Department of Chemical Engineering and Biotechnology , University of Cambridge , Philippa Fawcett Drive, West Site , CB3 0AS Cambridge , U.K.
Phillips 66 Research Center , Highway 60 & 123, Bartlesville , Oklahoma 74003-6607 , United States.
Environ Sci Technol. 2019 Apr 2;53(7):3538-3546. doi: 10.1021/acs.est.8b06861. Epub 2019 Mar 21.
In this work, we investigate the molecular composition and nanostructure of gasification charcoal (biochar) by comparing it with heat-treated fullerene arc-soot. Using ultrahigh resolution Fourier transform ion-cyclotron resonance and laser desorption ionization time-of-flight mass spectrometry, Raman spectroscopy, and high resolution transmission electron microscopy we analyzed charcoal of low tar content obtained from gasification. Mass spectrometry revealed no magic number fullerenes such as C or C in the charcoal. The positive molecular ion m/ z 701, previously considered a graphitic part of the nanostructure, was found to be a breakdown product of pyrolysis and not part of the nanostructure. A higher mass distribution of ions similar to that found in thermally treated fullerene soot indicates that they share a nanostructure. Recent insights into the formation of all carbon fullerenes reveal that conditions in charcoal formation are not optimal for the formation of fullerenes, but instead, curved carbon structures coalesce into fulleroid-like structures. Microscopy and spectroscopy support such a stacked, fulleroid-like nanostructure, which was explored using reactive molecular dynamics simulations.
在这项工作中，我们通过将其与热处理富勒烯电弧烟尘进行比较，研究了气化炭（生物炭）的分子组成和纳米结构。我们使用超高分辨率傅里叶变换离子回旋共振和激光解吸电离飞行时间质谱、拉曼光谱和高分辨率透射电子显微镜分析了从气化中获得的低焦油含量的木炭。质谱分析显示，木炭中没有 C 或 C 等魔术数富勒烯。先前被认为是纳米结构石墨部分的正分子离子 m/z 701 被发现是热解的分解产物，而不是纳米结构的一部分。与在热处理富勒烯烟尘中发现的类似的更高质量分布的离子表明它们具有相似的纳米结构。最近对所有碳富勒烯形成的研究表明，在木炭形成过程中的条件不利于富勒烯的形成，而是弯曲的碳结构聚合并融合成类富勒烯结构。显微镜和光谱学支持这种堆叠的类富勒烯纳米结构，使用反应分子动力学模拟对其进行了探索。
