Hwang Sun-Mi, Choi Song Yi, Youn Min Hye, Lee Wonhee, Park Ki Tae, Gothandapani Kannan, Grace Andrews Nirmala, Jeong Soon Kwan
Climate Change Technology Research Division, Korea Institute of Energy Research, 102 Gajeong-ro, Yuseong-gu, Daejeon 305-343, Korea.
Catalytic Materials Research Department, KORENS RTX, 76-32, Ibam-gil, Duma-myeon, Gyeryong-si, Chungcheongnam-do 328-42, Korea.
ACS Omega. 2020 Sep 14;5(37):23919-23930. doi: 10.1021/acsomega.0c03170. eCollection 2020 Sep 22.
A recent class of porous materials, viz., metal-organic frameworks (MOFs), finds applications in several areas. In this work, Cu-based MOFs (Cu-benzene-1,3,5-tricarboxylic acid) along with graphene oxide, viz., Cu-MOF/GO, are synthesized and used further for reducing CO electrochemically. The reduction was accomplished in various supporting electrolytes, viz., KHCO/HO, tetrabutylammonium bromide (TBAB)/dimethylformamide (DMF), KBr/CHOH, CHCOOK/CHOH, TBAB/CHOH, and tetrabutylammonium perchlorate (TBAP)/CHOH to know their effect on product formation. The electrode fabricated with the synthesized material was used for testing the electroreduction of CO at various polarization potentials. The electrochemical reduction of CO is carried out via the polarization technique within the experimented potential regime vs saturated calomel electrode (SCE). Ion chromatography was employed for the analysis of the produced products in the electrolyte, and the results showed that HCOOH was the main product formed through reduction. The highest concentrations of HCOOH formed for different electrolytes are 0.1404 mM (-0.1 V), 66.57 mM (-0.6 V), 0.2690 mM (-0.5 V), 0.2390 mM (-0.5 V), 0.7784 mM (-0.4 V), and 0.3050 mM (-0.45 V) in various supporting electrolyte systems, viz., KHCO/HO, TBAB/DMF, KBr/CHOH, CHCOOK/CHOH, TBAB/CHOH, and TBAP/CHOH, respectively. The developed catalyst accomplished a significant efficiency in the conversion and reduction of CO. A high faradic efficiency of 58% was obtained with 0.1 M TBAB/DMF electrolyte, whereas for Cu-MOF alone, the efficiency was 38%. Thus, the work is carried out using a cost-effective catalyst for the conversion of CO to formic acid than using the commercial electrodes. The synergistic effect of GO sheets at 3 wt % concentration and CuOH interaction leads to the formation of formic acid in various electrolytes.
最近一类多孔材料,即金属有机框架(MOF),在多个领域得到应用。在本工作中,合成了铜基金属有机框架(Cu-苯-1,3,5-三甲酸)与氧化石墨烯的复合材料,即Cu-MOF/GO,并进一步用于电化学还原CO。还原反应在多种支持电解质中进行,即KHCO₃/H₂O、四丁基溴化铵(TBAB)/二甲基甲酰胺(DMF)、KBr/C₂H₅OH、CH₃COOK/C₂H₅OH、TBAB/C₂H₅OH和高氯酸四丁基铵(TBAP)/C₂H₅OH,以了解它们对产物形成的影响。用合成材料制备的电极用于测试在不同极化电位下CO的电还原。在实验电位范围内相对于饱和甘汞电极(SCE),通过极化技术进行CO的电化学还原。采用离子色谱法分析电解质中产生的产物,结果表明HCOOH是还原形成的主要产物。在不同支持电解质体系中,即KHCO₃/H₂O、TBAB/DMF、KBr/C₂H₅OH、CH₃COOK/C₂H₅OH、TBAB/C₂H₅OH和TBAP/C₂H₅OH中,形成的HCOOH的最高浓度分别为0.1404 mM(-0.1 V)、66.57 mM(-0.6 V)、0.2690 mM(-0.5 V)、0.2390 mM(-0.5 V)、0.7784 mM(-0.4 V)和0.3050 mM(-0.45 V)。所开发的催化剂在CO的转化和还原方面实现了显著的效率。在0.1 M TBAB/DMF电解质中获得了58%的高法拉第效率,而单独的Cu-MOF的效率为38%。因此,与使用商业电极相比,该工作使用了一种经济高效的催化剂将CO转化为甲酸。3 wt%浓度的氧化石墨烯片与CuOH相互作用的协同效应导致在各种电解质中形成甲酸。