Construction of 3D carbon network with N,B,F-tridoping for efficient oxygen reduction reaction electrocatalysis and high performance zinc air battery
Construction of 3D carbon network with N,B,F-tridoping for efficient oxygen reduction reaction electrocatalysis and high performance zinc air battery
复制标题
N、B、F三掺杂构建3D碳网络用于高效氧还原反应电催化和高性能锌空气电池
DOI：
10.1016/j.apsusc.2019.145154
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发表时间：
2020-03-30
影响因子：
6.7
通讯作者：
Zhao, Yufeng
中科院分区：
文献类型：
--
作者：
Lu, Ziyang;Li, Zhiping;Zhao, Yufeng
纳米结构设计和电子结构工程对高效电催化至关重要。设计具有三维纳米结构的多杂原子掺杂碳可以有效地调节电子结构，产生更多的缺陷位点并提供3D导电电路，然而在制备中遇到了困难。本工作展示了一个N，B，F-三掺杂的三维碳网络的建设，通过一种新的NH 4 BF 4引发的自组装壳聚糖链。这种独特的结构呈现出丰富的表面活性边缘缺陷和面内纳米孔缺陷。密度泛函理论计算揭示了N，B，F三掺杂在原子尺度下的显著耦合效应，其中F的强电负性（chi = 4.0）可以使碳基质带正电并贡献更多的相邻碳活性位点。这赋予催化剂令人印象深刻的Pt类氧还原反应（ORR）催化性能，具有0.95 V的高起始电位、0.818 V（vs RHE）的半波电位和6.0 mA cm（-2）的极限电流密度。所构建的锌空气电池表现出最大功率密度为175 mW cm（-2），沿着，恒流放电25 h后电压几乎不变。
Nanoarchitecture design and electronic structure engineering are critically important for efficient electrocatalysis. Designing a multi-heteroatoms doped carbon with three dimensional nanoarchitectures can efficiently modulate the electronic structure, create more defective sites and offer a 3D electric conductive circuit, which however has been encountering difficulties in preparation. This work demonstrates the construction of a N,B,F-tridoped 3D carbon network through a novel NH4BF4 triggered self-assembly of chitosan chain. Such a unique structure presents abundant surface active edge defects and in-plane nanopore defects. Density functional theory calculations reveal the significant coupling effect of N,B,F-tridoping down to the atomic scale, whereby the strong electronegativity of F (chi = 4.0) can positively charge the carbon matrix and contribute more adjacent carbon active sites. This endows the catalyst with impressive Pt like oxygen reduction reaction (ORR) catalytic performance, with a high onset potential of 0.95 V, half-wave potential of 0.818 V (vs RHE), and limiting current density of 6.0 mA cm(-2). The as constructed zinc-air battery demonstrates a maximum power density of 175 mW cm(-2), along with almost unchanged voltage after 25 h galvanostatic discharge.