Liang Xuan, Jin Xiangxin, Yu Shixiang, Li Chengyu, Song Chuqiao, Sheng Guan, Ye Xuemin, Gao Rui, Lin Lili, Ma Ding
Beijing National Laboratory for Molecular Science, New Cornerstone Science Laboratory, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014, China.
Nat Commun. 2025 May 5;16(1):4159. doi: 10.1038/s41467-025-59321-0.
"Hydrogenation by crude H - dehydrogenation to produce pure H" strategy using liquid organic hydrogen carriers (LOHCs) can reduce the cost and shorten the process of hydrogen purification and utilization. The critical challenge is to eliminate catalyst poisoning by CO impurity in crude H. Here, we develop a Pd/α-MoC catalyst that enables efficient hydrogenation of N-LOHCs under crude hydrogen feeds (CO concentration>5 vol%) below 150 °C, and has an activity 1-2 orders of magnitude higher than that of traditional Pd-based catalysts. The CO-resistant hydrogenation is also successfully conducted in the models of industrial crude H including CO, CO and CH. Water, as solvent, contributes greatly to the hydrogenation activity against CO poisoning, since the utilization of low-temperature water gas shift (WGS) reaction. Moreover, the positive-charged Pd species hinder the combination of H* from WGS reaction and suppressed the undesirable H formation and release, which explains the substantial improvement in the performance of Pd/α-MoC compared to that of Pt/α-MoC.
使用液态有机氢载体(LOHCs)的“通过粗氢气脱氢制纯氢的加氢”策略可以降低成本并缩短氢气纯化和利用的过程。关键挑战在于消除粗氢气中CO杂质导致的催化剂中毒。在此,我们开发了一种Pd/α-MoC催化剂,该催化剂能够在低于150°C的粗氢气进料(CO浓度>5 vol%)下实现N-LOHCs的高效加氢,并且活性比传统Pd基催化剂高1-2个数量级。在包括CO、CO和CH的工业粗氢气模型中也成功进行了抗CO加氢。水作为溶剂,由于利用了低温水煤气变换(WGS)反应,对抵抗CO中毒的加氢活性有很大贡献。此外,带正电荷的Pd物种阻碍了WGS反应中H*的结合,并抑制了不希望的H的形成和释放,这解释了与Pt/α-MoC相比,Pd/α-MoC性能的大幅提升。