本研究論文主要在探討陽極注氧(Anode air-bleeding)對 CO 毒化質子交換膜燃料電池(PEMFC)的性能影響及其動態行為模式的分析，尤其是在高 CO 濃度進料(H2+200 ppm CO)，同時也進行各種操作參數(電池溫度、電池電壓、CO濃度、陽極注氧濃度)對CO毒化的影響及長時間陽極注氧對電池穩定性及耐久性的評估。藉此研究論文提供更多的研究資訊與測試數據，以做為解決燃料電池CO毒化的參考方案，同時期望能應用於燃料電池熱電共生(Combined heat and power, CHP)發電系統及達到簡化燃料重組器(Reformer)的設計與製作。
在實驗材料及測試分析方面，本研究是使用25 cm2單電池為測試電池，其中的膜電極材料為Gore PRIMEA 5621 MEA，並使用兩種氣體擴散層材料(碳布及碳紙)，型號分別為CARBEL CL® GDL及SIGRACET® GDL 10BC。測試電池的流道板使用POCO碳板材料，其中流道長度及型態為65cm/Serpentine。電池所有的性能測試都在標準的燃料電池性能測試系統(HEPHAS HTS-125)中進行，其中測試項目包括：極化曲線、電池阻抗變化及電壓/電流的輸出變化，同時也使用穿透式電子顯微鏡(TEM)及能量分散光譜(EDS)來分析觸媒材料的內部結構與化學組成。
以下為本研究論文所獲得的重要研究結果：
‧當操作在 Pure H2 時，電池可獲得優異的性能(1800 mA/cm2 @0.5V)，但是H2中只要含有微量CO濃度(例如:25及200 ppm)，電池性能會發生嚴重衰退(分別下降至920及315 mA/cm2 )。電池的電壓損失在高電壓區域(0.9~0.8V)，幾乎不受CO濃度的影響，但是在低電壓區域(< 0.8V)就明顯受到CO濃度的影響。其中可能的原因是在高電壓(低電流)時，CO於Pt觸媒上的吸附對活化過電位的影響很小；但是在低電壓(高電流)區域，CO於Pt觸媒上的吸附會對活化過電位造成重大的影響。
‧CO毒化會造成電池輸出電流密度的迅速下降，但是下降的電流密度最終會到達一穩定值(iss)，其中所需時間為 tss。此iss及tss都與CO濃度成反比的關係，但是在低CO濃度時，電池的iss明顯呈現較高的CO靈敏度(SCO)。所以陽極雖然使用具CO容忍度的 Pt-Ru 合金觸媒，即使只有微量CO濃度，電池仍然會在短時間內造成嚴重的性能損失。當CO濃度為25 ppm時，電池在40分鐘內就會造成40%的電流損失；當CO濃度為50 ppm時，電池在20分鐘內就會有高達80%的電流損失。
‧只要在陽極進料中注入小量空氣就可快速達到抑制CO毒化的功效，並且可大幅恢復電池的輸出性能。當CO濃度為50 ppm時，只要注氧 5% air就可在1分鐘內恢復90%的電池性能；即使在高CO濃度進料下(H2+200 ppm CO)，也可在10分鐘內達到90%的恢復率，但是過高的注氧濃度(>10% air)反而會造成電池性能的下降，所以適當的注氧量必須要依據CO濃度來調整。由測試結果顯示，當H2進料中含有25, 50, 100, 200 ppm CO時，最佳的陽極注氧濃度分別為2%, 3%, 5%及7% air，這些都可使電池性能大幅恢復達88%以上。
‧本研究提出一暫態的理論CO毒化模式，此模式最大特點是在陽極注氧時，有考慮N2分子在Pt觸媒上的吸附及脫附效應。另外也提出一簡易的半經驗方程式(Semi-empirical equation)，主要用來模擬在各種操作參數下(操作溫度、電壓、電流、CO濃度、注氧濃度)，燃料電池CO毒化的動態行為。從研究數據的比較與分析發現，所提出的兩種CO毒化模式在實驗值與模擬結果的趨勢都有很好的一致性。
‧陽極使用模擬重組氣體(45% H2、17% CO2、3% CH4及 25 ppm CO)，在定電流密度(@300 mA/cm2)下完成3,000小時燃料電池的耐久性測試。由實驗結果顯示，電池在陽極注氧下(5% air)具有相當穩定的電壓輸出，而且電壓衰退情形並不嚴重< 3% (或0.64×10−5 V/hr)。
‧提高電池的操作溫度可以大幅提升CO容忍度(CO tolerance)，但是溫度太高(>80℃)也會造成質子交換膜過於乾燥而降低H+ 質子傳導率。如果要同時改善電池的輸出性能及降低CO毒化效應，建議電池的操作溫度要比操作純H2進料時提高5~10℃。
‧電池的過電壓損失與電荷轉移阻抗都是隨著CO濃度的增加而大幅增加，而且是呈線性的正比關係，但是電池的內電阻幾乎不受CO濃度變化的影響。
‧電池在高CO濃度進料下(H2+200 ppm CO)，5% air的陽極注氧可提升電池性能達80%以上，其中電池性能的回升速度要比使用Pure H2快約15倍。電池在300小時的測試過程都維持相當穩定的電流輸出(@0.6 V)，其中電流密度的衰退率保持在2%以下。
‧對於質子交換膜燃料電池發電系統，如果它的陽極富氫氣體是來自於重組器，應用陽極注氧技術可帶來兩個獨特優點：(1)發電系統可獲得相當穩定的電力輸出，而且可大幅降低輸出功率的振盪幅度；(2)可提升發電系統對高CO濃度(200 ppm CO)的容忍度，因此可大幅簡化燃料重組器的設計與製作。

This study investigates the effectiveness of anode air-bleeding on the dynamic performance of a proton exchange membrane fuel cell (PEMFC) in a CO poisoning situation. The scope of the study covers various operational conditions at high CO concentrations (H2+200 ppm CO), including cell temperature, cell voltage, CO concentration, and the amount of air bleeding. The cell’s long-term durability under air bleeding conditions has also been evaluated. The results of this study provide additional data and information that may contribute to the resolution of PEMFC poisoning by CO and also towards a simple reformer design that incorporates a combined heat and power (CHP) unit.
A single cell with an active area of 25 cm2 was used for the testing. The membrane electrode assembly used was a Gore PRIMEA 5621 MEA. The gas diffusion layers were CARBEL CL® GDL and SIGRACET® GDL 10BC. The carbon plate was a POCO carbon plate with 65 cm serpentine flow channels. All the cell performance tests, I-V polarization curve, impedance, and dynamic behavior of the cell’s voltage/current, were carried out on a standard fuel cell testing station (HEPHAS HTS-125). The structure and chemical composition of the catalyst material were examined by TEM (tunneling electron microscopy) and EDS (energy dispersing spectra).

Important findings are summarized as follows:
‧Excellent cell performance was obtained (1800 mA/cm2 @0.5V) with pure H2. However, trace amounts of CO, i.e. 25 and 200 ppm, in the H2 fuel resulted in severe performance degradation with the cell’s output current dropping to 920 and 315 mA/cm2, respectively. The voltage loss in the high cell voltage region (0.9~0.8V) was independent of CO concentration: this might be due to low CO adsorption in this region. CO adsorption had only a minor effect on the activation overpotential. However, in the low cell voltage region (< 0.8V), CO adsorption became significant and the influence of CO on the activation overpotential is important.
‧CO poisoning can cause the cell’s output current to drop quickly. After tss, the current drop eventually reached a steady value (iss). Both tss and iss were inversely proportional to the CO concentration. At low CO concentrations, the value of iss was very sensitive to the presence of CO. Cell performance decreased significantly in a short time, even when a CO-tolerant catalyst (Pt-Ru) was used at the anode. Within 40 min, about 40% of the output current was lost with 25 ppm CO. With 50 ppm CO, about 80% of the output current was lost within 20 min.
‧The CO poisoning effect can be depressed by injecting a small amount of air into the anode fuel stream. At 50 ppm CO, about 5% air bleeding can recover 90% of the cell current within 1 minute. Even at high CO concentrations (H2+200 ppm CO), about 90% of the cell’s current could be recovered within 10 min. However, excessive air bleeding (> 10% air) will reduce the cell’s performance. The amount of air bleeding must be adjusted according to the CO concentration. Our results indicate that 88%, or above, cell current can be recovered if 2%, 3%, 5% and 7% air bleeding is used when the CO concentration is 25, 50, 100, and 200 ppm, respectively.
‧We have also proposed two transient CO poisoning models. One is a physical model and the other one is a semi-empirical model. The physical model considers the adsorption/desorption effect of N2 on Pt catalyst. The semi-empirical approach models the dynamic responses of CO poisoned PEMFCs under various temperature, voltage, current, CO concentration, and air bleeding conditions. Modeling results from both models were in good agreement with the experimental data.
‧At a constant current of 300mA/cm2, we have completed a 3,000 hour durability test using simulated reformate gas (45% H2, 17% CO2, 3% CH4, and 25 ppm CO) as the anode fuel. The results showed a more stable cell output voltage and that the cell voltage degradation was less than 3% (or 0.64×10−5 V/hr) with 5% air bleeding.
‧The cell is more tolerant to CO at elevated temperatures. However, the proton exchange membrane (PEM) may dry out and lose its proton conductivity if the cell temperature is too high (> 80 °C). To improve cell performance and reduce the effect of CO poisoning, we recommend operating the cell at 5-10 oC higher than the temperature for pure H2.
‧Cell voltage loss and resistance of charge transfer are linearly proportional to the CO concentration. However, the cell’s internal resistance is independent of the CO concentration.
‧At high CO concentrations (H2+200 ppm CO), 80% of the cell’s performance can be recovered by 5% air bleeding. The cell’s performance recovery rate with air bleeding was about 15 times faster than with pure H2. For a 300 hour durability test a stable cell current could be maintained (@ 0.6 V) with a degradation rate below 2%.
‧For a PEMFC power system, with hydrogen-rich reformate gas generated from a reformer, air bleeding offers two unique advantageous outcomes: (a) a stable power output with minimum power fluctuations, (b) the possibility of creating a robust reformer design with high CO tolerance (200 ppm).

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