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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 n /ND@G), demonstrating excellent catalytic performance for the multi-step hydrogenation of 2,4-dinitrotoluene. The TOF (40647 h -1 ) of Pt n /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 n /ND@G facilitate the co-adsorption/activation of reactants and H 2 , 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., (© 2024. The Author(s).)

Solid surfaces usually reach thermodynamic equilibrium through particle exchange with their environment under reactive conditions. A prerequisite for understanding their functionalities is detailed knowledge of the surface composition and atomistic geometry under working conditions. Owing to the large number of possible Miller indices and terminations involved in multielement solids, extensive sampling of the compositional and conformational space needed for reliable surface energy estimation is beyond the scope of ab initio calculations. Here, we demonstrate, using the case of iron carbides in environments with varied carbon chemical potentials, that the stable surface composition and geometry of multielement solids under reactive conditions, which involve large compositional and conformational spaces, can be predicted at ab initio accuracy using an approach that combines the bond valence model, Gaussian process regression, and ab initio thermodynamics. Determining the atomistic structure of surfaces under working conditions paves the way toward identifying the true active sites of multielement catalysts in heterogeneous catalysis., Competing Interests: The authors declare no competing interests., (© 2024 The Authors.)

Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalyst as the bridge between homogeneous and heterogeneous catalysis, which displays an outstanding catalytic performance for n-butane dehydrogenation, with a remarkable n-butane reaction rate (8.8 mol·g Ir -1 ·h -1 ) and high butene selectivity (95.6%) at low temperature (450 °C). Significantly, we correlate the BDH activity with the Ir species from nanoscale to sub-nanoscale, to reveal the nature of structure-dependence of catalyst. Moreover, we compare Ir single atoms with Pt single atoms and Pd single atoms for in-depth understanding the nature of metal-dependence at the atomic level. From experimental and theoretical calculations results, the isolated Ir site is suitable for both reactant adsorption/activation and product desorption. Its remarkable dehydrogenation capacity and moderate adsorption behavior are the key to the outstanding catalytic activity and selectivity., (© 2023. The Author(s).)

In this study, a series of Co nanoparticles (NPs) with different sizes and Co single-atom catalysts (SACs) with different cobalt-nitrogen coordination numbers (Co-N 2 , Co-N 3 , and Co-N 4 ) were synthesized and applied to the synthesis of ammonia catalyzed by plasma at low temperatures and atmospheric pressures. Under the same reaction conditions, the yield of nitrogen obtained from the reduction to ammonia over a series of Co NP catalysts varies with the Co particle size. The smaller the size of the Co NPs, the greater the number of exposed active centers, and the catalytic activity is higher. Among the Co SACs, the best catalyst was Co-N 2 with two coordinated nitrogen atoms, and the ammonia yield was 181 mg·h -1 ·g cat -1 . The experimental and theoretical calculations were consistent in that a low Co-N coordination number was beneficial to the adsorption and dissociation of N 2 , thereby enhancing the reduction activity of N 2 and promoting the increase of ammonia production.