600 nm) collected per MJ of output. Masonry stoves had the highest TSP concentration along with the highest emission factor of NPs per MJ. In comparison, automatic feed pellet boilers had the lowest TSP and the lowest total number emission factor of NPs. However, when looking at the emission factor (mg/MJ) for both TSP and NPs data in detail, the group noticed while each appliance type typically showed good correlation between the two values, individual cases such as the cordwood boiler showed roughly a 40% reduction in the NP emission factor from the TSP emission factor. This supports the suggestion to modify existing test method regulations or add to them a measurement involving particle

about source,

centration of total

size,

count,

surface

or

RWC

emissions

gative

health

41%

suggests wood

effects

surface

smoke

diesel NPs

as

PAH

was higher for combustion particles from wood smoke pared to vehicle exhaust, causing risk for a high mutagenic and nogenic potential [65].

carci-

content

8.

Conclusions

US

Current emission and EU are based

NPs

neither

are

on

measured

because

of their low

that NPs

account

for

with

standing argument regulations or add type

size,

or

wood

has

been

to

them

surface

area.

amount

combustion

the need a

NPs

in these

contribution.

mass

substantial

a

residential

This

review

of

from

RWC to

This

emissions devices.

A

better

predict

the environmental

mass

combustion

control

devices

are

sources.

Emission

include

ESPs

and

controlling

NP

in

been assessed.

1

to

York State Energy Research

New

(geanonimiseerd) Nanomaterials and nanoparticles: me

(geanonimiseerd) 4

result in with

and

(geanonimiseerd) th

environmental

that may associated

sources

toxicity. Biointerphases 2007;2(4):MR17—71.

long

generated nanoparticles, Zurich, Switzerland; 2012. Chemical characterisation of fine particles from biomass burning. ish Meteorological Institute; 2013. ence

on

combustion

mmm

(geanonimiseerd) A pollution in relation

conditions

they

area,

mor-

References

asso-

local

These

but

review revealed

concentrations in the

emissions.

size characterization

Development Authority (NYSERDA} for partial support of this research through contracts # 29697 and # 63038, Dr. Barbara PanessaWarren (Guest Scientist at Brookhaven National Laboratory), Dr. Thomas Butcher (Group Leader of the Energy Conversion Group at Brookhaven National Laboratory), and Dr. John B. Warren (Scientist in the Instrumentation Division at Brookhaven National Laboratory).

in the

large

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Si

E

nld (geanonimiseerd) enen (geanonimiseerd) Teven Bt forte characters noparticulates

controls. Atmos

and generate more mass PAH emissions, but lower NPs. It is a cause for concern that NPs may be undetected as by virtue of their large surface volume ratio

surface

composition data are limited. Predicting or aggregation, agglomeration, dispersion, size, solubility, charge, and composition are all necessary parameters to

the

show

and

evice type, its operation, and the fuel used. We often see an inverse relationship between the total PAH mass and its NP fraction. It is reported that PAH emissions could be up to 100 times higher if a stove was not operated properly, although NP production would be decreased. Also it is reported that, if an advanced system's heating load is ecreased, cordwood and automatic wood-fired boilers (pellet and chips} may have trouble modulating, causing them to cycle frequently

A

varoettenmeat

larger amounts of reactive compounds and, therefore, may induce a more pronounced pro-inflammatory response than larger particles of the same compound. A significant, and unexpected finding is that as conventional units are displaced by modern, to

studies chemical

Acknowledgement

com-

cause

of

NP

expected quantities or concentrations, and environmental help identify situations which may be more favorable than

of

particle

identified

amounts

effects associated

and

modify existing test method involving particle count,

to

the health

about the environmental fate of RWC

Several

has not

particles and emission regulations,

(RWC)

to

measurement

impacts and potential global impacts due atmosphere. increasing

combustion devices

concentration

mass

reflected

nor

allegedly ciated

from wood

overall

an

understand

strategies or higher quality fuel suggested for large biomass boilers condensing heat exchangers but their effectiveness

and recommendations

regulations

to

phology studying

control

may be associated with less nesmaller in diameter and have

study

done

others.

emission

were

[64]. Unfortunately another

area

been

fate and any health concerns of bioNPs. While biomass is often considered and encouraged as a renewable energy source, it is important to not ignore consequences of poor combustion practices and NP production. Several articles have suggested pathways to reduce NPs such as

vehicle emissions to

found

more

pathways

area.

positive note from a study which compared

One

has

with RWC NPs, but little is known NPs and their effect on climate.

adsorb

[10

in

the urban

atmosphere and

the

prospects

na

developing regulatory

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