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Nonmainstream Out‐Plane Fluoro‐ and Amino‐Cofunctionalized Graphene for a Striking Electrocatalyst: Programming Substitutive/Reductive Defluorination toward Graphite Fluoride
Advanced Materials Interfaces ( IF 4.3 ) Pub Date : 2019-01-16 , DOI: 10.1002/admi.201801699
Fu-Gang Zhao 1 , Bingyige Pan 1 , Yu-Ting Kong 1 , Lei Dong 2 , Cheng-Min Hu 1 , Ying-Ji Sang 1 , Xianjing Zhou 1 , Biao Zuo 1 , Xiaoping Dong 1 , Benxia Li 1 , Wei-Shi Li 3
Affiliation  

It is mostly reported that graphene lattice doped/codoped with heteroatoms (e.g., nitrogen and boron) in an in‐plane fashion exhibits an impressive oxygen reduction reaction (ORR) electrocatalytic efficiency when serving as a metal‐free catalyst, but the cases that graphene sheets functionalized with heteroatoms in an out‐plane scenario are rarely involved. Herein, amino (NH2)‐/fluoro (F)‐cofunctionalized graphene (NH2GF) is rationally designed and synthesized both in out‐plane modes through a programmable substitutive/reductive defluorination toward bulk graphite fluoride using NaNH2. Versatile NH2‐/F‐(co)functionalized graphene products with tunable fluorination and amination are readily yielded and their ORR electrocatalysis is evaluated. Intriguingly, the parameter of NH2/F molar ratio is determinative for their electrocatalytic performances. Consequently, graphene product (roughly formulated in (NH2)7.0C100F2.8, vide infra) dually functionalized with NH2 and F and with an optimized NH2/F factor of 2.5 outperforms others—overmuch in either NH2 only or F only. Encouragingly, (NH2)7.0C100F2.8 even delivers a slightly better electrocatalytic activity than Pt/C catalyst. This finding implies a significant synergistic effect between NH2 and F in boosting graphene electrocatalysis. Apart from fantastic electrocatalytic activity, (NH2)7.0C100F2.8 also exhibits remarkable resistance to crossover effect and exceptional cycling stability.

中文翻译:

非主流的平面氟和氨基共官能化石墨烯,用于醒目的电催化剂:对石墨氟化物的取代/还原脱氟编程

据报道,以杂原子(例如氮和硼)共面掺杂/共掺杂的石墨烯晶格在用作无金属催化剂时表现出令人印象深刻的氧还原反应(ORR)电催化效率,但是石墨烯的情况在外层情况下很少用杂原子功能化的床单。在本文中,氨基(NH 2) - /氟代(F)-cofunctionalized石墨烯(NH 2 ģ F)设计合理,并通过朝向使用NaNH块状石墨氟化物可编程代用/还原脱氟合成无论在平面外模式2。多功能NH 2容易产生具有可调氟化和胺化作用的-/ F-(共)官能化石墨烯产品,并对其ORR电催化性能进行了评估。有趣的是,NH 2 / F摩尔比的参数决定了它们的电催化性能。因此,石墨烯产物(大致配制在(NH 27.0 Ç 100 ˚F 2.8,见下文)与NH双重官能2和F,并用优化的NH 2 2.5性能优于的/ F因子他人-过多中任NH 2只或仅F。令人鼓舞的是,(NH 27.0 Ç 100 ˚F2.8甚至比Pt / C催化剂具有更好的电催化活性。该发现暗示了在促进石墨烯电催化中NH 2和F之间的显着协同作用。除了从奇异电催化活性,(NH 27.0 Ç 100 ˚F 2.8也表现出对交叉效果和优异的循环稳定性显着阻力。
更新日期:2019-01-16
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