Department of Chemistry, University of California, Berkeley, California 94720, United States.
J Am Chem Soc. 2011 Feb 23;133(7):2108-11. doi: 10.1021/ja110798w. Epub 2011 Feb 2.
Nitrous oxide (N(2)O), a widespread greenhouse gas, is a thermodynamically potent and environmentally green oxidant that is an attractive target for activation by metal centers. However, N(2)O remains underutilized owing to its high kinetic stability, and the poor ligand properties of this molecule have made well-characterized metal-N(2)O complexes a rarity. We now report a vanadium-pyrrolide system that reversibly binds N(2)O at room temperature and provide the first single-crystal X-ray structure of such a complex. Further characterization by vibrational spectroscopy and DFT calculations strongly favor assignment as a linear, N-bound metal-N(2)O complex.
一氧化二氮(N(2)O),一种广泛存在的温室气体,是一种热力学上有效的、环境友好的氧化剂,是金属中心激活的有吸引力的目标。然而,由于其高动力学稳定性,N(2)O 的利用率仍然很低,并且该分子的配体性质较差,使得特征明确的金属-N(2)O 配合物非常罕见。我们现在报告了一个钒-吡咯烷系统,该系统在室温下可逆地结合 N(2)O,并提供了第一个此类配合物的单晶 X 射线结构。通过振动光谱和 DFT 计算进一步表征强烈支持其作为线性、N 键合的金属-N(2)O 配合物的分配。