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首页> 外文期刊>Topics in Catalysis >Selective production of hydrogen for fuel cells via oxidative steam reforming of methanol over CuZnAl oxide catalysts: effect of substitution of zirconium and cerium on the catalytic performance
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Selective production of hydrogen for fuel cells via oxidative steam reforming of methanol over CuZnAl oxide catalysts: effect of substitution of zirconium and cerium on the catalytic performance

机译：在CuZnAl氧化物催化剂上通过甲醇的氧化蒸汽重整，选择性地生产燃料电池氢：锆和铈的取代对催化性能的影响

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摘要

H_2 fuel, for fuel cells, is traditionally produced from methanol by the endothermic steam reforming of methanol (SRM). Partial oxidation of methanol (POM), which is highly exothermic, has also been suggested as a route to extract H_2 from methanol. In both these reactions a considerable amount of CO is produced as a byproduct, which is a poison to the Pt anode of the fuel cell. A combined steam reforming and partial oxidation of methanol, which has been termed "oxidative steam reforming of methanol" (OSRM), reported recently is considered to be more efficient and convenient for the selective production of H_2 at a relatively low temperature. The catalysts used in the OSRM reaction were CuZnAl mixed oxides derived from hydroxycarbonate precursors containing hydrotalcite (HT)-like layered double hydroxides (LDHs)/aurichalcite phases. Substitution of Zr for Al in the CuZnAl oxide system was found to improve the catalytic performance. In the present study, the role of added Zr was investigated in detail by employing spectroscopic methods such as X-ray diffraction (XRD), temperature-programmed reduction (TPR), electron paramagnetic resonance (EPR) spectroscopy, X-ray photoelectron spectroscopy (XPS) and X-ray induced Auger electron spectroscopy (AES). The detailed spectroscopic studies revealed that substitution of Zr and for Al improved the reducibility and dispersion of copper species due to the operation of a synergistic interaction between copper and zirconium as a consequence of the formation of a "Cu~(2+) - O-Zr~(4+) - O-" solid solution. The higher catalytic performance of CuZn-based catalysts containing Zr in the OSRM reaction was attributed to the ease of reducibility and enhanced dispersion of copper particles on the support. The substitution of Ce in the CuZnAl system, on the other hand,did not alter the catalytic performance greatly.
机译：传统上，用于燃料电池的H_2燃料是通过甲醇的吸热蒸汽重整（SRM）由甲醇制成的。甲醇（POM）的高度放热也被认为是从甲醇中提取H_2的途径。在这两个反应中，都会产生大量的副产品CO，这对燃料电池的Pt阳极是有毒的。最近被报道的被称为“甲醇的氧化蒸汽重整”（OSRM）的甲醇的蒸汽重整和部分氧化的组合被认为在相对较低的温度下选择性地生产H_2更有效和方便。 OSRM反应中使用的催化剂是衍生自包含类水滑石（HT）的层状双氢氧化物（LDHs）/金铝石相的羟基碳酸盐前体的CuZnAl混合氧化物。发现Zr取代CuZnAl氧化物体系中的Al可改善催化性能。在本研究中，通过采用X射线衍射（XRD），程序升温还原（TPR），电子顺磁共振（EPR）光谱，X射线光电子能谱（ XPS）和X射线诱导俄歇电子能谱（AES）。详细的光谱研究表明，由于形成了“ Cu〜（2+）-O-”，因此铜和锆之间的协同相互作用的作用使Zr和Al的取代提高了铜的还原性和分散性。 Zr〜（4+）-O-“固溶体。在OSRM反应中，含Zr的CuZn基催化剂的较高催化性能归因于易还原性和铜颗粒在载体上的分散性增强。另一方面，CeZn在CuZnAl体系中的取代并没有极大地改变催化性能。

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