Si Yang, Jiao Yueyue, Wang Maolin, Xiang Shengling, Diao Jiangyong, Chen Xiaowen, Chen Jiawei, Wang Yue, Xiao Dequan, Wen Xiaodong, Wang Ning, Ma Ding, Liu Hongyang
School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, 110016, PR China.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, PR China.
Nat Commun. 2024 Jun 7;15(1):4887. doi: 10.1038/s41467-024-49083-6.
For di-nitroaromatics hydrogenation, it is a challenge to achieve the multi-step hydrogenation with high activity and selectivity due to the complexity of the process involving two nitro groups. Consequently, many precious metal catalysts suffer from low activity for this multi-step hydrogenation reaction. Herein, we employ a fully exposed Pt clusters catalyst consisting of an average of four Pt atoms on nanodiamond@graphene (Pt/ND@G), demonstrating excellent catalytic performance for the multi-step hydrogenation of 2,4-dinitrotoluene. The TOF (40647 h) of Pt/ND@G is significantly superior to that of single Pt atoms catalyst, Pt nanoparticles catalyst, and even all the known catalysts. Density functional theory calculations and absorption experiments reveal that the synergetic interaction between the multiple active sites of Pt/ND@G facilitate the co-adsorption/activation of reactants and H, as well as the desorption of intermediates/products, which is the key for the higher catalytic activity than single Pt atoms catalyst and Pt nanoparticles catalyst.
对于二硝基芳烃的氢化反应，由于涉及两个硝基的过程复杂，要实现具有高活性和选择性的多步氢化是一项挑战。因此，许多贵金属催化剂在这种多步氢化反应中活性较低。在此，我们采用了一种完全暴露的铂簇催化剂，其由平均四个铂原子组成，负载于纳米金刚石@石墨烯（Pt/ND@G）上，该催化剂对2,4-二硝基甲苯的多步氢化反应表现出优异的催化性能。Pt/ND@G的TOF（40647 h）显著优于单原子铂催化剂、铂纳米颗粒催化剂，甚至优于所有已知催化剂。密度泛函理论计算和吸附实验表明，Pt/ND@G多个活性位点之间的协同相互作用促进了反应物和氢气的共吸附/活化，以及中间体/产物的脱附，这是其催化活性高于单原子铂催化剂和铂纳米颗粒催化剂的关键。
