本研究主要探討氫氣添加對汽柴油引擎污染排放減量之影響。實驗結果顯示， 0.6%及1.2%氫氣添加能提升柴油引擎制動熱效率且降低制動燃料消耗率。氫氣添加0.6%及1.2%能有效減少CO和CO2；而NOx排放係數呈現低負載減量中高負載增量趨勢，此乃因氫氣添加提升燃燒效率所致；隨著引擎負載增加THC排放係數分別增量約4.94%及13.1%。粒狀物排放仍因引擎缸內溫度有關，因此氫氣添加於怠速或低負載條件下對於粒狀污染物呈現增量趨勢。醛酮類化合物排放以甲醛，乙醛和丙酮為主要貢獻物種，占總醛酮類化合物79.2-87.2%。氫氣添加於低負載下對於甲醛排放係數減量約10.4%-10.9%，隨著負載增加25%-75%，甲醛減量分別約2.93-25.1%、5.91-25.8%及2.28-40.5%；其他醛酮類化合物(Carbonyl compounds)排放係數如丙烯醛，丙酮，丙醛，巴豆醛和2-丁酮和丁醛也呈相同減量趨勢。醛酮類化合物衍生之臭氧生成潛勢(Ozone formation potential)，隨著引擎負載增加，1.2%之氫氣輔助具有較佳之減量影響。多環芳香烴(Polycyclic aromatic hydrocarbons)主要在石化燃料或有機物經燃燒不完全環境條件下生成。本研究結果顯示，引擎負載25%、50%及75%，氫氣添加對於多環芳香烴排放分別減量56.4%、34.5%及27.9%；而PAHs之總毒性當量(TEF-BaPeq)隨著氫氣添加也呈現減量之影響。另，汽油引擎主要於美國聯邦測試程序(FTP-75)，添加不同比例之生質酒精及0.6 (L/min) 之氫氣輔助探討汽油引擎冷啟動燃油消耗及污染減量之影響。實驗結果顯示，冷啟動條件下E3、E6具有較佳之污染減量；而氫氣添加有助於改善燃油消耗使引擎燃燒更完全，且具有較佳的污染減量效果。此外，應用GREET model作為本研究燃油溫室氣體生命週期評估，從油井到油箱(well-to-tank)分析結果顯示，其占總生命週期溫室氣體排放之22.3%。生質酒精E10於氫氣輔助燃料添加下，油井到油箱（well-to-tank）有較低的溫室氣體排放(65.3 g CO2 -e/km)；但由於(tank-to-wheel)整體燃料消耗及燃油CO2排放之影響結果，以生質酒精E10呈現較低之溫室氣體排放，其減量約6.96%。

This study investigated hydrogen addition (using de-ionized as the hydrogen source) on diesel and gasoline internal combustion engines. The results show that hydrogen addition (0.6% and 1.2% by volume) lead to an increase of brake thermal efficiency and decrease brake specific fuel consumption on the diesel engine. The hydrogen addition leads to reduce the traditional emissions such as CO2 and CO, but THC increased 4.94% and 13.1% on average with the low level of hydrogen addition (0.6% and 1.2% by volume). Nevertheless, the addition of hydrogen lowered nitrogen oxide emissions at the idling and low load conditions but increased during the high load. Particulate matter formation mainly comes from incomplete combustion, especially during idle condition with lower cylinder temperature. However, hydrogen addition could decrease by 14.1%, 6.86% and 9.75% with the increase of during engine load (25, 50 and 75% engine load). Formaldehyde, acetaldehyde, and acetone contributed 79.2–87.2% of total carbonyl compounds which are the more prominent when the engine operated at low load. With 0.6 and 1.2 vol% of hydrogen addition, formaldehyde decreased 10.4–10.9% at idling condition. As the load increases 25, 50 and 75%, the formaldehyde decreased by 2.93–25.1, 5.91–25.8 and 2.28–40.5%, respectively. The same reduction phenomenon can also be observed from acrolein, acetone, propionaldehyde, crotonaldehyde and 2-butanone & butyraldehyde emissions. The highest ozone-formation potential (OFP) from multi-pollution emissions was found an idling operation. The high OFP could be reduced by increasing hydrogen additions and eventually approached the lowest level with 1.2 vol% hydrogen addition at middle to high engine load. The average reduction for total PAHs after hydrogen addition were 56.4%, 34.5%, and 27.9%, respectively. The same trend of total toxicity equivalence (TEF-BaPeq) was pointed out and the average reduction was observed at 44.1%, 23.2%, and 25.4%, respectively after hydrogen addition. According to the gasoline vehicle was fueled with gasoline and multiple bioethanols applied with and without hydrogen addition. The results show that the E3, E6 in the fuel blends benefits the complete combustion of the fuel-air mixture during cold start transient phase compared to the base fuel of G0. Therefore, high inflammation with diffusion speeds of hydrogen addition with E6, E10 improve the combustion process, extend air and fuel mixing more homogeneous, which are average reduced 38.8%, 44.0% for CO, HC, respectively. The small amount of hydrogen addition with bioethanol/gasoline fuel blends slightly reduced the NOx accumulated mass, due to the leaner mixture during cold start. Especially, the dropping trend could also discern after the small amount of hydrogen addition in comparison with the base fuel of G0. The overall of average well-to-tank GHG emissions accounts for 22.3% of the well-to-wheel GHG emissions. This discrepancy is related to feedstock and fuel economy. However, the corn-based E10 offset the well-to-tank GHG emissions with the result of 65.6 g CO2 -e/km. The lowest GHG emissions could be found after the small amount of hydrogen addition within the well-to-tank process, due to lower fuel consumption relative to the lowest GHG emission (65.3 g CO2 -e/km). According to the result of well-to-wheel, the lowest GHG emissions was found 282.6 g CO2 -e/km in E10, which was reduced by 6.96% in comparison with base fuel (G0). However, the small amount of hydrogen for each test result was not a significant decrease in comparison with bioethanol, due to the reason of feedstock within the well-to-tank process.

TABLE OF CONTENTS
SECTION PAGE
國立中山大學研究生學位論文審定書 i
國立中山大學博碩士論文公開授權書 ii
致謝 iii
中文摘要 iv
ABSTRACT v
TABLE OF CONTENTS vii
LIST OF FIGURES xii
LIST OF TABLES xvi
ABBREVIATIONS xviii
CHAPTER 1 INTRODUCTION 1
1.1 Background 1
1.2 Objectives 4
CHAPTER 2 LITERATURE REVIEW 6
2.1 Overview of Environment 6
2.2 Diesel Engine Operation 7
2.3 Spark ignition engine 8
2.4 Fuel technology 9
2.4.1 Electric 9
2.4.2 Biofuel 10
2.4.3 Hydrogen (H2) 11
2.4.4 Natural Gas (NG) 12
2.5 Regulated exhaust emissions 12
2.5.1 Carbon dioxide (CO2) and carbon monoxide (CO) 13
2.5.2 Hydrocarbons (HCs) 13
2.5.3 Nitrogen Oxides (NOx) 14
2.5.4 Particulate Matters (PM) 15
2.6 Unregulated pollutants 16
2.6.1Carbonyl compounds (CBCs) 16
2.6.1.1Ozone formation potential (OFP) 16
2.6.1.2 Maximum Incremental Reactivity (MIR) 18
2.6.2 Polycyclic aromatic hydrocarbons (PAHs) 20
2.6.3 Health impact 23
2.7 Summary of pollutant reduction by hydrogen addition 26
2.7.1 Hydrogen addition for regulated pollutants reduction 26
2.7.2 Hydrogen addition for unregulated pollutants reduction 27
2.8 Summary of pollutant reduction fueled with bioethanol 28
2.9 Life cycle assessment 29
CHAPTER 3 MATERIALS AND METHODS 32
3.1 Structure and Scope 32
3.2 Overview of the Measurement Methods for Diesel engine 33
3.2.1 Speciation of the diesel engine 33
3.2.2 Carbonyl compounds measurement 38
3.2.3 Polycyclic aromatic hydrocarbons measurement 40
3.2.4 European Stationary Cycle (ESC) 41
3.3 Overview of the Measurement Methods for gasoline vehicle 45
3.3.1 Speciation of test vehicle and procedures 45
3.3.2 US Light-duty test cycle FTP-75 49
3.4 Life Cycle Assessment 50
3.4.1 Well-to-wheel assessment 50
3.4.2 System Boundary 52
CHAPTER 4 REDUCING POLLUTANTS EMISSIONS FROM A HEAVY-DUTY DIESEL ENGINE BY USING HYDROGEN ADDITION 54
4.1 Introduction 54
4.2 Engine Performance 54
4.2.1 Brake thermal efficiency and brake specific fuel consumption 54
4.2.2 Equivalence ratio 57
4.3 Traditional Pollutants 58
4.3.1 Carbon monoxide and carbon dioxide emissions (CO, CO2) 58
4.3.2 Total hydrocarbon emissions (THC) 60
4.3.3 Nitrogen oxides emissions (NOx) 61
4.3.4 Particulate matter (PM) 63
CHAPTER 5 EVALUATION OF THE TOXICITY EMISSIONS FROM HEAVY-DUTY DIESEL ENGINE BY HYDROGEN DUAL FUEL COMBUSTION 65
5.1 Introduction 65
5.2 Carbonyl compounds profile 65
5.3 Formaldehyde acetaldehyde emissions 66
5.4 Health risk assessment of formaldehyde (FOR) and acetaldehyde (ACE) 71
5.4.1 Acrolein, acetone, propionaldehyde, crotonaldehyde and 2-butanone & butyraldehyde emissions 75
5.4.2 Other carbonyl emissions 77
5.5 Ozone-formation potential 79
5.5.1 The annual CBCs and OFP reductions by using hydrogen addition 80
5.6 Polycyclic aromatic hydrocarbons emissions 83
5.6.1 Toxicity equivalence factors and excess cancer risk (ECR) assessment 87
CHAPTER 6 EVALUATION OF FUEL CONSUMPTION, POLLUTANT EMISSIONS AND WELL TO WHEEL GHGs ASSESMENT FROM A VEHICLE OPERATION FUELED WITH BIOETHANOL, GASOLINE AND HYDROGEN 91
6.1 Introduction 91
6.2 Data analysis 93
6.3 Life cycle assessment 95
6.4. Traditional Pollutants emissions 96
6.4.1 CO, HC and NOx exhaust after cold start transient cycle 96
6.4.2 CO, HC and NOx exhaust with hydrogen addition after cold start transient cycle 97
6.4.3 CO, HC and NOx exhaust emissions during FTP-75 start cycle 103
6.4.4 Fuel consumption during FTP-75 start cycle 106
6.4.5 Well-to-wheel greenhouse gas emissions 107
CHAPTER 7 CONCLUSIONS AND SUGGESTIONS 109
7.1 Conclusions 109
7.1.1 Diesel engine 109
7.1.2 Gasoline vehicle 112
7.2 Suggestions 113
CHAPTER 8 REFERENCES 115
APPENDIX 141
RESUME 142
LIST OF TABLES
TABLES PAGE
Table 2-1 Maximum incremental reactivity values of carbonyl compounds 19
Table 2-2a Twenty-one priority of polycyclic aromatic hydrocarbons (PAHs) 21
Table 2-2b Twenty-one priority of polycyclic aromatic hydrocarbons (PAHs) 22
Table 2-3 Traffic-related air pollutants potential human health risk 24
Table 2-4 PAH species with molecular weight and toxic equivalent factors (TEFs) 25
Table 3-1 The apparatus of measurements 34
Table 3-2 Specifications of tested engine 34
Table 3-3 Hydrogen generator typical properties 37
Table 3-4 Apparatus of sampling 38
Table 3-5 European Stationary Cycle (ESC) 13 modes test cycle 42
Table 3-6 Physical and chemical properties of diesel and hydrogen 43
Table 3-7 Experimental conditions 44
Table 3-8 Emission analyzer speciation 45
Table 3-9 Speciation of test vehicle 46
Table 3-10 Property of test fuels 48
Table 3-11 Well-to-tank CO2 equivalent emissions based on global warming potentials (GWPs) consider in this study. 51
Table 5-1 The summary of risk parameters for formaldehyde and acetaldehyde 72
Table 5-2 The inhalation lifetime cancer risk (LTCR) to the human health upon exposure to FOR (Unit: µg kg-1 day-1). 73
Table 5-3 The inhalation lifetime cancer risk (LTCR) to the human health upon exposure to ACE (Unit: µg kg-1 day-1). 74
Table 5-4 Other carbonyl emissions in the exhaust of the diesel engine with hydrogen addition under various engine operating conditions
(mg kW -1hr -1). 78
Table 5-5 Annual carbonyl compounds and ozone formation potential from a diesel engine with hydrogen addition 82
Table 5-6 Polycyclic aromatic hydrocarbons emission factor from a diesel engine with hydrogen addition 85
Table 5-7 PAHs and BaPeq and excess cancer risks (ECR) from a diesel engine with hydrogen addition. 88
Table 5-8 Health risk assessment of aerosol carcinogenicity from a diesel engine with hydrogen addition 89
Table 6-1 Accumulated emission mass during cold-start and full cycle during FTP-75 transient cycle 94
Table 6-2 Well-to-tank GHGs emissions for FTP-75 transient cycle 96
LIST OF FIGURES
FIGURES PAGE
Figure 1-1 Average annual growth in energy demand by fuel 1
Figure 1-2 Global Energy-Related CO2 Emissions 2
Figure 2-1 The diagram of typical combustion process of the diesel engine 7
Figure 2-2 Lifecycle assessment framework 30
Figure 2-3 Well-to-wheel life cycle assessment 31
Figure 3-1 Flow chart of this research 32
Figure 3-2 Diesel Engine and Emission test laboratory 35
Figure 3-3 Hydrogen Generator 36
Figure 3-4 Summary of carbonyl compounds sample collection and analysis 39
Figure 3-5 Cartridge (XAD-16 resin) and glass fiber filter 40
Figure 3-6 European stationary test cycle (ESC) 41
Figure 3-7 Schematic of the experimental setup, including Cummins B5.9-160 diesel engine, and sampling system 44
Figure 3-8 Schematic diagram of vehicle test apparatus 46
Figure 3-9 Gasoline vehicle and Emission test laboratory 47
Figure 3-10 Federal test driving schedule (FTP-75) 49
Figure 3-11 Well-to-wheels life cycle analysis system boundaries for bioethanol and gasoline 53
Figure 4-1 Variation of brake thermal efficiency (BTE) against engine loads for different fuel blends used in the study 56
Figure 4-2 Variation of brake specific fuel consumption (BSFC) against engine loads for different fuel blends used in the study 56
Figure 4-3 Equivalence ratio against engine loads for different fuel blends used in the study 57
Figure 4-4 Variation of carbon monoxide emissions against engine loads for different fuel blends used in the study 59
Figure 4-5 Variation of carbon dioxide emissions against engine loads for different fuel blends used in the study 59
Figure 4-6 Variation of total hydrocarbon emissions against engine loads for different fuel blends used in the study 61
Figure 4-7 Variation of NOx emissions against engine loads for different fuel blends used in the study 62
Figure 4-8 Variation of PM emissions against engine loads for different fuel blends used in the study 64
Figure 5-1 Composition profiles of CBCs from hydrogen blends under various engine operating conditions. FOR (formaldehyde), ACE (acetaldehyde), ACR (acrolein), ATN (acetone), PRO (propionaldehyde), CRO (crotonaldehyde), 2-BUT&BUTYR (2-butanone+butyraldehyde), BEN (benzaldehyde), ISO-VAL (iso-valeraldehyde), VAL (valeraldehyde), HEX (hexaldehyde) 69
Figure 5-2 Formaldehyde and acetaldehyde in the exhaust of the diesel engine with hydrogen addition under various engine operating conditions 70
Figure 5-3 Acrolein, acetone, propionaldehyde, crotonaldehyde and butyraldehyde & 2- butyraldehyde in the exhaust of the diesel engine with hydrogen addition under various engine operating conditions 76
Figure 5-4 Ozone formation potential of carbonyls in the exhaust of the diesel engine with hydrogen addition under various engine operating conditions 80
Figure 5-5 Three categories of polycyclic aromatic hydrocarbons (PAHs) emission factor base on molecular weight (LMW: Low molecular weights; MMW: Middle molecular weights; HMW: High molecular weights) at different engine load with hydrogen addition 86
Figure 5-6 Three categories of toxicity equivalence (TEF-BaPeq) base on polycyclic aromatic hydrocarbons (PAHs) molecular weight (LMW: Low molecular weights; MMW: Middle molecular weights; HMW: High molecular weights) at different engine load with hydrogen addition 90
Figure 6-1 (a) HC, (b) CO and (c) NOx accumulated emissions (grams) during FTP-75 cold-transient phase plotted against the oxygen content of testing fuels 100
Figure 6-2 Instantaneous HC emissions during the FTP-75 cold-transient phase with hydrogen addition. 101
Figure 6-3 Instantaneous CO emissions during FTP-75 cold-transient phase with hydrogen addition 102
Figure 6-4 (a) HC, (b) CO and (c) NOx emission factor over FTP-75 Transient Cycle. 105
Figure 6-5 Fuel consumption over FTP-75 Transient Cycle 106
Figure 6-6 Well-to-wheel (WTW) greenhouse gas (GHG) emissions for different fuel over FTP-75 transient Cycle, include tank-to-wheel (TTW) and well-to-tank (WTT) components. Well-to-tank GHG emissions represent the CO2-equivalent (CO2-e) emissions of the carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O). 102

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