基于醌基的共价有机框架用于电催化析氧反应

doi:10.7503/cjcu2020112

摘要/Abstract

摘要：

将蒽醌作为构筑单元设计合成了醌基功能化的新型2,6-二氨基蒽醌共价有机框架(DAAQ-COF). 粉末X射线衍射、氮气吸附-脱附、红外和热重等分析结果表明, DAAQ-COF具有高的结晶度和比表面积(577 m²/g). 此外, 醌基功能化的无金属DAAQ-COF显示出高的析氧反应(OER)活性(10 mA/cm²下, 过电位389 mV, Tafel斜率135 mV/dec). 这源于引入的醌基基团有效改变了COF框架的电子结构和化学特性, 加上COF材料本身的高结晶度和比表面积, 使得反应物能更有效地与活性位点接触, 从而促进OER进程. 这些结果表明合理地设计功能化的COF材料能够进一步推动此类材料在电催化领域的应用.

关键词: 共价有机框架, 醌, 电催化, 析氧反应

Abstract:

Covalent organic frameworks(COFs) are a new kind of crystalline organic porous polymers with high specific surface area, regular structure and designability, which has been applied in many domains. However, functionalized covalent organic frameworks still need to be further explored. Herein, a quinone-based COF(2,6-diaminoanthraquinone-COF, DAAQ-COF) was synthesized by using anthraquinone as building blocks, and characterized by powder X-ray diffraction(PXRD), nitrogen adsorption-desorption analysis, Fourier transform infrared(FTIR) spectrometry and thermogravimetry analysis(TGA) etc. It is showed that the synthesized DAAQ-COF has high crystallinity and specific surface area(577 m²/g). Furthermore, quinone-functionalized metal-free DAAQ-COF exhibits effective oxygen evolution reduction(OER), with a overpotential of 389 mV at 10 mA/cm² and a Tafel slope of 135 mV/dec. The introduced quinone group effectively changes the electronic structure and chemical properties of the COF framework, as well as the high crystallinity and specific surface area of the COF material itself, which allows the reactant more efficiently accessible to the active sites for better OER performance. These results show that the rational design of functionalized COFs can promote the development of their broader application prospects in OER.

Key words: Covalent organic framework, Quinone, Electrocatalysis, Oxygen evolution reaction

中图分类号:

O643
O622

常建红, 徐国杰, 李辉, 方千荣. 基于醌基的共价有机框架用于电催化析氧反应[J]. 高等学校化学学报, 2020, 41(7): 1609-1614.

CHANG Jianhong, XU Guojie, LI Hui, FANG Qianrong. Quinone-based Covalent Organic Frameworks for Efficient Oxygen Evolution Reaction^†[J]. Chemical Journal of Chinese Universities, 2020, 41(7): 1609-1614.

图/表 6

Scheme 1 Schematic representation of the strategy for preparing DAAQ-COF

Fig.1 PXRD pattern(A) and structure(B) of DAAQ-COF a. Experimental; b. Pawley refined; c. simulated AA stacking model; d. simulated AB stacking model; e. difference between experimental and simulated values.

Fig.2 N2 adsorption-desorption isotherm at 77 K(A) and pore size distribution(B) of DAAQ-COF

Fig.3 FTIR spectra(A), TGA curve(B) and SEM image(C) of DAAQ-COF

Fig.4 LSVs for OER in a N2-saturated 1.0 mol/L KOH aqueous solution(A) and Tafel plots obtained from OER polarization curves(B) a. DAAQ-COF; b. TpPa-COF; c. DAAQ. (B) Tafel slope/(mV·dec-1): a. 135; b. 153; c. 171.

Fig.5 EIS Nyquist comparison plots obtained from 100 kHz to 1 Hz at the amplitude of the applied voltage of 5 mV(A) and capacitive currents versus scan rates on the basis of CV curves recorded at di?erent scan rates(B) a. DAAQ-COF; b. TpPa-COF; c. DAAQ.

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