Subscriber access provided by NEW YORK UNIV

Article

Estimation of organic and elemental carbon emitted from wood burning in traditional and improved cookstoves using controlled cooking test Pooja Suresh Arora, and Suresh Jain Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/es504012v • Publication Date (Web): 17 Feb 2015 Downloaded from http://pubs.acs.org on February 18, 2015

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

Environmental Science & Technology is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 26

Environmental Science & Technology

Graphical abstract

ACS Paragon Plus Environment

Environmental Science & Technology

1 2

Estimation of organic and elemental carbon emitted from wood burning in traditional and improved cookstoves using controlled cooking test

3

Pooja Aroraa, Suresh Jaina, b1 a

4 5 6 7 8

Department of Natural Resources, TERI University, Delhi, 10, Institutional Area, Vasant Kunj, New Delhi 110070, India b Department of Energy and Environment, TERI University, Delhi, 10, Institutional Area, Vasant Kunj, New Delhi 110070, India

9

Abstract

10

Emission of various climate and health related pollutant species from solid biomass

11

burning in traditional cookstoves is a global concern. Improved cookstoves serve as a possible

12

solution to mitigate the associated impacts. However, there is a need to intensify the efforts in

13

order to increase the data availability and promote revision of existing metrics of cookstove

14

testing. In this study, the effect of different phases of a cooking cycle of Northern India on

15

emission factors of OC and EC (char and soot) was assessed for four cookstoves (advanced,

16

improved and traditional) using Acacia nilotica. Lowest EFs for OC (0.04 g/MJ) and EC (0.02

17

g/MJ) were observed in case of the forced draft cookstove; while the traditional and natural

18

draft top feed cookstove emitted the highest OC (0.07 g/MJ) and EC (0.09 g/MJ),

19

respectively. Variation in terms of EFs for OC and EC (char & soot) within the cooking cycle

20

was also found to be significant.

21

Key words: Biomass energy; Controlled cooking test; Black carbon; Regional cooking cycle;

22

Regression analysis

23 24

Introduction

25

In India, ~66% percent of the households depend on solid biomass fuels such as wood,

26

cow dung and crop residues in order to fulfil their cooking energy needs.1 Combustion of these

27

solid biomass fuels in inefficient traditional cookstoves leads to deterioration of indoor air

28

quality due to emission of both particulate matter (PM) and gaseous pollutants. A characteristic 1

Corresponding author, Department of Natural Resources, TERI University, 10, Institutional Area, Vasant Kunj, New Delhi-110070, India; Tel: +91-11-2612 2222; Fax: +91-11-2612 2874; Email: [email protected]; [email protected]

1 ACS Paragon Plus Environment

Page 2 of 26

Page 3 of 26

Environmental Science & Technology

29

of carbonaceous part (organic and black carbon) of PM has a strong bearing on the atmospheric

30

radiative balance. Black carbon (BC) or elemental carbon (EC) content of PM has been

31

identified as the major precursor of climate change due to its high intensity radiative forcing

32

despite its short residence time in the atmosphere.2 Organic carbon (OC), on the other hand, has

33

been linked to light scattering properties3 leading to cooling effect in earth’s atmosphere. OC

34

(also known as ‘brown carbon’) has recently been found to be a significant source of light

35

absorption activity in the atmosphere.4,5 Apart from impact at the global level, chemical

36

composition of PM is also responsible for altering the environmental conditions at regional and

37

local levels, which primarily include visibility reduction and changed rainfall patterns in areas

38

where biomass burning is a common practice.6,7 Chemical characteristics of PM emitted from

39

inefficient cookstoves can also be linked to adverse effects on human health because of their

40

toxicity.8-10

41

Chemical composition of PM is highly dependent on the type of combustion device, fuel

42

properties and type of activity leading to variation in emissions.11 Field studies have a definite

43

advantage over laboratory studies when the primary aim of the study is to build emission

44

inventories and assess the impacts on human health. There have been a few field studies, which

45

focus on quantification of emissions of carbonaceous aerosols from cookstoves under actual

46

operating conditions.12,13 However, due to high variation within the data, it is difficult to

47

ascertain the variables responsible for a typical performance of a cookstove.14 One such variable

48

is the “burn cycle” or ‘cooking cycle”, which has been found to influence cookstove

49

performance.15-17 The effect of different cooking cycles can be captured using a laboratory based

50

cooking test by controlling the fuel characteristics such as fuel size and moisture, which has also

51

been found to affect the cookstove performance in a few studies.18-21 The laboratory based

52

cooking tests, such as the controlled cooking test (CCT), can serve as a standard protocol to

53

assess the performance of cookstoves under the influence of different cooking cycles. To the best

54

of the author’s knowledge, no attempt has been made to use CCT as a test in order to identify

55

and assess variation in chemical composition of PM with different cooking cycles associated

56

with diverse food items consumed and the sequence in which they are cooked in different

57

regions. Additionally, the present study has also quantified emission of char and soot-EC from

58

biomass burning in cookstoves. Quantification of these light absorbing chemical species is

59

important since both char and soot-EC act as light absorbing fraction of PM; however, soot-EC 2 ACS Paragon Plus Environment

Environmental Science & Technology

60

has a high light absorption potential compared to char-EC. Char-EC is generated during low

61

temperature combustion while formation of soot-EC takes place under high temperature

62

combustion conditions. Therefore, their quantification can also be used to identify dominant

63

combustion conditions in a particular cooking activity in context of cookstoves.22 The studies

64

conducted on carbonaceous aerosols emitted from cookstoves so far, have not considered char

65

and soot-EC as a measure to predict the dominant combustion conditions in a particular cooking

66

activity. Therefore, the aim of the present study is to quantify the OC and EC content of the PM

67

and further analyse the char and soot EC fractions and their relationship with different

68

combustion conditions in different cookstoves by using the cooking cycle of Northern India.

69

However, the scope of the study is limited to three cookstoves selected under the improved and

70

advanced category, which were readily available in India. Nevertheless, the distinctiveness in

71

designs adopted in the selected cookstoves provides, to some extent, useful set of data on effect

72

of some specific variables on the cookstove performance.

73

Materials and methods

74

Survey

75

A survey was conducted in two villages, Thalan village in district Uttarkashi and Aam

76

Kheri village in Roorkee lying in the plains of Uttarakhand. The households were selected using

77

stratified random sampling with 50 households in each village. The survey was conducted using

78

a semi-structured questionnaire, which comprised of questions related to primary food type, its

79

quantity, frequency and sequence of cooking. However, tasks other than cooking food were not

80

considered during the study. The data collected from the survey was used to standardize the

81

amount and type of each food item cooked in a single meal.

82

Traditional cookstove

83

Traditional (TR) cookstove used in the study was constructed in the laboratory with

84

dimensions and material same as those observed on the field. The cookstove was made up of six

85

bricks covered with mixture of clay, hay and cow dung. The cookstove was constructed on a

86

thick metal sheet to allow ease of movement under the hood during testing. The walls of the

87

cookstove were ~6 cm thick and the height, width and length of the combustion chamber was

88

~22, ~14 and 18 cm, respectively, giving it a U-shaped top view. The cookstove design was

89

similar to the traditional cookstove used by Kar et al.23 in field based studies conducted in

90

Northern India. The cookstove was recoated with clay slurry at the completion of each meal 3 ACS Paragon Plus Environment

Page 4 of 26

Page 5 of 26

Environmental Science & Technology

91

preparation. The traditional cookstove design selected for baseline study holds a great

92

importance in order to assess the actual improvement in a particular study area. For example, the

93

single pot traditional cookstove design in Maharashtra (Western region of India) as reported by

94

Dutta et al. 24 has a V-shaped combustion chamber, which might perform differently from the

95

traditional cookstoves used in Northern India.

96

Improved cookstoves

97

The improved cookstoves (ICSs) were selected for the study among some of the popular

98

designs available in the Indian markets. ICSs can be placed in three common categories, i.e.,

99

basic, intermediate and advanced depending on the technology used to upgrade its performance

100

as described in a report by Dalberg Global Development Advisors.25 The forced draft cookstove

101

(PF) used in this study is manufactured by Philips and can be placed under advanced cookstove

102

category. The PF (Model-4012) cookstove works as a “quasi-gasifier” cookstove. The forced air

103

supply in this cookstove (both primary and secondary) allows adequate mixing of air and

104

combustible gases leading to efficient combustion of fuel.26,27 The other ICSs were; a top feed

105

natural draft cookstove (PN) manufactured by Philips and a front feed natural draft (EN)

106

cookstove manufactured by Envirofit International Ltd, Colorado, USA. The PN (Model-

107

HD4008) and EN (Model-G3300) cookstoves can be considered as an intermediate technology

108

where the former is also a “quasi-gasifier” but with natural air convection and latter is a rocket

109

cookstove. Rocket cookstoves utilize “L” shaped structure in order to enhance the combustion

110

process. The photographs of the cookstoves can be accessed in the research article by Arora et

111

al.16

112

Fuel used

113

Acacia nilotica (Keeker) wood was used in the present study owing to its availability at

114

the test location. Keeker was also found to be one of the commonly used wood species for

115

cooking purposes in the surveyed areas. Since the aim of the study was to assess the relative

116

performance of different cookstoves with a common cooking cycle of the Uttarakhand region,

117

the use of different wood types could be overlooked. Still, the emission factors (EFs) generated

118

in the present study will not be specific to Uttarakhand region in terms of fuel practice and may

119

vary with other wood species used in the study area. In the study region, wood was collected

120

from the closest forest area and gathered wood consisted of a combination of thin and thick

121

stems, which were used for ignition and high power cooking, respectively. A similar pattern was 4 ACS Paragon Plus Environment

Environmental Science & Technology

122

followed in the laboratory experiments where wood was procured from a common source of fuel

123

and only thick branches were used for each cooking task. However, the wood logs were cut into

124

pieces according to the recommended size for the two top feed cookstoves. In case of PF and PN

125

cookstoves, wood size was kept 2×3×10 cm while it was 1.5×1.5×25 cm for EN cookstove. In

126

case of TR cookstove, the wood pieces were also cut into a uniform size of 3×3×25 cm (without

127

bark). The wood moisture during the testing period was 10-18%, which is also the case in field

128

during actual cooking. The calorific values for wood and charcoal were calculated using bomb

129

calorimeter and were found to be ~21 MJ/kg and ~32 MJ/kg respectively.

130

Test protocols

131

The CCT Version 2.0 developed under Household Energy and Health Programme, Shell

132

Foundation (28) was used as a test method to assess the cookstove performance in terms of mass

133

emission factors (EFs) of OC, EC and PM. The EFs were calculated using the total fuel energy

134

consumed for specified cooking task. CCT is a laboratory based international protocol, which is

135

used to compare cookstoves in terms of fuel savings, and involves actual cooking of a meal

136

dominant in the study area. The meal was prepared by a female cook who was a resident of the

137

same region. The experiments were started after adequate training of the female cook with the

138

new ICSs. All relevant parameters were measured during the test in order to calculate OC/EC

139

EFs. During each test, sampling was started as soon as the vessel was put over the cookstove and

140

start time was recorded, which also included the ignition phase emissions. The wood chips were

141

prepared from the same lot of wood used as kindling fuel, in order to maintain consistency. At

142

the end of each cooking phases, sampling was terminated followed by weighing of cooked food

143

and wood left, and the end time was recorded. The charcoal formed was also weighed along with

144

the cookstove and was used for next cooking phase. The graphic representation of steps carried

145

out in CCT is presented in Figure S1 of SI.

146

The Water Boiling Test (WBT) Version 4.1.229 was also used to compare performance of

147

cookstoves with the results obtained from CCT. WBT is a simulation of actual cooking cycles

148

designed principally to study the effect of design on the performance of cookstoves (for more

149

details related to the protocols, please refer to research article by Arora et al.21

150

Sampling set-up

151

The experiments were performed at TERI University’s testing facility located in New

152

Delhi. The testing facility consists of an extraction hood and a dilution tunnel with location 5 ACS Paragon Plus Environment

Page 6 of 26

Page 7 of 26

Environmental Science & Technology

153

provided for PM sampling. Size of the hood was large enough to accommodate the cookstoves

154

manufactured for domestic cooking purposes. The PM sampling point was kept ~9 times the duct

155

diameters from the closest point of disturbance and the PM deposited on the filter (Whatman, 47

156

mm quartz Q-MA, with pore size 0.2 µm) consisted of total particulate matter (TPM). The

157

details of the experimental setup and sampling procedure have been mentioned in detail by Arora

158

et al.16, 17 The schematic diagram of the experimental set-up can be referred in the research article

159

by Arora et al.16

160

OC/EC analysis

161

PM samples collected on quartz microfiber filters (pore size, 0.2 µm) were preserved at a

162

temperature of around -20ºC until the OC/EC analysis was carried out. The filter samples for

163

correction of OC artifacts were collected for few experiments; however, the values were not

164

reduced from the actual concentrations. This was because of the variation of data observed in gas

165

phase OC artifacts, which might result in over or underestimation of the actual OC concentration

166

in the rest of the experiments for which the artifact samples were not collected.

167

The analysis was conducted with the help of thermal-optical method using EC/OC

168

analyser (DRI, Model 2001) using the IMPROVE-TOR carbon analysis.30 The PM mass

169

deposited on the quartz filter is analysed using a 0.5 cm2 section of the filter. In the thermal-

170

optical analyser, the filter punch is first heated in an inert atmosphere (100% Helium, He) which

171

converts the OC fraction into carbon dioxide (CO2). The EC fraction is converted to CO2 in an

172

oxidizing atmosphere (98% He/ 2% Oxygen, O2). The concentration of CO2 produced during

173

both the conditions is analysed by reducing it to methane, which is eventually measured on a

174

flame ionization detector (FID). Transmittance of laser light (633 nm) through the filter is

175

measured to set the split between OC and EC. Further, the actual EC is calculated by correcting

176

for the pyrolysed carbon formed during charring of OC in the first phase. EC data was also used

177

to calculate the char and soot-EC concentrations using EC1, EC2 and EC3, which are produced

178

at a temperature of 550, 700 and 800˚C respectively in 2% O2 and 98% He atmosphere during

179

analysis. Char-EC was calculated by using EC1 minus pyrolysed carbon (PC) and soot-EC using

180

sum of EC2 and EC3. However, limited studies are available in the literature where TOR method

181

has been employed for estimation of char and soot-EC, and the method is still under scientific

182

scrutiny.31

183

Statistical analysis 6 ACS Paragon Plus Environment

Environmental Science & Technology

184

The experimental design for the study consisted of two factors i.e. cookstove types (four

185

levels - TR, PF, PN and EN) and cooking cycle (three levels – pulse (legumes), rice and roti

186

making). Both single and two-way analysis of variance (ANOVA) with replicates were used to

187

confirm significant (α = 0.05) difference in average values of OC and EC EFs and interaction

188

between cookstoves and burn cycle. Further Student’s-test was conducted in order to identify

189

pairs with statistically significant difference in average OC and EC EFs with the help of

190

Bonferroni correction method, where α=α/c (c is the number of paired means compared).32

191

The relationship was established using the coefficient of determination (R2) and

192

Pearson’s correlation coefficients, which confirm that variation in PM EFs was associated to the

193

change in OC and EC EFs.

194

Results and discussion

195

Cooking cycles – Survey results

196

The data collected through the survey conducted in the villages of Uttarakhand, showed

197

that ~64% of the households show two prominent sequences in a single meal i.e. pulse-rice-roti

198

(Indian wheat bread) or pulse-vegetable-roti. Rice and vegetable were found to be cooked

199

alternatively in a single meal throughout the week. Roti's were cooked mostly at the end because

200

of its tendency to loose moisture. Therefore, in the present study the cooking sequence followed

201

an order in which pulse was cooked in the first place, followed by rice and roti, for all the

202

experiments. The vegetable preparation was omitted from the cooking cycle because of the

203

possible interference in the OC quantification in PM due to use of cooking oil. The survey results

204

also showed that the average quantity of pulse, rice and wheat flour consumed in a single meal

205

was around 250 ± 20 g, 300 ± 34 g and 500 ± 23 g, respectively for an average household size of

206

five members. Detailed survey results are available in the study conducted by Arora et al.16

207

Variation in emission factors for OC and EC

208

The variation in EFs for OC and EC during different phases of cooking cycle and their

209

average in the four cookstoves during CCT are presented in Figure 1 and Table 1, respectively.

210

The average EF for OC was found to be the highest in TR cookstove followed by EN, PN and PF

211

cookstoves and difference in average OC EF between TR, and three cookstoves was found to be

212

statistically significant (p

Estimation of organic and elemental carbon emitted from wood burning in traditional and improved cookstoves using controlled cooking test.

Emission of various climate- and health-related pollutant species from solid biomass burning in traditional cookstoves is a global concern. Improved c...
748KB Sizes 0 Downloads 7 Views