Rapid, low-temperature nanodiamond formation by electron-beam activation of adamantane C–H bonds

IF 45.8 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Science Pub Date : 2025-09-04 DOI:10.1126/science.adw2025
Jiarui Fu, Takayuki Nakamuro, Eiichi Nakamura
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引用次数: 0

Abstract

Diamond and adamantane (Ad) share a Td-symmetric carbon skeleton, but converting Ad to diamond has been challenging because it requires selective carbon-hydrogen (C–H) bond cleavage and monomer assembly into a diamond lattice. Our approach differs from the conventional high-temperature, high-pressure diamond syntheses. We electron-irradiated Ad submicrocrystals at 80 to 200 kilo–electron volts and 100 to 296 kelvin in vacuum for tens of seconds. This process yielded defect-free nanodiamonds (NDs) of cubic crystal structure, accompanied by hydrogen gas evolution. Time-resolved transmission electron microscopy revealed the initial formation of Ad oligomers transforming into spherical NDs. A sizable kinetic isotope effect indicates that C–H cleavage was rate-determining, and other hydrocarbons tested failed to form NDs.
通过电子束激活金刚烷C-H键快速、低温形成纳米金刚石
金刚石和金刚烷(Ad)共享一个td对称的碳骨架,但将Ad转化为金刚石一直具有挑战性,因为它需要选择性的碳氢键(C-H)裂解和单体组装成金刚石晶格。我们的方法不同于传统的高温高压金刚石合成。我们在真空中以80至200千电子伏特和100至296开尔文的温度对Ad亚微晶体进行数十秒的电子辐照。该工艺制备了立方晶体结构的无缺陷纳米金刚石(NDs),并伴有氢气的析出。时间分辨透射电镜显示Ad低聚物的初始形成转化为球形nd。相当大的动力学同位素效应表明,C-H裂解是速率决定的,而测试的其他碳氢化合物不能形成nd。
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来源期刊
Science
Science 综合性期刊-综合性期刊
CiteScore
61.10
自引率
0.90%
发文量
0
审稿时长
2.1 months
期刊介绍: Science is a leading outlet for scientific news, commentary, and cutting-edge research. Through its print and online incarnations, Science reaches an estimated worldwide readership of more than one million. Science’s authorship is global too, and its articles consistently rank among the world's most cited research. Science serves as a forum for discussion of important issues related to the advancement of science by publishing material on which a consensus has been reached as well as including the presentation of minority or conflicting points of view. Accordingly, all articles published in Science—including editorials, news and comment, and book reviews—are signed and reflect the individual views of the authors and not official points of view adopted by AAAS or the institutions with which the authors are affiliated. Science seeks to publish those papers that are most influential in their fields or across fields and that will significantly advance scientific understanding. Selected papers should present novel and broadly important data, syntheses, or concepts. They should merit recognition by the wider scientific community and general public provided by publication in Science, beyond that provided by specialty journals. Science welcomes submissions from all fields of science and from any source. The editors are committed to the prompt evaluation and publication of submitted papers while upholding high standards that support reproducibility of published research. Science is published weekly; selected papers are published online ahead of print.
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