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研究生： 曾家麟
Chia-lin Tseng
論文名稱： 光電化學法產氫反應器之設計與熱流特性分析
Design and Thermal-Fluid Analysis of Photoelectrochemical Hydrogen Production Reactor
指導教授： 曾重仁
Chung-jen Tseng
口試委員:
學位類別： 博士
Doctor
系所名稱： 工學院 - 機械工程學系
Department of Mechanical Engineering
畢業學年度： 99
語文別： 中文
論文頁數： 163
中文關鍵詞： 太陽能產氫 、光電化學法 、反應器設計 、產氫量及產氫效率
外文關鍵詞： photoelectrochemical method, solar-to-hydrogen efficiency, hydrogen volume production, reactor design, solar hydrogen production
相關次數： 點閱：18  下載：0 
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    • 第一部份，探討AM 1.5(G)太陽光於光電化學法產氫的熱力學分析。因裂解水的能量隨著反應器的溫度升高而降低，故利用太陽光長波能量加熱反應器可增加產氫的效率。
    半導體光電極能隙的增加會降低光電流的輸出，當AM 1.5(G)太陽光全部激發成電子產生光電流，理論最大的光電流為63.8 mA/cm2。對半導體能隙2.0 eV及3.0 eV的理論最大光電流分別為12.4 mA/cm2及1.29 mA/cm2。太陽光理論最大功率轉換效率為44.1 %，對能隙2.0 eV及3.0 eV的功率轉換效率則分別為24.7 %及3.9 %。探討溫度及量子效率上，當溫度為647 K及量子效率為30 %時，半導體能隙為2.0 eV及3.0 eV的理論最大產氫量分別為47.5 L/m2-hr及8.0 L/m2-hr；而理論最大產氫效率則分別為16.1 %及2.7 %。增加量子效率較提升反應器溫度能更有效地增加產氫量及產氫量效率，但若固定量子效率下，提升反應器溫度對增加產氫量及產氫效率為一非常有效的方法。
    第二部份，探討4種不同光電化學法產氫反應器的熱傳設計及熱流特性。AM 1.5(G)太陽光根據半導體光電極的能隙，分為短波及長波。短波能量用來產生電子與電洞對，長波能量則利用於加熱反應器。由於裂解水所需的能量隨溫度升高而降低，故利用長波能量加熱反應器可增加系統效率。因此，長波能量如何利用來加熱反應器，為非常重要的課題。
    結果顯示，越多長波能量被反應器所吸收，產氫量及產氫效率越高。D設計下，太陽光強度為4000 W/m2及量子效率為30 %時，產氫量及產氫效率於能隙2.0 eV分別為186.5 L/m2-hr及15.9 %。光電化學法產氫反應器參數設計的影響，將於本論文中詳細討論。

    In partⅠ, the thermodynamic analysis of photoelectrochemical (PEC) hydrogen production is performed in this thesis for air mass 1.5 solar irradiation. Because the energy required for splitting water decreases as temperature is increased, heating the system by using the long wavelength energy will increase the system efficiency.
    As the energy band gap of the photoelectrode increases, the induced photo-current is decreased. If photons absorbed are all excited, the maximum photo-current is 63.8 mA/cm2. For energy band of 2.0 eV and 3.0 eV, the maximum photo-current is respectively 12.4 mA/cm2 and 1.29 mA/cm2. The maximum power conversion efficiency of a PEC cell is 44.1 %. For 2.0 eV and 3.0 eV, the power conversion efficiency is 24.7 % and 3.9 %, respectively. At 647 K and quantum efficiency=30 %, the maximum hydrogen production rate is 47.5 L/m2-hr and 8.0 L/m2-hr for 2.0 eV and 3.0 eV, and the maximum solar-to-hydrogen efficiency is 16.1 % and 2.7 % for 2.0 eV and 3.0 eV, respectively. In order to increase the maximum hydrogen production rate and the solar-to-hydrogen efficiency, it is more effective to raise the quantum efficiency than raising the reaction temperature. But for fixed quantum efficiency, raising the reactor temperature is also an effective way to increase the solar-to-hydrogen efficiency.
    In part Ⅱ, the heat transfer and flow characteristics of a PEC hydrogen generation reactor are investigated numerically. Four different reactor designs are considered. The solar irradiation is separated into short and long wavelength parts depending on the energy band gap of the photoelectrode used. While short wavelength part is used to generate electron and hole pairs, the long wavelength part is used to heat the system. Because the energy required for splitting water decreases as temperature is increased, heating the reactor by using the long wave energy increases the system efficiency. Thus, how the long wavelength energy is absorbed by the reactor is very important.
    The results show that more long wavelength energy kept inside the reactor can increase the solar-to-hydrogen efficiency. For energy band gap of 2.0 eV photoelectrode, careful reactor design can increase solar-to-hydrogen efficiency by 9.7 %. For design D under 4000 W/m2 irradiation and a quantum efficiency of 30 %, is found to be 15.9 % and the hydrogen volume production rate is 186.5 L/m2-hr for 2.0 eV. Effects of several parameters on the PEC hydrogen reactor are discussed in detail.

    摘 要 i Abstract iii 誌 謝 v 目 錄 vi 圖目錄 ix 表目錄 xiv 符號表 xv 第一章 前 言 1 1.1 能源概述 1 1.2 氫能技術 5 1.3 光電化學法產氫系統 11 1.3.1 光電化學法產氫原理 11 1.3.2 太陽輻射之特性 17 1.3.3 光電化學法產氫系統之阻抗 20 第二章 文獻回顧 23 2.1 半導體之能隙 24 2.2 光電極材料之演進 28 2.3 熱力學之分析 34 2.4 反應器之架構 39 2.5 研究動機與主題 51 第三章 物理模型與數值方法 52 3.1 物理模型 52 3.2 輻射傳輸方程式 62 3.3 數值模型驗證 70 第四章 結果與討論 76 4.1 第一部份 76 4.1.1 光電流的影響 76 4.1.2 PEC反應器I-V曲線特性 80 4.1.3 光子轉換為電子之能量損失 82 4.1.4 理論最大產氫量 84 4.1.5 理論最大產氫效率 86 4.2 第二部份 88 4.2.1 反應器設計的影響 97 4.2.2 太陽光強度的影響 107 4.2.3 玻璃厚度G及水厚度W的影響 112 4.2.4 量子效率的影響 117 第五章 結 論 122 第六章 未來建議 125 參考文獻 126 作者簡介 138 圖目錄 圖1-1　各種內燃機引擎與燃料電池系統所產生之二氧化碳濃度比較 [6] 3 圖1-2　全球能源過去利用趨勢與未來市場預測圖 [24] 10 圖1-3　n型半導體光電化學法產氫系統之示意圖 [25] 13 圖1-4　n型半導體光電化學法產氫之能帶操作原理示意圖 [26] 13 圖1-5　pH＝2.0下，不同氧化物半導體與水裂解氧化還原電位之關係 [27] 16 圖1-6　太陽輻射能量光譜圖 [28] 19 圖1-7　不同能隙所能利用之太陽輻射能量 [28] 19 圖1-8　不同能隙下，太陽光子數量圖 [29] 22 圖2-1　直接與間接能隙半導體再結合效應之光與熱轉換過程。(a) 直接能隙半導體之光轉換過程；(b) 間接能隙半導體之熱轉換過程 [32]。 25 圖2-2　壓力1 bar與500 bar下，理論電解水所需要之電位關係 [57] 36 圖2-3　太陽光譜中，長波輻射與短波輻射利用範圍示意圖 [58] 36 圖2-4　不同半導體能隙下，可利用的太陽光長波能量比例 [59] 37 圖2-5　太陽光照射下，PEC產氫長短波輻射能量利用示意圖 [60, 61] 37 圖2-6　雙光電極系統電極－電解液電位之能量關係圖 [66] 42 圖2-7　混合式光電極系統 [48] 43 圖2-8　不同硫化物濃度下，硫化鎘電極形成光電流與電壓之關係 [67, 68] 47 圖2-9　加裝玻璃（塗佈SnO2:F）下，ITO塗佈非晶矽薄膜產氫反應器示意圖 [69] 47 圖2-10　彈性塑膠袋狀產氫反應器 [70] 48 圖2-11　剛體球狀產氫反應器 [70] 49 圖2-12　Z機制原理示意圖 [72, 73] 50 圖2-13　Z機制之雙反應槽產氫反應器示意圖 [71] 50 圖3-1　光電化學法產氫反應器之示意圖 54 圖3-2　AM 1.5(G)太陽光譜中，能隙與能量百分比關係 55 圖3-3　FTO與玻璃吸收光譜 56 圖3-4　水吸收光譜 [77] 56 圖3-5　太陽能聚光系統 57 圖3-6　輻射傳輸過程之能量變化示意圖 65 圖3-7　輻射方向立體角離散座標系統示意圖 66 圖3-8　不透明表面輻射傳遞邊界條件示意圖 69 圖3-9　Williams等人 [82]在光學厚度1.0下，不同輻射模組之壁面無因次 73 圖3-10　Williams等人 [82]在光學厚度5.0下，不同輻射模組之壁面無因次化結果與本論文計算比對圖 73 圖3-11　太陽光強度4000 W/m2與QE=30 %下，A設計及D設計反應器的　網格獨立性驗證 74 圖3-12　太陽光強度4000 W/m2與QE=30 %下，A設計及D設計反應器的立體角數量獨立性驗證 74 圖4-1　AM 1.5(G)太陽照射與對應波長下的光子數量關係圖 78 圖4-2　AM 1.5(G)太陽照射與對應波長下可激發的光電流關係圖 78 圖4-3　AM 1.5(G)太陽光I-V曲線圖 81 圖4-4　AM 1.5(G)太陽光，最大可激發電子能量及有效可激發電子能量關係圖 83 圖4-5　不同量子效率下，300 K及647 K理論最大產氫量 85 圖4-6　不同量子效率下，300 K及647 K理論最大產氫效率 87 圖4-7　傳統雙電極反應器及多接合單電極反應器設計示意圖。 92 圖4-8　不同能隙下，傳統雙電極反應器及多接合單電極反應器的陽極平均溫度曲線圖 93 圖4-9　水的自由能隨著不同溫度變化關係圖 93 圖4-10　太陽光強度6000 W/m2、QE＝30 %、G=5 mm及W＝30 mm，反應器Ι、Ⅱ及Ⅲ於Eg＝2.0 eV的溫度分佈與速度向量圖 95 圖4-11　太陽光強度4000 W/m2、QE＝30 %及水厚度W＝10 mm，四種不同反應器設計於不同能隙的光電極平均溫度曲線圖 99 圖4-12　太陽光強度4000 W/m2、QE＝30 %及水厚度W＝10 mm，四種不同反應器設計於不同能隙的溫度分佈圖 103 圖4-13　太陽光強度4000 W/m2、QE＝30 %及水厚度W＝10 mm，四種不同反應器設計於Eg＝2.0 eV的速度向量與溫度分佈圖 104 圖4-14　太陽光強度4000 W/m2、QE＝30 %及水厚度W＝10 mm，四種不同反應器設計於不同能隙的產氫量關係圖 106 圖4-15　太陽光強度4000 W/m2、QE＝30 %及水厚度W＝10 mm，四種不同反應器設計於不同能隙的產氫效率關係圖 106 圖4-16 QE＝30 %、W＝10 mm、G＝10 mm及A＝20 mm下，D設計反應器於不同太陽光強度的光電極平均溫度曲線圖 109 圖4-17　QE＝30 %、W＝10 mm、G＝10 mm及A＝20 mm下，D設計反應器於不同太陽光強度的產氫量關係圖 110 圖4-18　QE＝30 %、W＝10 mm、G＝10 mm及A＝20 mm下，D設計反應器於不同太陽光強度的產氫效率關係圖 110 圖4-19　Eg=2.0 eV、QE＝30 %、W＝10 mm、G＝10 mm及A＝20 mm下，D設計反應器於不同太陽光強度的溫度分佈及速度向量圖 111 圖4-20　太陽光強度4000 W/m2、QE＝30 %及A＝20 mm下，D設計反應器於不同G及W的光電極平均溫度曲線圖 114 圖4-21　太陽光強度4000 W/m2、QE＝30 %及A＝20 mm下，D設計反應器於不同G及W的產氫效率關係圖 114 圖4-22　Eg=2.0 eV、QE＝30 %、A＝20 mm及4000 W/m2下，不同G及W設計反應器的溫度分佈及速度向量圖 116 圖4-23　太陽光強度4000 W/m2、G＝5 mm、W＝10 mm及A＝20 mm下，D設計反應器於不同QE的光電極平均溫度曲線圖 119 圖4-24　太陽光強度4000 W/m2、G＝5 mm、W＝10 mm及A＝20 mm下，D設計反應器於不同QE的產氫量關係圖 120 圖4-25　太陽光強度4000 W/m2、G＝5 mm、W＝10 mm及A＝20 mm下，D設計反應器於不同QE的產氫效率關係圖 120 圖4-26　太陽光強度4000 W/m2、G＝5 mm、W＝10 mm及A＝20 mm下，D設計反應器於不同QE的溫度分佈及速度向量圖 121 表目錄 表一　各種不同PEC系統之實驗光電極與效率 29 表二 反應器材料之物理參數 58 表三　Williams等人 [82]不同輻射條件下結果與本論文計算數據比對表 75 表四　AM 1.5(G)太陽照射與對應波長下可激發的能量百分比及光電流 79

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