Jeffrey D. Ward臺灣大學:化學工程學研究所洪愛真Hung, Ai-JenAi-JenHung2010-06-302018-06-282010-06-302018-06-282009U0001-1908200915560500http://ntur.lib.ntu.edu.tw//handle/246246/186962近幾十年來，由於石油存量耗竭及能源問題日益嚴重，使得燃料電池系統之研究發展備受關注，利用氫氣當作燃料供給燃料電池產生電力之系統主要涵蓋三個議題: 產氫、儲氫與發電；因此，此研究目的在建立一套完整燃料供應設施之質子交換膜燃料電池系統，著重在系統化設計、模式建立與控制方面探討，藉此歸納整理一套系統化之設計流程步驟與合適之控制架構。於模式建立階段，藉由回歸實驗數據獲得模式參數與靈敏度分析方式找出影響製程之重要設計變數，此有助於確定最適化之操作條件與製程改良，最後，設計不同之控制架構評估其可行性與韌性。於製程階段，針對硼氫化鈉水解反應之化學儲氫系統進行動力式、穩態模式建立與最適化設計，使其有效提高儲氫效能，在控制方面為達到穩定產氫速率進而設計兩種可行之控制架構。接著，探討質子交換膜燃料電池系統以實驗數據為輔建立模式，利用穩態分析系統操作變數，設計一有效操作方式以達到電池最高效能。建構一解析之成本模式描述燃料電池系統之經濟權衡關係，以年總成本為考量分析投資成本(質子交換膜)與操作成本(氫氣燃料)進而找出最適化之設計。The depletion of fossil fuel has lead to renewed interest in fuel cell systems. The last decade has seen significant progress in power generation using fuel cell systems. It is well known that power generation using hydrogen as fuel involves three important issues: Hydrogen generation, Hydrogen storage, and Power generation. The objective of this work is to emphasize systematic approaches to the modeling, design, and control of fuel cell systems. At the modeling stage, a first principles model of a fuel cell is constructed and model parameters are identified via regression from the experimental data (provided by ITRI). Next, sensitivity of dominant process variables to design and operating efficiency is examined. This facilitates locating the optimal operating condition as well as improved design. Finally, a control system is designed to ensure operating flexibility as well as good disturbance rejection. The model of an experimental proton exchange membrane fuel cell for power generation is developed for process design and optimization. An analytical cost model is constructed to describe such an economic tradeoff between capital cost (membrane electrode assembly area) and operating cost (hydrogen fuel) in a proton exchange membrane fuel cell system. At the process level, the kinetics development, modeling and control of a hydrogen storage process (using sodium borohydride) is investigated.致謝 Ibstract III要 Vist of Figures XIist of Tables XV Introduction 1.1 Hydrogen generation system using sodium borohydride hydrolysis reaction 1.2 Proton exchange membrane fuel cell 3.3 Dissertation organization 6 Kinetics of a sodium borohydride hydrolysis reaction for a hydrogen generation system 8.1 Overview 8.2 Hydrolysis reaction 12.3 Results and discussion 13.3.1 Kinetics 13.3.1.1 Data treatment 13.3.1.2 Zero-order 17.3.1.3 First-order 23.3.1.4 Langmuir-Hinshelwood 25.3.2 Batch reactor model 28.3.3 Validation of the kinetic model 29.4 Conclusions 30 Design and control of a sodium borohydride hydrolysis reaction for a hydrogen generation system 33.1 Overview 33.2 Process description 34.3 Steady-state model of a hydrogen generation reactor 34.3.1 Model assumptions 35.3.2 Modeling equations 35.3.3 Process constraints: Solubility of NaBH4 and NaBO2 in water 37.3.4 Simulation result 38.4 Results and discussion 39.4.1 Sensitivity analysis 39.4.1.1 Effect of feed ratio (FR) 42.4.1.2 Effect of inlet temperature (Tin) 44.4.1.3 Effect of total pressure in the reactor (Pt) 45.4.2 Optimization of operating variables 46.5 Dynamic model of a hydrogen generation reactor 49.5.1 Model assumptions 49.5.2 Dynamic modeling equations 49.6 Control structure design 51.6.1 On-supply control structure 52.6.2 On-demand control structure 53.6.3 Dynamic results 53.7 Conclusions 60 Operation-relevant modeling of an experimental proton exchange membrane fuel cell 63.1 Overview 63.2 Steady-state model of a PEM fuel cell 64.2.1 Model assumptions 64.2.2 Modeling equations 65.2.3 Equation solving procedure 70.3 Results and discussion 71.3.1 Regression and validation 71.3.2 Sensitivity analysis 77.3.2.1 The fuel cell temperature 79.3.2.2 The anode and cathode pressures 80.3.2.3 The stoichiometric ratios of the reactants 81.3.2.4 The humidification temperatures of the reactants at the anode and cathode 81.3.2.5 Summary 82.3.3 Nonlinearity 84.4 Conclusions 86 Cost analysis of proton exchange membrane fuel cell systems 89.1 Overview 89.2 PEM fuel cell system 90.2.1 Operating components in hydrogen-air PEM fuel cell systems 90.2.2 System efficiency 90.3 Economic analysis of PEM fuel cell systems 94.3.1 Linear approximation of a polarization curve 94.3.2 Nondimensionalization 96.3.3 Relationship between MEA area and hydrogen flow rate 97.4 Cost model 101.4.1 Total annual cost (TAC) 101.4.2 Capital cost 104.4.3 Operating cost 106.4.4 Analytical expression of total annual cost (TAC) 107.4.5 Simplified system efficiency 109.4.6 Analytical expressions for TAC optimal design with numbering up (n=1) 110.5 Analysis and discussions 112.5.1 Cost factors: prices of MEA (and bipolar plate) and hydrogen 112.5.2 Reliability factor (life-cycle) for the MEA 114.5.3 Material factors for the MEA 115.5.4 Cost factors in the future 117.5.5 Two methods of varying the MEA area to achieve the same desired power output 119.6 Conclusions 119 Conclusions 124ppendix A 128ppendix B 133ppendix C 134ppendix D 138eferences 140utobiography 1501459136 bytesapplication/pdfen-US儲氫質子交換膜燃料電池程序設計模式化控制hydrogen storageproton exchange membrane fuel cellprocess designmodelingefficiencycontrolthesishttp://ntur.lib.ntu.edu.tw/bitstream/246246/186962/1/ntu-98-D94524019-1.pdf