质子交换膜燃料电池抗CO电催化剂的研究
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摘要
PtRu/C催化剂是目前应用最广泛的质子交换膜燃料电池(PEMFCs)抗CO阳极电催化剂,但其性能仍不能满足PEMFCs商业化的要求。本论文从载体、活性组分和制备方法等三个方面对PEMFCs抗CO电催化剂进行了系统研究。
首先,以多壁碳纳米管(MWCNTs)为载体制备了PtRu/MWCNTs催化剂,利用N2吸附、TEM、XRD、ICP、FTIR和TPD-MS等多种表征手段,深入研究了载体经不同浓度H_2O_2处理以及制备催化剂所用溶剂(乙二醇和水)对催化剂的担载量和粒子分散性以及电池抗CO性能的影响,首次提出了溶剂极性和碳纳米管表面化学相结合是最重要的影响因素,并通过直接测量载体在溶剂中的润湿热以及载体表面含氧官能团进行了验证。
其次,开发了微波辅助乙二醇还原并热处理的方法制备了PtRuIr/C和PtRuNi/C催化剂。CO溶出伏安、单电池评价和阳极进出口气体气相色谱分析等测试表明,两者具有很高抗CO氢氧化活性。在与采用相同方法制备的PtRu/C催化剂对比的前提下,详细研究了加入Ir和Ni对催化剂粒子形貌、粒子大小和分布、组成均匀性以及体相结构等的影响,在此基础上结合XPS表征深入探讨了催化剂结构-性能的关系,并提出了催化剂性能增强的机理。
此外,本论文还开发了简单、低成本且完全水相的真空浸渍法制备PtRu/C催化剂,考察并优化了制备过程中的若干因素,对该催化剂进行的CO溶出伏安、单电池评价以及阳极进出口气体气相色谱分析等测试表明,利用这个方法制备的PtRu/C催化剂具有高于商品PtRu/C催化剂的抗CO性能。
PtRu/C is now recognized as the most promising CO-tolerant anode electrocatalyst for proton exchange membrane fuel cells (PEMFCs). However, the modified performance by PtRu/C is still not good enough for the commercialization of PEMFCs, and more active CO-tolerant electrocatalysts are critically needed for the practical application of this technology. In this paper, intensive study, in which the support, the active components and the synthesis strategy were involved, were carried out.
Firstly, A series of PtRu nanocomposites supported on H_2O_2-oxidized multi-walled carbon nanotubes (MWCNTs) were synthesized via two chemical reduction methods—the HCHO method and the EG method. The effects of the solvents (water and ethylene glycol) and the surface composition of the MWCNTs on the deposition and the dispersion of the metal particles were investigated through N2 adsorption, TEM, ICP, FTIR, TPD-MS and the measurements of the wetting heats of the MWCNTs in the corresponding solvents. The characterizations suggested that combination of the surface chemistry of the MWCNTs with the polarity of the solvents was the most important factor. Evaluations of the catalysts at the anode of the single PEMFCs were conducted. Structure–performance relationship of the PtRu/MWCNTs catalysts were also studied.
Secondly, the PtRuIr/C and PtRuNi/C catalysts were synthesized via a microwave-irradiated polyol plus annealing (MIPA) synthesis strategy. The catalysts were characterized by TEM, XRD, ICP, EDS, CO-stripping voltammetry, single cell
首先,以多壁碳纳米管(MWCNTs)为载体制备了PtRu/MWCNTs催化剂,利用N2吸附、TEM、XRD、ICP、FTIR和TPD-MS等多种表征手段,深入研究了载体经不同浓度H_2O_2处理以及制备催化剂所用溶剂(乙二醇和水)对催化剂的担载量和粒子分散性以及电池抗CO性能的影响,首次提出了溶剂极性和碳纳米管表面化学相结合是最重要的影响因素,并通过直接测量载体在溶剂中的润湿热以及载体表面含氧官能团进行了验证。
其次,开发了微波辅助乙二醇还原并热处理的方法制备了PtRuIr/C和PtRuNi/C催化剂。CO溶出伏安、单电池评价和阳极进出口气体气相色谱分析等测试表明,两者具有很高抗CO氢氧化活性。在与采用相同方法制备的PtRu/C催化剂对比的前提下,详细研究了加入Ir和Ni对催化剂粒子形貌、粒子大小和分布、组成均匀性以及体相结构等的影响,在此基础上结合XPS表征深入探讨了催化剂结构-性能的关系,并提出了催化剂性能增强的机理。
此外,本论文还开发了简单、低成本且完全水相的真空浸渍法制备PtRu/C催化剂,考察并优化了制备过程中的若干因素,对该催化剂进行的CO溶出伏安、单电池评价以及阳极进出口气体气相色谱分析等测试表明,利用这个方法制备的PtRu/C催化剂具有高于商品PtRu/C催化剂的抗CO性能。
PtRu/C is now recognized as the most promising CO-tolerant anode electrocatalyst for proton exchange membrane fuel cells (PEMFCs). However, the modified performance by PtRu/C is still not good enough for the commercialization of PEMFCs, and more active CO-tolerant electrocatalysts are critically needed for the practical application of this technology. In this paper, intensive study, in which the support, the active components and the synthesis strategy were involved, were carried out.
Firstly, A series of PtRu nanocomposites supported on H_2O_2-oxidized multi-walled carbon nanotubes (MWCNTs) were synthesized via two chemical reduction methods—the HCHO method and the EG method. The effects of the solvents (water and ethylene glycol) and the surface composition of the MWCNTs on the deposition and the dispersion of the metal particles were investigated through N2 adsorption, TEM, ICP, FTIR, TPD-MS and the measurements of the wetting heats of the MWCNTs in the corresponding solvents. The characterizations suggested that combination of the surface chemistry of the MWCNTs with the polarity of the solvents was the most important factor. Evaluations of the catalysts at the anode of the single PEMFCs were conducted. Structure–performance relationship of the PtRu/MWCNTs catalysts were also studied.
Secondly, the PtRuIr/C and PtRuNi/C catalysts were synthesized via a microwave-irradiated polyol plus annealing (MIPA) synthesis strategy. The catalysts were characterized by TEM, XRD, ICP, EDS, CO-stripping voltammetry, single cell
引文
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