Ding Qiuyue, Zhang Yixuan, Wei Huijie, Li Qing, Xi Yanyan, Hu Songqing, Lin Xufeng
College of Material Science and Engineering, China University of Petroleum (East China) 266580 Qingdao P. R. China
College of Chemistry and Chemical Engineering, China University of Petroleum (East China) 266580 Qingdao P. R. China
RSC Adv. 2025 Apr 7;15(14):10700-10710. doi: 10.1039/d5ra00385g. eCollection 2025 Apr 4.
Precious metal catalysts are widely used in the field of heterogeneous catalysis in general and, in particular, for the dehydrogenation process of liquid organic hydrogen carriers (LOHCs). However, improving their catalytic activity and selectivity simultaneously is challenging owing to the characteristics of transition metals. Herein, a catalyst, namely, PtCu/AlO-H, was developed that could break the negative correlation between catalytic activity and selectivity, improving the overall dehydrogenation performance and reducing costs. This method achieved highly dispersed nanoparticles (NPs) and co-localization to form a unique PtCu alloy with reduced Pt electron density by anchoring low loadings of Cu-doped Pt on an alumina support. It also suppressed strong metal support interactions (SMSIs), as confirmed by characterization results such as XPS and HRTEM, resulting in excellent bimetallic synergistic catalytic dehydrogenation activity and selectivity in perhydromonobenzyltoluene (12H-MBT), compared with Pt/AlO-H. The reaction energy barrier for the dehydrogenation of 12H-MBT was relatively low (∼94 kJ mol), and the rate-determining step of the whole catalytic dehydrogenation was identified to be 4H-MBT → 0H-MBT.
贵金属催化剂在多相催化领域广泛应用，尤其是用于液态有机氢载体（LOHCs）的脱氢过程。然而，由于过渡金属的特性，同时提高其催化活性和选择性具有挑战性。在此，开发了一种名为PtCu/AlO-H的催化剂，它能够打破催化活性与选择性之间的负相关关系，提高整体脱氢性能并降低成本。该方法通过将低负载量的铜掺杂铂锚定在氧化铝载体上，实现了高度分散的纳米颗粒（NPs）和共定位，形成了具有降低的铂电子密度的独特PtCu合金。正如XPS和HRTEM等表征结果所证实的，它还抑制了强金属-载体相互作用（SMSIs），与Pt/AlO-H相比，在全氢单苄基甲苯（12H-MBT）中产生了优异的双金属协同催化脱氢活性和选择性。12H-MBT脱氢的反应能垒相对较低（约94 kJ/mol），并且确定整个催化脱氢的速率决定步骤为4H-MBT → 0H-MBT。
