Stable Radicals with Protective Umbrellas Integrated on the Surface of 2D Layered Materials

Chen Yuanyuan; Peng Jian; Sheng TianQin RuixuanDai ShuqiShi ZaifaTang ZichaoWang LaisenZhang QinghuaHan BinSun LipingXu JunWeng Jian

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Stable Radicals with Protective Umbrellas Integrated on the Surface of 2D Layered Materials

机译：Stable Radicals with Protective Umbrellas Integrated on the Surface of 2D Layered Materials

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Radicals are closely related to human life and health and have been widely used in biology, chemistry, functional materials, etc. However, the high reactivity, disorder, and short half-lives limit their wide applications. Therefore, it remains a great challenge to prepare stable and ordered radicals. Herein, radicals are prepared with protective umbrellas (diethylmethyleneamine, DEMA) that are integrated on the surface of 2D layered materials to isolate water and oxygen and enhance the stability of radicals. Taking 2D black phosphorus (BP) as an example: triethylamine reacts with dichloromethane to form quaternary ammonium salts with further Hoffmann elimination to produce DEMA radicals that could react with one electron of a lone pair electrons in P on the surface of BP to produce P radicals, which shows a prolonged half-life of 21 days at room temperature. First-principle calculations and electron paramagnetic resonance fitting confirm that the steric hindrance constructed by dense DEMA passivation layer acts as a protective umbrella and the 2D coupling of P radicals and other P atoms in 2D BP plane to enhance the stability and strong superexchange interaction of P radicals. Furthermore, it is a general strategy to produce stable radicals integrated on the 2D plane.

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《Advanced functional materials》 |2021年第42期|2104246.1-2104246.10|共10页
作者
Chen Yuanyuan; Peng Jian; Sheng TianQin RuixuanDai ShuqiShi ZaifaTang ZichaoWang LaisenZhang QinghuaHan BinSun LipingXu JunWeng Jian;
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作者单位

Xiamen Univ, Coll Mat, Xiamen 361005, Peoples R China|Wuhan Univ Sci & Technol, Med Coll, Dept Pharmacol, Wuhan 430070, Peoples R China;

Xiamen Univ, Coll Mat, Xiamen 361005, Peoples R China|Wuhan Univ Technol, Biomed Mat & Engn Res Ctr Hubei Prov, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China;

Xiamen Univ, Coll Chem & Chem Engn, Collaborat Innovat Ctr Chem Energy Mat, Xiamen 361005, Peoples R ChinaChinese Acad Sci, Inst Phys, Beijing 100190, Peoples R ChinaXiamen Univ, Fujian Prov Key Lab Soft Funct Mat, Res Inst Biomimet & Soft Matter, Dept Phys, Xiamen 361005, Peoples R ChinaXiamen Univ, Coll Mat, Xiamen 361005, Peoples R ChinaXiamen Univ, Coll Mat, Xiamen 361005, Peoples R China|Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China;

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2D materials; integration; protective umbrella; radicals; stability;

Stable Radicals with Protective Umbrellas Integrated on the Surface of 2D Layered Materials

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