直接醇类燃料电池阳极铂基电催化剂的研究
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摘要
直接乙醇燃料电池除具有功率密度高、操作简单、携带方便等特点外，其独特的优势是乙醇是一种价廉易得的可再生绿色燃料。然而，乙醇电氧化的复杂性使得探索高效乙醇电氧化催化剂成为一项具有挑战性的工作。
本文采用三种方法制备了PtSn／C催化剂，并对制备条件进行了优化。考察了不同Sn前体、Pt／Sn比例、还原温度及后处理气氛对乙醇催化活性的影响。通过XRD和分析电镜研究了PtSn／C和PtRu／C催化剂结构的不同，并将其结构与催化氧化乙醇的活性进行了关联。
在对SnO_2纳米粒子粒径可控的基础上，设计并制备了三种具有不同微观结构—表层富铂、表层富锡及铂锡合金纳米粒子，并采用紫外可见光谱、红外光谱、分析电镜、X光能谱、X射线衍射等技术对催化剂进行了深入研究。电化学及单池性能测试结果表明，表层富铂的PtSn纳米粒子对乙醇电氧化具有更好的催化活性，其作为阳极催化剂的直接乙醇燃料电池单池性能达到80mW cm~(-2)，比相同操作条件下文献报道的最高值高约一倍。对自制铂基催化剂组装的DEFC单池进行了稳定性测试，分析性能衰减的原因。
采用二氯二乙二胺合铂和硝基硝酰钌为前驱体，利用浸渍氢还原法制备了PtRu／C催化剂，并将其甲醇氧化活性与商品PtRu催化剂进行了比较，发现催化剂对甲醇电氧化活性随PtRu合金度的增大而提高。
开发了全氟磺酸离子交联聚合物(PFSt)稳定的Pt胶体及Pt／C催化剂，其作为DMFC阴极的性能要远高于PTFE为稳定剂的催化剂。
Direct alcohol fuel cells have gained amount of attentions within the last years due to its high power density, simple operation, and portability. As a green and renewable fuel, ethanol is less toxic and is available from crop ferment. However, the complete electrooxidation of ethanol involves the transfer of 12 electronics and 12 protons arising from not only dehydrogenation but cleavage of C-C bonds. The electrooxidation process of ethanol, resulting to more by-products, is much more complex than methanol. This makes the development of anode electrocatalysts for ethanol electrooxidation a great challenge task.
PtSn/C electrocatalyst was prepared by three methods and the results show that the modified polyol method is suitable for preparing high metal-loading nanocatalysts with uniform distribution and small particle size. The synthesis parameters, including tin precursors, Pt/Sn atomic ratio, reduction temperature, and the post treatment atmosphere, etc., were investigated in detail. Employing X-ray Diffraction and Analysis Electron Microscopy, the effect of Sn and Ru on the variation of the Pt lattice parameter was studied. The relationship between the structure of PtSn and PtRu nanoparticles and their catalytic activity on ethanol electrooxidation was studied. It was found that PtSn/C with the dilated lattice parameter of Pt showed higher activity for ethanol electrooxidation than PtRu/C with the contracted Pt lattice parameter.
On the basis of the controllable synthesis of SnO_2 nanopartilces, three kinds
本文采用三种方法制备了PtSn／C催化剂，并对制备条件进行了优化。考察了不同Sn前体、Pt／Sn比例、还原温度及后处理气氛对乙醇催化活性的影响。通过XRD和分析电镜研究了PtSn／C和PtRu／C催化剂结构的不同，并将其结构与催化氧化乙醇的活性进行了关联。
在对SnO_2纳米粒子粒径可控的基础上，设计并制备了三种具有不同微观结构—表层富铂、表层富锡及铂锡合金纳米粒子，并采用紫外可见光谱、红外光谱、分析电镜、X光能谱、X射线衍射等技术对催化剂进行了深入研究。电化学及单池性能测试结果表明，表层富铂的PtSn纳米粒子对乙醇电氧化具有更好的催化活性，其作为阳极催化剂的直接乙醇燃料电池单池性能达到80mW cm~(-2)，比相同操作条件下文献报道的最高值高约一倍。对自制铂基催化剂组装的DEFC单池进行了稳定性测试，分析性能衰减的原因。
采用二氯二乙二胺合铂和硝基硝酰钌为前驱体，利用浸渍氢还原法制备了PtRu／C催化剂，并将其甲醇氧化活性与商品PtRu催化剂进行了比较，发现催化剂对甲醇电氧化活性随PtRu合金度的增大而提高。
开发了全氟磺酸离子交联聚合物(PFSt)稳定的Pt胶体及Pt／C催化剂，其作为DMFC阴极的性能要远高于PTFE为稳定剂的催化剂。
Direct alcohol fuel cells have gained amount of attentions within the last years due to its high power density, simple operation, and portability. As a green and renewable fuel, ethanol is less toxic and is available from crop ferment. However, the complete electrooxidation of ethanol involves the transfer of 12 electronics and 12 protons arising from not only dehydrogenation but cleavage of C-C bonds. The electrooxidation process of ethanol, resulting to more by-products, is much more complex than methanol. This makes the development of anode electrocatalysts for ethanol electrooxidation a great challenge task.
PtSn/C electrocatalyst was prepared by three methods and the results show that the modified polyol method is suitable for preparing high metal-loading nanocatalysts with uniform distribution and small particle size. The synthesis parameters, including tin precursors, Pt/Sn atomic ratio, reduction temperature, and the post treatment atmosphere, etc., were investigated in detail. Employing X-ray Diffraction and Analysis Electron Microscopy, the effect of Sn and Ru on the variation of the Pt lattice parameter was studied. The relationship between the structure of PtSn and PtRu nanoparticles and their catalytic activity on ethanol electrooxidation was studied. It was found that PtSn/C with the dilated lattice parameter of Pt showed higher activity for ethanol electrooxidation than PtRu/C with the contracted Pt lattice parameter.
On the basis of the controllable synthesis of SnO_2 nanopartilces, three kinds
引文
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32．梁振兴，直接甲醇燃料电池Nafion膜的红外光谱表征和阻醇质子交换膜的研究，大连化学物理研究所硕士学位论文，2004