Preparation of Bimetallic Conductive Metal-organic Framework Material Ni/Co-CAT for Electrocatalytic Oxygen Reduction

doi:10.6023/A21120617

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (6): 748-755.DOI: 10.6023/A21120617 Previous Articles Next Articles

Article

双金属导电金属有机框架材料Ni/Co-CAT的制备及其氧还原催化性能研究

耿元昊^a^,^b^,^c, 林小秋^a^,^b^,^c, 孙亚昕^a^,^b^,^c, 李惠雨^a^,^b^,^c, 秦悦^a^,^b^,^c, 李从举^a^,^b^,^c^,^*()

a 北京科技大学能源与环境工程学院北京 100083
b 北京科技大学北京市工业典型污染物资源化处理重点实验室北京 100083
c 北京市高校节能与环保工程研究中心北京 100083

投稿日期:2021-12-31 发布日期:2022-07-07
通讯作者: 李从举
基金资助:
国家自然科学基金(52170019); 国家自然科学基金(51973015); 中央高校基本科研业务费专项资金(06500100); 中央高校基本科研业务费专项资金(FRF-TP-19-046AIZ)

Preparation of Bimetallic Conductive Metal-organic Framework Material Ni/Co-CAT for Electrocatalytic Oxygen Reduction

Yuanhao Geng^a^,^b^,^c, Xiaoqiu Lin^a^,^b^,^c, Yaxin Sun^a^,^b^,^c, Huiyu Li^a^,^b^,^c, Yue Qin^a^,^b^,^c, Congju Li^a^,^b^,^c()

a School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China
b Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants, Beijing 100083, China
c Energy Conservation and Environmental Protection Engineering Research Center in Universities of Beijing, Beijing 100083, China

Received:2021-12-31 Published:2022-07-07
Contact: Congju Li
Supported by:
National Natural Science Foundation of China(52170019); National Natural Science Foundation of China(51973015); Fundamental Research Funds for the Central Universities(06500100); Fundamental Research Funds for the Central Universities(FRF-TP-19-046AIZ)

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Abstract

Ni-catecholate and Ni-Co-catecholate (hereafter referred to as Ni-CAT and Ni-Co-CAT) were prepared by hydrothermal method using 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) as the organic ligand and Ni and Co as the metal centers, respectively. After characterization, a microbial fuel cell (MFC) was constructed in a single chamber reactor device. Single chamber air cathode microbial fuel cell reactors offer the advantages of both small reactor size and no aeration. Ni-CAT and Ni-Co-CAT were mixed with carbon black in a 3∶1 mass ratio and applied to the cathode of MFC to catalyze the oxygen reduction reaction (ORR). The experiments included the preparation of M-CAT (M=Co or Ni), the preparation of air cathode and the assembly and operation of MFC. When preparing the catalytic layer of the air cathode, the conductive MOF and carbon black were mixed in a 3∶1 mass ratio to improve the catalytic effect. Furthermore, the air cathode was mixed with dispersant (isopropanol) and polytetrafluoroethylene (PTFE) to make it waterproof and breathable. The results showed that the MFC reactor catalyzed by Ni-Co-CAT had the best performance. This is due to the fact that bimetallic MOFs have stronger oxygen reduction activity compared to their monometallic counterparts. The MFC reactor catalyzed by Ni-Co-CAT had a maximum output voltage and power density of 310 mV and 190 mW/cm², respectively, which were comparable to the performance of commercial Pt/C. The limiting current density of the MFC reactor catalyzed by Ni-Co-CAT was 2.84 mA/cm², which was better than that of Ni-CAT (2.18 mA/cm²), indicating that the MFC power production efficiency was enhanced by the introduction of Co in the Ni-CAT structure. The main reason is that Ni-Co-CAT has a higher porosity and specific surface area when fully mixed with carbon black, and the metal sites M-O₆ (M=Ni or Co) on its structure provide more catalytic activity, which gives Ni-Co-CAT an optimal electrochemical catalytic performance.

Key words: microbial fuel cell, new conductive metal organic frameworks, air cathode, power generation efficiency, oxygen reaction reduction

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Yuanhao Geng, Xiaoqiu Lin, Yaxin Sun, Huiyu Li, Yue Qin, Congju Li. Preparation of Bimetallic Conductive Metal-organic Framework Material Ni/Co-CAT for Electrocatalytic Oxygen Reduction[J]. Acta Chimica Sinica, 2022, 80(6): 748-755.

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Fig. & Tab. 6

Figure 1. (a) High power SEM of Ni-CAT with a magnification of 92000 times; (b) high power SEM of Ni-Co-CAT with a magnification of 90000 time; (c) structural schematic of Ni-CAT along the c axis[22]; (d) schematic representation for the construction of Ni-Co-CATs for ORR[29]; (e) EDS pattern and elemental mass fraction of Ni-Co-CAT

Figure 2. (a) XRD patterns of Ni-CAT and Ni-Co-CAT; (b) C 1s and (c) Ni 2p XPS spectra of Ni-CAT; (d) C 1s, (e) Ni 2p and (f) Co 2p XPS spectra of Ni-Co-CAT

Figure 3. N2 adsorption-desorption isotherms (a) and pore size distribution curves (b) of Ni-CAT and Ni-Co-CAT

Figure 4. (a) CV curves of Ni-CAT, Ni-Co-CAT, carbon black and Pt/C; (b) LSV curves of Ni-CAT, Ni-Co-CAT, carbon black and Pt/C; (c) EIS curves of Ni-CAT, Ni-Co-CAT, carbon black and Pt/C; (d) Tafel curves of Ni-CAT, Ni-Co-CAT, carbon black and Pt/C

Figure 5. (a) The power density curves of the reactor decorated with Ni-CAT, Ni-Co-CAT, carbon black and Pt/C catalysts after domestication; (b) the polarization curves of the reactor decorated with Ni-CAT, Ni-Co-CAT, carbon black and Pt/C catalysts after domestication; (c) output voltage curve of Ni-CAT; (d) output voltage curve of Ni-Co-CAT; (e) output voltage curve of carbon black; (f) output voltage curve of Pt/C

Figure 6. COD removal rates of Ni-Co-CAT, Ni-CAT, carbon black and Pt/C catalysts

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双金属导电金属有机框架材料Ni/Co-CAT的制备及其氧还原催化性能研究

Preparation of Bimetallic Conductive Metal-organic Framework Material Ni/Co-CAT for Electrocatalytic Oxygen Reduction

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