The nature of interfacial catalysis over Pt/NiAl2O4: Effects of metal identity and CO tolerance in hydrogen production from methanol reforming reaction

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-12-24 DOI:10.1016/j.jcat.2024.115923
Xiuyi Wang, Hongbo Zhang
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Abstract

In this study, we investigate the effect of interfacial structure on the methanol steam reforming (MSR) reaction by systematically varying the transition metals (Pt, Ru, Rh, Pd, and Ir) over a NiAl2O4 support. At similar methanol conversions at ∼ 5 %, H2 formation exhibits superior reaction performance at ∼ 0.14 molH2·molmetal-1·s−1 over Pt/NiAl2O4 than any other counter parts, which was attributed to the enhanced ability in tolerance of CO from catalytic surface and the greater ability in CH3O– activation with the activation energies of MSR, methanol dehydrogenation (MD), and water-gas shift (WGS) reaction at 70 kJ/mol, 79 kJ/mol, and 97 kJ/mol, respectively, which is obviously smaller than the other transition metal catalysts. More importantly, the higher reduction degree of Pt and more stabilized transition state along methanol activation might be additional reasons for this superior reaction performance on H2 formation.

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Pt/NiAl2O4界面催化性质:金属同一性和CO耐受性对甲醇重整制氢反应的影响
在本研究中,我们通过系统地改变NiAl2O4载体上的过渡金属(Pt, Ru, Rh, Pd和Ir)来研究界面结构对甲醇蒸汽重整(MSR)反应的影响。在相似的甲醇转化率为 ~ 5 %时,Pt/NiAl2O4在 ~ 0.14 molH2·molmetal-1·s−1上的反应性能优于其他任何对应组分,这是由于其对CO和催化表面的耐受能力增强,以及对ch30 -的活化能力更强,MSR、MD和WGS的活化能分别为70 kJ/mol、79 kJ/mol和97 kJ/mol,明显小于其他过渡金属催化剂。更重要的是,Pt的高还原度和更稳定的过渡态沿甲醇活化可能是这种优越的H2生成性能的另一个原因。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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