Acknowledged as an ideal method for in situ hydrogen generation, methanol steam reforming (MSR) requires high-performance catalysts to enhance production efficiency. Herein, we prepared a series of Zr-modified Cu-based catalysts by a coprecipitation method and conducted a systematic analysis of the impacts of structural variations on MSR performance. Extensive characterization reveals a strong dependence of the catalyst’s surface structure on Zr content. Introducing a moderate amount of Zr to the Cu/ZnO catalysts forms ZnZrOx solid solution and increases Cu dispersion, forming more Cu-ZnZrOx and Cu-ZnO interfacial sites with higher H2 production rate. Further increases in Zr content enlarge Cu nanoparticles and multiply Cu-ZrO2 interfacial sites. The optimal catalyst with a Zn/Zr molar ratio of 5, with the richest Cu-ZnO/Cu-ZnZrOx interfacial sites, achieves the highest H2 production rate of 117.4 mmolH2gcat-1h-1 at 200 °C, which is 1.3 times and 6.8 times higher than those of Cu/ZnO and Cu/ZrO2, respectively.

中文翻译：

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甲醇水蒸气重整过程中锆改性铜基催化剂的构效关系


甲醇蒸汽重整（MSR）被认为是原位制氢的理想方法，需要高性能催化剂来提高生产效率。在此，我们通过共沉淀法制备了一系列Zr改性的铜基催化剂，并系统分析了结构变化对MSR性能的影响。广泛的表征揭示了催化剂的表面结构对 Zr 含量的强烈依赖性。在Cu/ZnO催化剂中引入适量的Zr形成ZnZrOx固溶体并增加Cu分散度，形成更多的Cu-ZnZrOx和Cu-ZnO界面位点，从而具有更高的H2产率。 Zr含量的进一步增加扩大了Cu纳米颗粒并增加了Cu-ZrO2界面位点。 Zn/Zr摩尔比为5的最优催化剂，具有最丰富的Cu-ZnO/Cu-ZnZrOx界面位点，在200 ℃时实现最高产氢率117.4 mmolH2gcat-1h-1，分别是1.3倍和6.8倍。分别比 Cu/ZnO 和 Cu/ZrO2 高 1 倍。