Preparation and electrochemical properties of new porous carbon materials by synthesizing graphene oxide and waste activated sludge

doi:10.11949/0438-1157.20201825

Abstract

Abstract:

Graphene is a special two-dimensional material with excellent conductivity. However, graphene sheets would easily agglomerate, leading to a large decrease in its conductivity and capacitance. In this study, a three-dimensional activated sludge graphene hydrogel (SGH) was formed by mixing the suspension of graphene oxide (GO) and domesticated waste activated sludge, due to the biocompatibility of GO and the colloidal properties of bacteria. GO was reduced to conductive reduced graphene oxide (rGO) during the formation of hydrogel. SGH can be lyophilized to obtain a porous O and N self-doped porous material with good hydrophilicity and conductivity, namely activated sludge graphene aerogel (SGA). The annealing process in high temperature was found a crucial factor in improving the electrochemical properties of SGA. The specific capacitance of the modified SGA (ANSGA) was increased to 174 F/g at a current density of 2 A/g, after annealing in argon gas with 700℃, 2 h. In addition, the excellent rate capability, ion transport properties and cycling stability make ANSGA a promising material for the probable use of processing electrode materials, which points to a green and dual-beneficial way to produce graphene-based materials and reuse waste activated sludge.

Key words: waste activated sludge, graphene, hydrogel, bacteria, electrochemistry

摘要：

石墨烯是导电性良好的二维材料，但易重新堆叠而导致导电率和电容量下降。氧化石墨烯（GO）的生物相容性和细菌的胶体特性可使二者在水溶液中聚集为三维石墨烯基材料。将剩余活性污泥与GO悬浮液共培养形成活性污泥石墨烯水凝胶（SGH），剩余活性污泥中的细菌可将GO还原为导电的rGO。SGH经冻干可得到具有良好亲水性和导电性的O、N自掺杂多孔材料，即活性污泥石墨烯气凝胶（SGA）。在氩气中高温退火可进一步提高材料的电化学性能。经700℃、2 h退火后的改性SGA（ANSGA）具有174 F/g的比电容值（2 A/g），以及优异的倍率性能、离子传输性能和循环稳定性，具有进一步加工制备电极材料的应用潜力，为石墨烯基材料绿色制备和剩余活性污泥资源化利用提供方向。

关键词: 剩余活性污泥, 石墨烯, 水凝胶, 细菌, 电化学

CLC Number:

TQ 028.8

XIAO Xian, XU Wenhao, SHEN Liang, WANG Yuanpeng, LU Yinghua. Preparation and electrochemical properties of new porous carbon materials by synthesizing graphene oxide and waste activated sludge[J]. CIESC Journal, 2021, 72(7): 3869-3879.

肖弦, 徐文昊, 沈亮, 王远鹏, 卢英华. 氧化石墨烯与剩余活性污泥聚合制备多孔碳材料及其电化学性能[J]. 化工学报, 2021, 72(7): 3869-3879.

Figures/Tables 9

Fig.1 Schematic diagram of a self-assembly method for preparing SGH

Fig.2 XPS C 1s spectra of GO (a) and SGH-rGO (b)

Fig.3 FTIR spectra(a), XRD patterns (b)， and Raman spectra (c) of GO and SGH-rGO

Fig.4 Contact angle of SGA at 0 s(a); Contact angle of SGA at 9 s (b); FTIR spectra (c) and XPS C 1s spectra[(d),(e)] of GO and SGA-rGO

Fig.5 XPS survey spectra of SGA

Fig.6 SEM images of SGA [(a)—(c)] and ANSGA[(d)—(f)]

Fig.7 Electrochemical performance of ANSGA： CV curves (a), GCD curves (b), specific capacitance at different current densities (c), and cyclic stability test at a current density of 21 A/g (d)

Table 1 Comparison of specific capapcitance， capacitance retention and N-doped content of graphene-based carbon material

主要材料	比电容/(F/g)	电容保留率/%	掺氮量/%(质量)	文献
GO/ammonia water	233.3(0.5 A/g)	64.3(20 A/g)	4.4	[31]
GO/NH₃	175(2 A/g)	53.8(6 A/g)	3.97	[32]
GO/uric acid	196(2 A/g)	79.1(3 A/g)	5.63	[33]
GO/MnCo₂O₄/DMF	95.1(2 A/g)	65.2(4 A/g)	4.14	[34]
GO/CuO/NH₄NO₃	197(5 A/g)	57.9(5 A/g)	4.54	[35]
GO/Fe₃O₄/Mn₂O₃/N₂H₄	90.58(0.5 A/g)	80.7(2.5 A/g)	—	[36]
GO/FeCl₃/E.coli	224(2 A/g)	51.3(5 A/g)	5.58	[37]
ANSGA(GO/activated sludge)	174(2 A/g)	74.7(48 A/g)	5.61	本文

Fig.8 Electrochemical performance of SGA and ANSGA： CV curves at a scan rate of 50 mV/s (a)， CV curves of SGA (b)， GCD curves at a current density of 2 A/g (c), and specific capacitance at different current densities (d)

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