Li Linfeng, Vozniuk Olena, Cao Zhengwen, Losch Pit, Felderhoff Michael, Schüth Ferdi
Department of Heterogeneous Catalysis, Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.
Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao Key Laboratory of Functional Membrane Material and Membrane Technology, No.189 Songling Road, 266101, Qingdao, China.
Nat Commun. 2023 Aug 29;14(1):5257. doi: 10.1038/s41467-023-40915-5.
The conversion of carbon-based solids, like non-recyclable plastics, biomass, and coal, into small molecules appears attractive from different points of view. However, the strong carbon-carbon bonds in these substances pose a severe obstacle, and thus-if such reactions are possible at all-high temperatures are required. The Bergius process for coal conversion to hydrocarbons requires temperatures above 450 °C, pyrolysis of different polymers to pyrolysis oil is also typically carried out at similar temperatures. We have now discovered that efficient hydrogenation of different solid substrates with the carbon-based backbone to light hydrocarbons can be achieved at room temperature by ball milling. This mechanocatalytic method is surprisingly effective for a broad range of different carbon substrates, including even diamond. The reaction is found to proceed via a radical mechanism, as demonstrated by reactions in the presence of radical scavengers. This finding also adds to the currently limited knowledge in understanding mechanisms of reactions induced by ball milling. The results, guided by the insight into the mechanism, could induce more extended exploration to broaden the application scope and help to address the problem of plastic waste by a mechanocatalytic approach.
从不同角度来看，将碳基固体（如不可回收塑料、生物质和煤炭）转化为小分子似乎很有吸引力。然而，这些物质中强大的碳 - 碳键构成了严重障碍，因此，如果这类反应确实可行，就需要高温。煤转化为碳氢化合物的伯格ius法需要450°C以上的温度，不同聚合物热解为热解油通常也在类似温度下进行。我们现在发现，通过球磨可以在室温下实现将具有碳基主链的不同固体底物高效氢化为轻质烃。这种机械催化方法对于广泛的不同碳底物（甚至包括金刚石）都出奇地有效。正如在自由基清除剂存在下的反应所表明的，该反应通过自由基机制进行。这一发现也增加了目前在理解球磨诱导反应机制方面有限的知识。基于对反应机制的洞察所得到的结果，可能会引发更广泛的探索，以扩大应用范围，并有助于通过机械催化方法解决塑料垃圾问题。
