论文标题
二维材料的自由基阴离子功能化，作为同时高度电子和离子电导率固体工程的一种手段
Radical Anion Functionalization of Two-Dimensional Materials as a Means of Engineering Simultaneously High Electronic and Ionic Conductivity Solids
论文作者
论文摘要
在本研究中提出了二维（2D）材料基底平面的基于自由基阴离子的功能化。简单的电荷中性自由基官能化通常在还原时从基础平面上脱离。例如，当用碱金属还原时，环氧氧不可逆地从石墨烯中脱离。 2D材料的自由基阴离子功能化导致稳定的降低状态，由于阳离子在表面上带负电荷的官能团之间的阳离子的较大迁移率，因此可以可逆地被氧化并具有高离子电导率。根据这些系统的氧化状态，还可以实现高浓度的孔状态，以获得良好的电子电导率。这些特性可以进一步通过非过渡金属阴极的活性物种，固体电解质，电导性添加剂，分离器，金属阳极的涂料和热导体通过单个材料来改善储能装置。上述原理的一种可能实现是2D盐A（Bn）2OBX3，其中A是碱原子（Li，Na等； 0 = <N = <2）或碱土（mg，etc et eet eq et; 0 = <n = <1），而x是halide（通常是f或cl）。该材料可以源自六角硼的基底平面功能化H-BN，在A阳离子的存在下，具有.obx3^ - 自由基阴离子。 .OBX3^ - 自由基阴离子的一个潜在来源是它们的重组形式，即[X3B-O-O-BX3] 2-阴离子，可以在Ano2离子过氧化物的Lewis加合物中找到，其bx3：a [x3b-o-o-bx3]。可以通过在重组阴离子中热拆分O-O键来获得单个自由基阴离子。使用LI，NA和MG阳极，热稳定性以及高能和功率密度的过渡金属全稳态电池可以使用（BN）2OBX3实现。
A radical anion based functionalization of the basal plane of two-dimensional (2D) materials is proposed in the present study. Simple charge neutral radical functionalizations typically detach from the basal planes upon reduction. For example, epoxy oxygens irreversibly detach from graphene when reduced by an alkali metal. The radical anion functionalization of 2D materials results in a stable reduced state that can reversibly be oxidized and has high ionic conductivity due to the great mobility of the cations between the negatively charged functional groups on the surface. Depending on the oxidation state of these systems, a high concentration of hole states can also be realized allowing for good electronic conductivity. These properties can further allow for improved energy storage devices via transition metal free cathode active species, solid electrolytes, electroconductive additives, separators, coatings for metal anodes and heat conductors through a single material. One possible realization of the above principles is the 2D salt An(BN)2OBX3, where A is an alkali atom (Li, Na, etc; 0=<n=<2) or alkaline earth (Mg, etc; 0=<n=<1) and X is a halide (typically F or Cl). This material can be derived from the basal plane functionalization of hexagonal boron nitride, h-BN, with .OBX3^- radical anions in the presence of the A cations. One potential source of .OBX3^- radical anions is their recombined form, the [X3B-O-O-BX3]2- anion, which can be found in the Lewis adduct of an AnO2 ionic peroxide with BX3: An[X3B-O-O-BX3]. The individual radical anions can be obtained by thermally splitting the O-O bond in the recombined anion. Transition metal free all-solid-state batteries with Li, Na and Mg anodes, thermal stability and high energy and power densities may be realizable using An(BN)2OBX3.
