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Removal of Carbon Monoxide from Simulated Flue Gas Using Two New Fenton Systems: Mechanism and Kinetics Yan Wang, Xuan Han, and Yangxian Liu Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.9b02975 • Publication Date (Web): 07 Aug 2019 Downloaded from pubs.acs.org on August 8, 2019

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Environmental Science & Technology

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Removal of Carbon Monoxide from Simulated Flue Gas Using Two

2

New Fenton Systems: Mechanism and Kinetics Yan Wang, Xuan Han and Yangxian Liu*

3 4

School of Energy and Power Engineering, Jiangsu University, Zhenjiang, 212013, China

5

ABSTRACT: Two novel removal processes of carbon monoxide using two new Fenton systems (i.e. Cu2+/Fe2+

6

and Mn2+/Fe2+ co-activated H2O2 systems) were developed. Effect of several process parameters (concentrations

7

of H2O2, Fe2+, Cu2+ and Mn2+, reagent pH value, solution temperature, and simulated flue gas components) on CO

8

removal was studied in a bubbling reactor. The mechanism and kinetics of CO removal were also revealed.

9

Results show that adding Cu2+ or Mn2+ obviously enhance the removal process of CO in new Fenton systems. The

10

measuring results of free radical yield demonstrate that the enhancing role is derived from producing more ·OH

11

(they are produced due to the synergistic activation role of Cu2+/Fe2+ or Mn2+/Fe2+ in new Fenton systems.

12

Removing efficiency of CO is raised by increasing concentrations of Fe2+, Cu2+ and Mn2+, and is reduced by

13

raising concentrations of CO, NO and SO2. Increasing H2O2 concentration, reagent pH and solution temperature

14

demonstrate a dual impact on CO absorption. Three oxidation pathways are found to be responsible for CO

15

removal in new Fenton systems. Results of mass transfer-reaction kinetics reveal that CO removal processes are

16

located in a fast-speed reaction kinetics region (CO removal process is controlled by mass transfer rate).

17

Keywords: Carbon monoxide; ·OH oxidation; new Fenton systems; synergistic activation; mass transfer-reaction

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1. Introduction

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With the continuous expansion of urban population, the treatment of solid wastes such as domestic refuse,

20

sludge, medical waste, etc. has become a major problem in urban development.1,2 Incineration has become an

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important development direction of solid wastes treatment because of its advantages in volume reduction and

22

*Contact

information: Tel., +86-0511-88780012; Fax, +86-0511-88780012; E-mail: [email protected] (X.Y. Liu)

1

ACS Paragon Plus Environment


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energy recovery.1,2 However, various gaseous pollutants, mainly including sulfur dioxide, nitrogen oxides,

24

hydrogen chloride, mercury, carbon dioxide, carbon monoxide, dioxine, particulate matter, etc., will be produced

25

in the combustion process of solid wastes.3-16 At present, these pollutants are mainly controlled using complex

26

combined processes (e.g, SNCR/SCR denitration + acid gases absorption +activated carbon adsorption + dust

27

removal, etc.).16,17

28

CO has serious harmful effect on the environment and health because it is colorless, tasteless and highly

29

toxic.16,17 In 2014, China's Ministry of Environmental Protection has released the ‘Standards for Pollution Control

30

of Domestic Waste Incineration (GB 18485-2014)’ to control the emission of CO from combustion process of

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solid wastes.17,18 From a theoretical point of view, combustion is a feasible way to reduce emission of carbon

32

monoxide, but combustion treatment will be very expensive because of the very low concentration of carbon

33

monoxide in flue gas (it's often only tens to hundreds of ppm).16,17 Recently, some studies on separation of CO

34

from waste gas have been carried out.16,17 Based on the difference of separation principle, the separation

35

techniques of CO from waste gas mainly include two ways (e.g., dry and wet).16,17,18 Representative dry way

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generally involves adsorption, photo-catalysis, plasma elimination, catalytic degradation, etc.6-28 Representative

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wet way generally contains ionic liquid absorption, complex absorption, oxidation scrubbing, etc.19-22 These CO

38

separation methods still have a variety of defects (e.g, low removal efficiency, high cost, pipeline corrosion, poor

39

security, or secondary pollution trouble).16,17 Therefore, it is very necessary to develop new separation

40

technologies of CO from waste gas.

41

Fenton-based oxidation technologies have obtained extensive research in remediation of pollutants from

42

various exhaust gas and wastewater because of simple and cleaning process.33 However, the development of

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traditional Fenton-based oxidation technologies is limited due to poor free radical yield.33 Our recent works found

44

that adding trace Cu2+ or Mn2+ into traditional Fenton reagent could effectively elevate the free radical yield, and

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enhance the oxidation capacity of traditional Fenton reagent. In addition, many industrial processes (e.g., chemical

46

plants or power plants) will discharge containing-trace Cu2+ and Mn2+ industrial wastewater.34-38 The "Hygienic

47

Standard for Drinking Water" (GB5749-85) and “Comprehensive Wastewater Discharge Standard (GB

48

8978-1996)” promulgated by the Chinese Government stipulate that manganese and copper contents in

49

wastewater must be less than 2.0 mg/L. Hence, it will be also a very valuable exploration that trying to use Cu2+

50

and Mn2+-containing industrial wastewater to strengthen the oxidation absorption of CO from tail gas in

51

traditional Fenton system.

52

Related researchers39-41 indicated that simultaneous removal processes of multi-pollutants from exhaust gas

53

(e.g, SO2, NOx, CO, H2S, Hg0 and VOCs) have more obvious advantages such as simple process and low

54

expenses than the united treating systems (e.g, SNCR/SCR denitration + acid gases absorption process +activated

55

carbon adsorption + dust removal, etc.). In the waste gas treatment area, various Fenton-based oxidation systems

56

had been applied to simultaneously eliminate SO2, NO, H2S, Hg0 and VOCs from gas, and achieved good

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simultaneous removal performance of multi-pollutants.42-48 This article aims to explore for the first time the

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oxidation absorption of CO in flue gas using two new Fenton systems (i.e. Cu2+/Fe2+ and Mn2+/Fe2+ co-activated

59

H2O2 systems).

60

In addition, bubble column reactor and spray reactor are the gas-liquid reactors that are widely studied and

61

used in the field of flue gas treatment. Compared with the spray reactor, the bubble column reactor is often more

62

suitable for these flue gas treatment processes that the reaction processes will produce bubbles (the Fenton reagent

63

will produce many bubbles, which will affect the good atomization of the solution). Hence, the bubble column

64

reactor is chosen as the gas-liquid reactor in this article. The research contents mainly involve the technological

65

influencing factors, mechanism and mass transfer-reaction kinetics of CO absorption using two new Fenton

66

systems in a bubble column reactor. The developed novel processes and obtained results will provide valuable

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guidance for emission reduction of CO and multi-pollutants from waste incineration flue gas, and recycling of

68

Cu2+ and Mn2+ from containing-Cu2+ and Mn2+ industrial wastewater.

69

2. Experimental

70

2.1 Experimental setup

71

Figure 1 demonstrates the flow-process diagram of experimental setup used in this work, which includes the

72

several key sub-devices as below: (1) A CO-containing artificial gas blending system with six cylinders (mainly

73

including CO, SO2, CO2, NO, N2 and O2) and a Hg0 vapor generator, a mixer, six fluid meters, and two gas valves

74

for gases; (2) A temperature control unit that has a thermocouple and a water bath with constant temperature

75

function; (3) A corrosion resistant glass bubbling reactor, mainly comprising a reactor cover (rubber plug) and a

76

bubbling device (i.e., a fritted glass bubbler, and the sieve plate apertures of bubbler are about 20-60 micron). The

77

height and diameter of the gas-liquid absorber are 300 mm and 90 mm; (4) An analytical and tail purification unit,

78

mainly including a tail gas analyzer (with five sensors such as O2, CO2, SO2, NO and CO), a mercury analyzer

79

(Qing'an Instrument in Suzhou, China) and an exhaust absorber.

80

2.2 Experimental flow and means

81

CO, N2, NO, CO2, Hg0, SO2 and O2 simulation exhaust gas (0.15 L/min, which corresponds to the gas flow

82

velocities of the empty bubble column of 0.04 cm/s) was produced based on the high pure gases of CO, N2, NO,

83

CO2, SO2 and O2 from cylinders gases and Hg0 vapor generator. The concentrations of CO were monitored using

84

an exhaust gas analyzer. 0.5 L of modified Fenton reagents (i.e., Mn2+/Fe2+/H2O2 and Cu2+/Fe2+/H2O2,

85

respectively) were produced using commercial reagents (MnCl2·4H2O, FeCl2·4H2O, CuCl2·2H2O, and H2O2,

86

analytically pure agent) and deionized H2O. The reagent pH value of modified Fenton reagents was changed

87

through acid-base solutions (the acidometer with detection limit of 0.1 was used to measure the reagent pH value).

88

Then one of modified Fenton reagents was moved to the absorber. The set values of the temperatures of modified

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89

Fenton reagents were adjusted based on a temperature water and a thermocouple. The CO, N2, CO2, NO, Hg0, SO2

90

and O2 simulation exhaust gas entered the absorber to conduct a washing reaction via switching the valves on the

91

main and bypass lines. The exit concentration of CO was also monitored via an exhaust gas analyzer, and the

92

average concentration during an experimental period was used as the outlet concentration of CO.

93

Figure 1. Experimental setup flow-process diagram

94 95

2.3 Characterization methods

96

ESR characterization technique (ESP-300) was applied to measure hydroxyl radicals based on the used

97

method in the literatures.49-51 The important liquid ions, CO32-, HCO3-, SO42-, SO32-, NO3- and NO2- had been

98

measured using acid-base titration method (GB/T 11064.12-2013) and chromatography of ions (Dionex from

99

USA; Model: ICS-1600).49-51 The concentrations of mercury in reaction solutions were analyzed using liquid

100

fluorescence mercury analyzer.52,53 The CO2 in gas phase had been measured by a high precision carbon dioxide

101

analyzer (the resolution is up to 0.1 ppm). Concentrations of ferrous ions and ferric ions in solutions were

102

determined using o-phenanthroline spectrophotography (Uniko (Shanghai) Instruments Co., Ltd.; UV-2000). 5



103 104

105

106 107 108

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2.4 Removal efficiencies and removal rates of CO The efficiencies of CO removal are calculated using the formula (1):

Efficiency of CO removal 

Cin ,CO  Cout ,CO  100% Cin ,CO

(1)

In the formula (1), Cin , CO and Cout , CO are respectively the inlet and exit concentrations of CO. The removal rates of CO are calculated using the formula (2):52-54

N CO  (CO  CCO ,in  QG ) /(60  M CO  aCO  VL )

(2)

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In the formula, N CO represents the removal rate of CO, mol / m  s ;CO represents the removing efficiency

110

of CO, %; CCO , in represents the inlet concentration of CO, mg/m3; QG represents the total flow rate of

111

simulated exhaust gas, L / min ; M CO represents the molecular weight of CO, g/mol ; VL represents the

112

solution volume in absorber, L ; aCO represents the specific interfacial area of CO, m2/m3.

113

3. Results and discussions

114

3.1 Effect of H2O2 concentration on removal efficiency and removal rate of CO

2

115

Figure 2(a) reveals the effect of H2O2 concentration on removal efficiency and removal rate of CO in two

116

new Fenton systems. Result reveals that in two new Fenton systems, as the concentration of H2O2 rises from 0 to

117

1.5 mol/L, both of the removal efficiency and removal rate of CO firstly rise and then drop. The maximum

118

removing efficiencies are 95.8% and 85.1% for Cu2+-modified and Mn2+-modified new Fenton systems. Both of

119

the optimized values of H2O2 concentrations are 0.8 mol/L for the two new Fenton systems.

120 121

Many studies have confirmed that Fe2+ could effectively catalyze H2O2 to form ·OH with strong oxidation ability through the formulas (3)-(5) as below.42,43,46

122

H 2O 2  Fe2   OH  Fe3  OH 

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H 2O 2  Fe3  H   [Fe(HO2 )]2 

k  1.0  102 M 1s 1

(4)

124

[Fe(HO2 )]2   HO 2   Fe2 

k  2.7  103 M 1s 1

(5)

6


k  63 M 1s 1

(3)

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The produced ·OH is able to effectively oxidize CO to produce bicarbonate, carbonic acid and/or carbon dioxide

126

(the type and concentration of the specific products depend on the reagent pH value), with large rate constants,

127

according to the formulas (6)-(11) as below.16,17,32,55-57

k  2.0  109 M 1s 1

 OH  CO   CO 2 H

128

(6)

129

 CO 2 H  H 2O 2  H 2CO3  OH

(7)

130

 CO 2 H   OH  H 2CO3

(8)

131

 CO 2 H   CO 2 H  H 2CO3  CO 

(9)

132

H 2CO3  CO 2   H 2O

(10)

133

H 2CO3  HCO3-  H 

(11)

134

Based on the above formulas (3)-(11), a rise of H2O2 dosage will elevate the yield of ·OH, being beneficial to CO

135

absorption. Hence, the appropriate rise of H2O2 concentration has a large promoting role for the removal of CO in

136

the two new Fenton systems.

137

Nevertheless, an excess addition of H2O2 would lead to the consumption of ·OH based on the side reactions

138

described in the formulas (12)-(16).42-49 The formulas (12)-(15) for chemical reactions have large reaction rates,

139

which are harmful for the removal of CO by consuming ·OH.39,42,43,45

k  2.7  107 M 1 s 1

140

H 2O 2  HO  HO 2   H 2O

141

HO   HO   H 2O 2

142

HO 2   HO 2   H 2O 2  O 2 

143

HO   HO 2   H 2O  O 2 

144

H 2O 2  HO 2   HO   H 2O 2  O 2 

k  4.2  109 M 1 s 1 k  8.3  105 M 1 s 1 k  1.0  1010 M 1 s 1 k  5.0  101 M 1 s 1

(12) (13) (14) (15) (16)

145

Consequently, H2O2 dosage shows a double role on the CO removal, and 0.8 mol/L is found to be the optimized

146

value of H2O2 concentration in the two new Fenton systems.

7



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3.2 Effect of Fe2+ concentrations on removal efficiency and removal rate of CO

148

Figure 2(b) exhibits the effect of Fe2+ concentrations on removal efficiency and removal rate of CO in two

149

new Fenton systems. The results show that as the concentration of Fe2+ rises from 0 to 0.16 mol/L, CO removing

150

efficiency substantially and respectively increases from 15.8% to 98.6% for Cu2+-modified new Fenton system,

151

and from 2.7% to 88.6% for Mn2+-modified new Fenton system (CO removal rates also increase in the two new

152

Fenton systems). Based on the front formulas (3)-(5), the rise of Fe2+ dosage will substantially improve the yield

153

of ·OH by accelerating the rates of chemical reactions, being beneficial to removing CO. Hence, raising the Fe2+

154

concentration has a large promoting role for the removal of CO in two new Fenton systems.

155

156

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Figure 2. Effect of technological parameters on removal efficiency and removal rate of CO : concentrations of

159

H2O2 (a) and Fe2+ (b); reagent pH value (c); concentrations of Mn2+ and Cu2+ (d); ); reaction temperature (e).

160

Benchmark test conditions: H2O2 concentrations of 0.8 mol/L; Fe2+ concentration of 0.1 mol/L; pH value of

161

3.01; Cu2+/Mn2+ concentration of 0.008 mol/L; Temperatures of 308 K (Cu2+) and 318 K (Mn2+); inlet

162

concentration of CO of 150 ppm; NO concentration of 400 ppm; SO2 concentration of 1000 ppm; CO2

163

concentration of 12%; Hg0 concentration of 60 μg/m3.

164

3.3 Effect of solution pH value on removal efficiency and removal rate of CO

165

Figure 2(c) exhibits the effect of reagent pH value on removal efficiency and removal rate of CO. Result

166

finds that with raising the pH value of reagent from 1.01 to 9.25, the removal efficiency and removal rate of CO

167

first rise and then reduce in the two new Fenton systems. Both of the optimal reagent pH values are 3.01. It can be

168

observed from the formulas (4) and (6)-(11), high concentration H+ (low pH) will hinder these reactions, and thus

169

are not conducive to the removal of CO. Hence, the appropriate rise of the reagent pH value will availably

170

promote the removal of CO in the two new Fenton systems.

171

Nevertheless, ·OH would be consumed based on the quenching reaction of free radicals, which is described

172

in the equation (17) (its rate constant is 1.3  10 M s , and the O·- has far lower oxidative potential

173

than ·OH).58-61 Consequently, too high reagent pH value will hinder the removal of CO.

174

1 1

10

 OH  OH -  H 2O  O - 

k  1.3  1010 M 1 s 1

9


(17)


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175

Furthermore, transition metal ions can easily form the precipitations in alkaline mediums via reacting with

176

OH-, which can be described by the general equation (18) as below (Cu2+, Fe2+ and Mn2+ in solutions will begin to

177

precipitate in the pH values of 4.2, 5.9 and 8.8, respectively, and completely precipitate in the pH values of 6.7,

178

8.4 and 10.8 respectively).48,53,62,63

M 2   2OH -  M(OH)2  M  (Cu 2  , Fe 2  , Mn 2  )

179

(18)

180

High reagent pH value will lead to the consumption of Cu2+, Mn2+ and Fe2+, being not conducive for the CO

181

removal. Hence, in this work, the reagent pH value shows a dual influence on the removal of CO.

182

3.4 Effect of Mn2+/Cu2+ concentrations on removal efficiency and removal rate of CO

183

Figure 2(d) exhibits the effect of Mn2+ and Cu2+ concentrations on removal efficiency and removal rate of

184

CO. Result shows that with raising the concentrations of Mn2+ and Cu2+ from 0 to 0.012 mol/L, the CO removing

185

efficiencies and removal rates clearly increase. Both Mn2+ and Cu2+ could also catalyze H2O2 to form ·OH to

186

oxidize CO, which can be described via the formulas (19)-(22) as follows.33,37,38,48

187

Cu 2   H 2O 2  Cu   H   HO 2 

(19)

188

Cu   H 2O 2  Cu 2   OH  OH 

(20)

189

Mn 2   H 2O 2  Mn 3  OH  OH 

(21)

190

Mn 3  H 2O 2  Mn 2   HO 2   H 

(22)

191

In addition, both Mn2+ and Cu2+ could enhance the Fenton reaction through strengthening the conversion of

192

Fe3+ and Fe2+ (it has been proved by the results in Figure 4e). The above formulas (4) and (5) (conversion of Fe3+

193

and Fe2+) had been widely confirmed to be the leading rate controlling steps of Fenton reaction system (their rate

194

constants are only 3.1  10 M s and 2.7  10 M s , respectively).33,35,37 Addition of Cu2+ and Mn2+

195

could availably accelerate the conversion rate of Fe3+ and Fe2+ (see Figure 4(e)), which will be beneficial to

196

increase the yield of hydroxyl radicals (see Figure 4(d)), and thus was able to effectively strengthen the CO

-3

1 1

-1

1 1

10


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removal in the two new Fenton systems.

198

3.5 Effect of temperature on removal efficiency and removal rate of CO

199

Figure 2(e) exhibits the effect of temperature on removal efficiency and removal rate of CO in two new

200

Fenton systems. As the reacting temperature increases, the CO removing efficiencies and removal rates first rise,

201

and then drop (308 K is the best temperature for CO removal efficiency and 338 K is the best temperature for CO

202

removal rate in Cu2+-modified new Fenton system; 318 K is the best temperature for CO removal efficiency and

203

328 K is the best temperature for CO removal rate in Mn2+-modified new Fenton system). Related researchers64,65

204

suggest that the reaction rates (eg., those of Eqs. (3)-(11) and (19)-(22)) will be elevated by the rise of temperature,

205

thereby being able to improve the removal of CO. But some investigators66-68 also had pointed out that raising

206

temperature would cause a decline of solubility of CO in liquid phase. The drop of solubility of CO in liquid

207

phase would elevate the resistance of CO mass transfer on phase interface, which would hinder removal of CO.

208

Thus, reacting temperature exhibits double effect on removing of CO in the two new Fenton systems.

209

3.6 Effect of CO/NO/CO2/Hg0/O2/SO2 concentrations on removal efficiency and removal rate of CO

210

For different incineration systems and operational conditions, the concentrations of the main exhaust gas

211

pollutants such as CO, NO, CO2, Hg0, O2 and SO2 in waste incineration exhaust gas significantly change.68,69 It is

212

very necessary to explore the effect of the changes of exhaust gas component concentrations on CO absorption in

213

the two new Fenton systems. Results have been given in Figure 3(a)-(f).

214

It has been observed that with the rise of CO inlet concentration, CO removing efficiencies decrease, but CO

215

removal rates almost has a linear increase. That is because a rise in CO inlet concentration will elevate the total

216

amount of CO through the absorber (actually, it will drop the ratio between H2O2 and ·OH to CO), which is

217

unfavorable to the removal of CO. However, the rise of CO inlet concentration will increase the CO partial

218

pressure in gas phase main body, which will raise the mass transfer driving force, and thus is able to increase the

11



219

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CO removal reaction rates.

220

With the rise of the concentrations of NO and SO2, all CO removing efficiencies and removal rates clearly

221

drop in the two new Fenton systems. Relevant research shows that both NO and SO2 could react with ·OH, which

222

could be expressed through the following E.q.s (23)-(28).50,51,66-68 Hence, the rise of NO and SO2 concentrations

223

restrains the oxidation removal of CO. In addition, the present results show that SO2 has a greater effect on the

224

removal of CO than NO. This is because SO2 is more soluble in water than NO.50,51 Therefore, SO2 in the liquid

225

phase will have a smaller mass transfer resistance, thus achieving a higher liquid concentration.50,51 From the point

226

of view of chemical reaction, a higher liquid concentration will effectively promote the chemical reaction. Hence,

227

under the same conditions, SO2 is more likely to consume oxidants in the liquid phase, so it usually has a greater

228

impact on removal of target pollutants.

229

 OH  NO  HNO 2

(23)

230

 OH  HNO 2  HNO3  H

(24)

231

H 2O  SO 2  HSO3  H 

(25)

232

HSO3-  H   SO32 

(26)

233

 OH  HSO3-  H 2O  SO3

(27)

234

 OH  SO32 -  OH -  SO3

(28)

235

With the change of the concentrations of CO2, Hg0 and O2, CO removing efficiencies and removal rates remained

236

almost unchanged. The contensts of CO2 and O2 often reach 10-15% and 4-7%, respectively.69,70 This shows that

237

the new removal technology can have a good adaptability to the changes of flue gas component concentrations.

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238

239

240 241

Figure 3. Effect of technological parameters on removal efficiency and removal rate of CO: (a) CO

242

concentrations; (b) NO concentrations; (c) SO2 concentrations; (d) CO2 concentrations; (e) O2 concentrations; (f)

243

Hg0 concentrations. The benchmark test conditions are same as those under the title of Figure 2.

244

3.7 Routes and mechanism of CO absorption in two new Fenton systems

245

The comparing data of CO removing efficiencies in several absorption systems had been depicted in Figure

246

4 (a). As depicted in Figure 4 (a), as contrast, all H2O (A), H2O/Cu2+ (B), H2O/Mn2+ (C), H2O/Fe2+ (D) and H2O2 13



Page 14 of 26

247

(E) five removal systems can not eliminate CO. From the Figure 4 (c), H2O (A), H2O/Cu2+ (B), H2O/Mn2+ (C),

248

H2O/Fe2+ (D) and H2O (E) five removal systems can not produce any radical signals. The result proves that CO

249

can not be removed by oxidation of H2O2 and absorption of Cu2+, Mn2+, Fe2+ or/and H2O.

250

However, it is seen from the Figure 4 (b) and (c), explicit hydroxyl radical signals63,67,71 were found via ESR

251

spectrometer in Fe2+/H2O2 (F), Cu2+/H2O2 (G), Mn2+/H2O2 (H), Cu2+-based new Fenton system (I) and Mn2+-

252

based new Fenton system (J). As indicated in the Figure 4 (a), Fe2+/H2O2 (F), Cu2+/H2O2 (G) and Mn2+/H2O2 (H)

253

three removal systems attain CO removing efficiencies of 60.2%, 15.8% and 2.7%, respectively. The CO

254

eliminated is mainly oxidized by ·OH that is generated by Fe2+/H2O2 (F), Cu2+/H2O2 (G) and Mn2+/H2O2 (H) (as

255

described in the equations (3)-(10) and (19)-(22)).

256

After Mn2+ or Cu2+ (0.008 mol/L) was supplemented into the Fenton (Fe2+/H2O2) system, the CO removing

257

efficiencies remarkably rise to 85.1% in Mn2+-based new Fenton system, and to 95.8% in Cu2+-based new Fenton

258

system, respectively. As the contrast, the CO removing efficiencies in Mn2+/H2O2 and Cu2+/H2O2 are only

259

respectively 2.7% and 15.8%. Compared with the CO removing efficiency of 60.2% in Fenton (Fe2+/H2O2), and

260

the CO removing efficiencies of 2.7% and 15.8% in Mn2+/H2O2 and Cu2+/H2O2, the new increasing of CO

261

removing efficiencies (22.2% = [85.1% - 60.2% - 2.7%] and 19.8% = [95.8% - 60.2% - 15.8%]) in Mn2+-based

262

and Cu2+-based new Fenton systems are obtained.

263

To verify the synergistic effect of multi-ions in the two new Fenton systems. The concentration changes of

264

Fe2+ and Fe3+ and the yields of ·OH in several contrast systems were measured, and the results are shown in

265

Figure 4 (d) and (e). As shown in the Figure 4 (e), the concentrations of Fe2+ in the two new Fenton systems are

266

significantly higher than those in the Fenton (Fe2+/H2O2) system. And the concentrations of Fe3+ in the two new

267

Fenton systems are significantly lower than those in Fenton (Fe2+/H2O2) system. As shown in the Figure 4(f), it

268

can be seen that in the two new Fenton systems, the CO removing efficiencies with running time maintain better

14


Page 15 of 26


269

stability as compared with those in the Fenton (Fe2+/H2O2) system. As shown in the Figure 4 (d), the ·OH yields in

270

the two new Fenton systems are higher than the sum of the ·OH yields in independent systems (Fenton +

271

Mn2+/H2O2 and Fenton + Cu2+/H2O2). The above comparison results well show that the synergistic activation

272

effect of multi-ions exist in the two new Fenton systems, which is favorable for the CO removal.

273

In addition, by comparing with the CO removing efficiencies and the yields of ·OH in several systems, it

274

can be inferred that CO is mainly removed by ·OH oxidation in the two new Fenton systems, and can be divided

275

into three reaction pathways: (1) CO removal by ·OH from Fenton (Fe2+/H2O2) system; (2) CO removal by ·OH

276

from Cu2+/H2O2 system or CO removal by ·OH from Mn2+/H2O system; (3) CO removal by ·OH from the

277

synergistic activating role of Mn2+/Fe2+ and Cu2+/Fe2+ in the new Fenton systems.

278

To further verify the above discussion of CO removing mechanism, the products of CO removal were

279

analyzed, and the calculation of total carbon balance was also carried out (it is worth noting that when CO

280

removal products were analyzed, CO2 was not included in the simulated flue gas). The detection results of liquid

281

and gaseous reaction products under acidic conditions proved that bicarbonate were produced in reaction solution,

282

and carbon dioxide was produced in the tail gas. The calculation results of total carbon balance show that the

283

calculated and measured values are in basically good agreement, which further proved that carbon monoxide from

284

gas is mainly removed based on a series of the mentioned-above oxidative reactions. In addition, to evaluate the

285

post-treatment practicability of multi-pollutants simultaneous removal products (an experiment on simultaneous

286

removal efficiency of multi-pollutants such as CO, SO2, NO, Hg0 can be seen in the Figure S1), the removal

287

products of the other pollutants such as SO2, NO, Hg0 were also determined. The results are also shown in Table 1.

288

The relevant removal process flow and post-processing discussions of products can be found from the Support

289

Information (Section 2). The synergistic mechanism and reaction routes of CO removing can be expressed via the

290

Fig. 5 as below.

15



291

Page 16 of 26

Table 1. Removal products and total carbon balance for CO in the two new Fenton systems

Cu2+-new Fenton system

CO32-

HCO3-

CO2

Total carbon

SO42- mg/L

NO3-

SO32-

NO2-

Hg2+μg/L

Measured mass (mmol)

～

0.004

0.009

0.013

18.92

4.51

～

～

0.26

Calculated value (mmol)

～

～

～

0.015

～

～

～

～

～

Total carbon error (%)

～

～

～

13.3%

～

～

～

～

～

CO32-

HCO3-

CO2

SO42- mg/L

NO3-

SO32-

NO2-

Hg2+μg/L

Measured mass (mmol)

～

0.003

0.008

0.011

18.10

4.19

～

～

0.22

Calculated value (mmol)

～

～

～

0.013

～

～

～

～

～

Total carbon error (%)

～

～

～

15.4%

～

～

～

～

～

Mn2+-new Fenton system

Total carbon

292

293

294

16


Page 17 of 26


295 296

Figure 4. (a) Comparing results of CO removing efficiencies in several removal systems; (b) ESR spectrums

297

of ·OH in Cu2+-based new Fenton system; (c) ESR spectrums of ·OH in Mn2+-based new Fenton system; (d)

298

Comparing results of ·OH yield in several removal systems; (e) Concentration changes of Fe2+/Fe3+ in several

299

comparing systems; (f) CO removing efficiencies with running time in several removal systems. The benchmark

300

test parameters are same as those under the title of Figure 2.

301

302 303 304

Figrue 5. CO removal mechanism using two new Fenton systems 3.8 Removal kinetics of CO

305

As a heterogeneous reaction that involves gas-liquid two-phases, revealing the mass transfer-reaction kinetic

306

law and obtaining the mass transfer and kinetic parameters (removal rate, rate constant and Hatta coefficient) are

17



Page 18 of 26

307

the key works for further strengthening the CO removal, and optimizing design of reactor. Based on the results of

308

CO removal mechanism and products, the total reaction of CO removal can be described by the following

309

equation (29):

310

a CO  b H 2O 2  cFe2   dM 2    e (HCO3- / CO 2 )  f Other by - products

311

where a,b,c,d,e and f are the stoichiometric coefficients for CO, H2O2, Fe2+, M2+ (Cu2+ or Mn2+) , HCO3-/CO2 and

312

by-products, respectively.

313 314

(29)

The intrinsic rate equation of CO removal using two new Fenton systems can be expressed as the following equation (30):53,54,71-73 mx nx hx jx rCO , x  km x , n x ,i x , j x  CCO , i , x  C H 2 O2 , x  C Fe 2 , x  C M 2 , x

315

(30)

316

where rCO , x is the chemical reaction rate of CO, mol /( L  s ) ; k m x , n x , h x , j x is the pseudo-(mx+nx+hx+jx)-order

317

reaction rate constant for the total reaction (30), L

318

interface concentration,

319

mol / L ; CMj x 2 , x is Cu2+ or Mn2+ concentration, mol / L ; mx , nx hx and jx are the partial reaction order for CO,

320

H2O2, Fe2+ and M2+, respectively; x is Cu2+ or Mn2+ (Cu2+ represents Cu2+-based new Fenton system, and Mn2+

321

represents Mn2+-based new Fenton system).

( m x  n x  h x  j x 1)

 mol (1 m x  n x  hx  j x )  s 1 ; CCO ,i , x is CO

mol / L ; CH 2 O2 , x is H2O2 concentration,

hx is Fe2+ concentration, mol / L ; CFe 2 ,x

322

The concentration of CO in liquid phase, CCO , i , x , is the order of magnitude of 10-8. The concentrations of

323

H2O2, Fe2+ and M2+ are the orders of magnitude of 10-1, 10-2, 10-3, respectively, and thus all of them can be

324

recognized as the constants in a short period of time.53,54,71-73 Thus the above equation (30) can be further reduced

325

to the equation (31): mx rCO , x  km x  CCO ,i , x

326

(31)

327

where k m x  k n x , h x , j x  CHx2 O2  CFex 2 , x  CMx 2 , x represents pseudo-mx-order reaction rate constant for CO in the

328

Cu2+-based and Mn2+-based new Fenton systems, L

n

h

j

,x

( m x 1)

 mol (1 m x )  s 1 .

18


Page 19 of 26


329

Based on the intrinsic rate equation (31), the double-film theory and the results of the other

330

researchers,53,54,71-73 for a fast reaction, the removal rate of CO in solution can be described by the following

331

equation (32): 1/ 2

N CO , x

332

m x 1  2 DCO , L , x  km x  CCO  ,i , x      m  1 x  

(32)

333

where N CO , x is the CO removal rate, mol / m  s ; DCO , L , x is the liquid phase diffusion coefficient of CO,

334

respectively, m / s .

335 336 337

2

2

In the equation (32), N CO , x can be calculated by the equation (2). CO interface concentration, CCO , i , x , can be calculated by the following equation (33):53,54,71-73

CCO ,i , x  H CO , L , x ( pCO ,G , x  N CO , x kCO ,G , x )

(33)

338

where H CO , L , x is the solubility coefficient of CO in solution, mol /( L  Pa ) ; pCO , G , x is CO partial pressure in gas

339

phase body, Pa ; kCO , G , x is CO gas phase mass transfer coefficient, mol / s  m  Pa . 2

340

In the formulas (32) and (33), H CO , L , x was calculated via the methods in references;73-76 DCO , L , x was

341

calculated basing on Wilke-Chang correlation formula.73-76 aCO , x , kCO , G , x and kCO , L , x were obtained basing on

342

Danckwerts plot model and chemical absorption approach.73-76 In addition, in order to determine mx value in the

343

equation (32), a series of data processing and deduction processes were performed. The described processes and

344

methods can be found in Support information. The key mass transfer and kinetic parameters such as removal rate,

345

quasi-first-order rate constant, and Hatta coefficient are summarized in Table 2.

346

From the Table 2, the data indicate that all the Hatta coefficients are very large and far greater than 3.0,

347

excepting for these zero points (at this time, the chemical reaction enhancement factor E  Ha ). It shows that the

348

chemical reaction rate is far larger than mass transfer rate, and thus the mass transfer has been proved to be the

349

rate control step of CO removal in the two new Fenton systems.73-76 Thus, CO removal can be elevated via the rise

350

of mass transfer. The mass transfer and kinetic data in Table 2 and Table S1 can provide an important support for 19



Page 20 of 26

the amplification and design of reactor and numerical simulation of CO removal in the two new Fenton systems.

351

Table 2. Mass transfer-reaction kinetic parameters of CO removal

352

Removal systems

Cu2+ based-new Fenton system

Mn2+ based- new Fenton system

→

N CO ,Cu  106

kmCu  105

s 1

s 1

0

0

0

0

0

0

0.05

1.10

0.66

199.6

199.6

0.1 0.3 0.5 0.8 1.1 1.5 0 0.005 0.02 0.04 0.07 0.1 0.16 1.01 3.01 5.64 7.29 9.25 0 0.001 0.002 0.003 0.005 0.008 0.012

1.87 2.27 2.42 2.45 2.39 2.24 0.40 1.08 1.58 2.07 2.32 2.45 2.52 2.36 2.45 2.28 1.97 1.07 1.54 1.93 2.15 2.28 2.36 2.45 2.52

1.92 2.82 3.21 3.29 3.13 2.75 0.09 0.64 1.37 2.35 2.95 3.29 3.48 3.05 3.29 2.85 2.13 0.63 1.30 2.04 2.53 2.85 3.05 3.29 3.48

340.4 412.5 440.1 445.6 434.6 407.4 73.7 196.5 287.5 376.6 421.9 445.6 458.3 429.0 445.6 414.7 358.5 195.0 280.1 350.9 390.7 414.7 429.0 445.6 458.3

298

1.94

1.93

353.4

Studied parameters

HaCu

ECu

N CO , Mn  106

kmMa  105

HaMn

EMn

0

0

0

0.69

0.28

124.5

124.5

340.4 412.5 440.1 445.6 434.6 407.4 73.7 196.5 287.5 376.6 421.9 445.6 458.3 429.0 445.6 414.7 358.5 195.0 280.1 350.9 390.7 414.7 429.0 445.6 458.3

1.35 1.76 1.84 2.00 1.96 1.80 0.06 0.75 1.06 1.49 1.80 2.00 2.08 1.93 2.00 1.92 1.72 1.20 1.41 1.50 1.67 1.92 1.99 2.00 2.04

1.08 1.84 2.01 2.38 2.28 1.93 0.00 0.33 0.67 1.32 1.93 2.38 2.57 2.21 2.38 2.19 1.76 0.86 1.18 1.34 1.66 2.19 2.35 2.38 2.47

244.6 319.2 333.7 363.1 355.4 326.9 0 135.2 192.6 270.4 326.9 363.1 377.3 349.9 363.1 348.3 312.2 218.2 255.6 272.4 303.2 348.3 360.8 363.1 369.9

244.6 319.2 333.7 363.1 355.4 326.9 0 135.2 192.6 270.4 326.9 363.1 377.3 349.9 363.1 348.3 312.2 218.2 255.6 272.4 303.2 348.3 360.8 363.1 369.9

353.4

1.60

1.33

258.1

258.1

s 1

s 1

↓ CH2O2 (mol/L)

CFe2+ (mol/L)

Solution pH

CM2+ (mol/L)

Solution temperature (K)

20


Page 21 of 26

CCO (ppm)

CSO2 (ppm)

CNO (ppm)

CO2 (%)

CCO2 (%)

CHg0 (μg/m3)


308 318 328 338 348 50 100 150 200 250 300 200 500 1000 1500 2000 2500 200 400 600 800 1000 1200 0 2 5 7 9 0 2 6 9 12 16 0 15 25 50 80

2.46 2.58 2.71 2.87 2.78 0.76 1.65 2.46 3.14 3.79 4.41 2.53 2.48 2.45 2.40 2.27 2.10 2.51 2.45 2.43 2.40 2.37 2.31 2.44 2.43 2.45 2.48 2.48 2.46 2.43 2.44 2.42 2.45 2.41 2.44 2.43 2.43 2.45 2.47

3.32 3.55 3.73 3.79 3.02 3.45 3.29 3.20 2.76 2.41 2.05 3.51 3.37 3.29 3.16 2.82 2.42 3.45 3.29 3.24 3.16 3.08 2.92 3.26 3.24 3.29 3.37 3.37 3.32 3.24 3.26 3.21 3.29 3.20 3.26 3.24 3.24 3.29 3.34

447.6 454.1 471.1 485.7 442.0 456.3 445.6 439.4 408.1 381.4 351.7 460.2 451.0 445.6 436.7 412.5 382.1 456.3 445.6 442.2 436.7 431.1 419.8 443.5 442.2 445.6 451.0 451.0 447.6 442.2 443.5 440.1 445.6 440.0 443.5 442.2 442.2 445.6 448.9

447.6 454.1 471.1 485.7 442.0 456.3 445.6 439.4 408.1 381.4 351.7 460.2 451.0 445.6 436.7 412.5 382.1 456.3 445.6 442.2 436.7 431.1 419.8 443.5 442.2 445.6 451.0 451.0 447.6 442.2 443.5 440.1 445.6 440.0 443.5 442.2 442.2 445.6 448.9

353 354

■ ASSOCIATED CONTENT

355

*S Supporting Information 21


1.87 2.00 2.26 2.24 2.23 0.63 1.38 2 2.55 3.19 3.78 2.13 2.07 2.00 1.95 1.80 1.74 2.03 2.00 1.98 1.95 1.92 1.88 2.00 1.98 2.00 2.02 2.02 2.01 1.98 2.00 1.97 2.00 1.99 2.01 1.98 2.02 2.00 2.03

1.88 2.38 2.67 2.34 1.97 2.35 2.26 2.12 1.92 1.66 1.29 2.70 2.55 2.38 2.26 1.93 1.80 2.45 2.38 2.33 2.26 2.19 2.10 2.38 2.33 2.38 2.42 2.42 2.40 2.33 2.38 2.31 2.38 2.36 2.40 2.33 2.42 2.38 2.45

313.3 363.1 372.1 344.5 316.2 366.4 359.3 348.0 331.2 308.0 271.5 386.7 375.8 363.1 353.8 326.9 315.7 368.4 363.1 359.2 353.8 348.3 341.0 363.1 359.2 363.1 366.1 366.1 364.6 359.2 363.1 357.7 363.2 362.1 364.6 359.2 366.1 363.1 368.4

313.3 363.1 372.1 344.5 316.2 366.4 359.3 348.0 331.2 308.0 271.5 386.7 375.8 363.1 353.8 326.9 315.7 368.4 363.1 359.2 353.8 348.3 341.0 363.1 359.2 363.1 366.1 366.1 364.6 359.2 363.1 357.7 363.2 362.1 364.6 359.2 366.1 363.1 368.4


Page 22 of 26

356

The Supporting Information is available free of charge on the

357

ACS Publications website at DOI:

358

Simultaneous removal of multi-pollutants from waste incineration flue gas (Text 1), process flow and removal

359

products processing strategy (Text 2), derivation/establishment of removal rate equation (Text 3), calculation and

360

measurement methods of physical and mass transfer parameters (Text 4). Simultaneous removal efficiency vs

361

running time of multi-pollutants (Figure S1), Simultaneous removal of multi-pollutants using new Fenton systems,

362

and a contrast with independent systems (Figure S2), Log(NCO,Cu) vs Log(CCO,i,Cu) (a) and Log(NCO,Mn) vs

363

Log(CCO,i,Mn) (b) (Figure S3). The diffusion coefficients, solubility coefficients and mass transfer parameters

364

(Table S1).

365

Acknowledgements This study was supported by National Natural Science Foundation of China (Nos. U1710108; 51576094),

366 367

Jiangsu ‘‘Six Personnel Peak” Talent-Funded Projects (GDZB-014).

368 369

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Removal of Carbon Monoxide from Simulated Flue ... - ACS Publications

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