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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >UV Photofragmentation and IR Spectroscopy of Cold, G-Type beta-O-4 and beta-beta Dilignol-Alkali Metal Complexes: Structure and Linkage-Dependent Photofragmentation
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UV Photofragmentation and IR Spectroscopy of Cold, G-Type beta-O-4 and beta-beta Dilignol-Alkali Metal Complexes: Structure and Linkage-Dependent Photofragmentation

机译：紫外光碎裂和冷G型β-O-4和β-β地尼诺尔碱金属配合物的红外光谱：结构和链接依赖的光碎裂

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摘要

Ultraviolet photofragmentation spectroscopy and infrared spectroscopy were performed on two prototypical guaiacyl (G)-type dilignols containing beta-O-4 and beta beta linkages, complexed with either lithium or sodium cations. The complexes were generated by nanoelectrospray ionization, introduced into a multistage mass spectrometer, and subsequently cooled in a 22-pole cold ion trap to T similar to 10 K. A combination of UV photofragment spectroscopy and IR-UV double resonance spectroscopy was used to characterize the preferred mode of binding of the alkali metal cations and the structural changes so induced. Based on a combination of spectral evidence provided by the UV and IR spectra, the Li+ and Na+ cations are deduced to preferably bind to both dilignols via their linkages, which constitute unique, oxygen-rich binding pockets for the cations. The UV spectra reflect this binding motif in their extensive FranckCondon activity involving low-frequency puckering motions of the linkages in response to electronic excitation. In the pinoresinol center dot Li+/Na+ complexes involving the beta beta linkage, the spectra also showed an inherent spectral broadening. The photofragment mass spectra are unique for each dilignol center dot Li+/Na+ complex, many of which are also complementary to those produced by collision-induced dissociation (CID), indicating the presence of unique excited state processes that direct the fragmentation. These results suggest the potential for site-selective fragmentation and for uncovering fragmentation pathways only accessed by resonant UV excitation of cold lignin ions.
机译：在两个含有β-O-4和β-β键并与锂或钠阳离子络合的原型愈创木脂（G）型二木酚上进行了紫外光碎裂光谱和红外光谱分析。通过纳米电喷雾电离生成复合物，将其引入多级质谱仪中，然后在22极冷离子阱中冷却至类似于10 K的T。使用紫外光碎裂光谱法和IR-UV双共振光谱法进行表征碱金属阳离子结合的优选方式和由此引起的结构变化。基于由UV和IR光谱提供的光谱证据的组合，推导Li +和Na +阳离子优选地通过它们的键合而结合到两个二戊醇，这构成了阳离子的独特的，富氧的结合口袋。紫外线光谱在其广泛的FranckCondon活性中反映了这种结合基序，涉及到响应电子激发而产生的键的低频起皱运动。在涉及β-β键的松脂醇中心点Li + / Na +络合物中，光谱还显示出固有的光谱展宽。每个dilignol中心点Li + / Na +配合物的光致碎裂质谱都是唯一的，其中许多也与碰撞诱导解离（CID）产生的质谱互补，表明存在指导断裂的独特激发态过程。这些结果表明了位点选择性裂解和揭示裂解途径的潜力，这些途径只有通过冷木质素离子的共振紫外线激发才能进入。

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