摘要：Adsorption and activation of dinitrogen(N_(2)) is an indispensable process in nitrogen *** nitride species continue to attract attention as a promsing catalyst for ammonia ***,the detailed mechanisms at a molecular level between reactive nitride species and N_(2) remain unclear at elevated temperature,which is important to understand the temperature effect and narrow the gap between the gas phase system and condensed phase ***,the ^(15)N/^(14)N isotopic exchange in the reaction between tantalum nitride cluster anions Ta_(3)^(14)N_(3)^(-) and ^(15)N_(2) leading to the regeneration of ^(14)N_(2)/^(14)N^(15)N was observed at elevated temperature(393-593 K)using mass *** the aid of theoretical calculations,the exchange mechanism and the effect of temperature to promote the dissociation of N_(2) on Ta_(3)N_(3)^(-) were elucidated.A comparison experiment for Ta_(3)^(14)N_(4)^(-)/^(15)N_(2) couple indicated that only desorption of ^(15)N_(2) from Ta_(3)^(14)N_(4)^(15)N_(2)^(-) took place at elevated *** different exchange behavior can be well understood by the fact that nitrogen vacancy is a requisite for the dinitrogen activation over metal nitride *** study may shed light on understanding the role of nitrogen vacancy in nitride species for ammonia synthesis and provide clues in designing effective catalysts for nitrogen fixation.

摘要：This review summarizes a variety of experimentally identified gas‐phase catalytic cycles,all of which are mediated by atomic metal ions,bare metal clusters,metal oxide clusters or metal *** is placed on the latest advances in the unique catalytic reactivity of cluster‐confined single noble metal *** cycles discussed in this paper cover a wide range of inorganic and organic *** use of start‐of‐the‐art mass spectrometric instrumentation in conjunction with quantum chemistry calculations is also reported,as these techniques have determined the mechanistic details of the elementary steps of such catalytic *** important role of gas‐phase data in guiding the rational design of better‐performing catalysts in related condensed phase reactions is also *** particular,this review focuses on the following three topics:(1)the catalytic oxidation of carbon monoxide,(2)the catalytic functionalization of methane,and(3)catalytic decarboxylation.

摘要：Computational design of proteins is a relatively new field, where scientists search the enormous sequence space for sequences that can fold into desired structure and perform desired functions. With the computational approach, proteins can be designed, for example, as regulators of biological processes, novel enzymes, or as biotherapeutics. These approaches not only provide valuable information for understanding of sequence-structure-function relations in proteins, but also hold promise for applications to protein engineering and biomedical research. In this review, we briefly introduce the rationale for computational protein design, then summarize the recent progress in this field, including de novo protein design, enzyme design, and design of protein-protein interactions. Challenges and future prospects of this field are also discussed.