Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants

doi:10.1016/j.cjche.2021.12.029

中国化学工程学报 ›› 2023, Vol. 53 ›› Issue (1): 124-132.DOI: 10.1016/j.cjche.2021.12.029

• Full Length Article • 上一篇下一篇

Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants

Jian Tian¹, Gen Li¹, Wang He¹, Kok Bing Tan¹, Daohua Sun¹, Junfu Wei², Qingbiao Li^1,3

1. Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;
2. College of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China;
3. College of Food and Biological Engineering, Jimei University, Xiamen 361021, China

收稿日期:2021-07-07 修回日期:2021-12-03 出版日期:2023-01-28 发布日期:2023-04-08
通讯作者: Daohua Sun,E-mail:sdaohua@xmu.edu.cn;Junfu Wei,E-mail:jfwei@tjpu.edu.cn
基金资助:
This research was supported by the National Natural Science Foundation of China (22078269 and 51708406).

Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants

Jian Tian¹, Gen Li¹, Wang He¹, Kok Bing Tan¹, Daohua Sun¹, Junfu Wei², Qingbiao Li^1,3

1. Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;
2. College of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China;
3. College of Food and Biological Engineering, Jimei University, Xiamen 361021, China

Received:2021-07-07 Revised:2021-12-03 Online:2023-01-28 Published:2023-04-08
Contact: Daohua Sun,E-mail:sdaohua@xmu.edu.cn;Junfu Wei,E-mail:jfwei@tjpu.edu.cn
Supported by:
This research was supported by the National Natural Science Foundation of China (22078269 and 51708406).

摘要/Abstract

摘要： Graphene oxide (GO) channels exhibit unique mass transport behaviors due to their flexibility, controllable thinness and extraordinary physicochemical properties, enabling them to be widely used for adsorption and membrane separation. Nevertheless, the adsorption behavior of nanosized contaminants within the channels of GO membrane has not been fully discussed. In this study, we fabricated a GO membrane (PGn, where n represents the deposition cycles of GO) with multi channels via the cross-linking of GO and multibranched poly(ethyleneimine) (PEI). Phenol was used as molecularprobe to determine the correlations between dynamic adsorption behavior and structural parameters of the multilevel GO/PEI membrane. PG8 shows higher adsorption capacities and affinity, which is predominantly attributed to the multichannel structure providing a large specific surface for phenol adsorption, enhancing the accessibility of active sites for phenol molecules and the transport of phenol. Density functional theory calculations demonstrate that the adsorption mechanism of phenol within GO channel is energetically oriented by hydrogen bonds, which is dominated by oxygen-containing groups compared to amino groups. Particularly, the interfaces which facilitate strong π-π interaction and hydrogen bonds maybe the most active regions. Moreover, the as-prepared PG8 membrane showed outstanding performance for other contaminants such as methyl orange and Cr(VI). It is anticipated that this study will have implications for design of GO-related environmental materials with enhanced efficiency.

关键词: Graphene oxide, Multichannel, Adsorptive behavior, Phenol, DFT calculations

Abstract: Graphene oxide (GO) channels exhibit unique mass transport behaviors due to their flexibility, controllable thinness and extraordinary physicochemical properties, enabling them to be widely used for adsorption and membrane separation. Nevertheless, the adsorption behavior of nanosized contaminants within the channels of GO membrane has not been fully discussed. In this study, we fabricated a GO membrane (PGn, where n represents the deposition cycles of GO) with multi channels via the cross-linking of GO and multibranched poly(ethyleneimine) (PEI). Phenol was used as molecularprobe to determine the correlations between dynamic adsorption behavior and structural parameters of the multilevel GO/PEI membrane. PG8 shows higher adsorption capacities and affinity, which is predominantly attributed to the multichannel structure providing a large specific surface for phenol adsorption, enhancing the accessibility of active sites for phenol molecules and the transport of phenol. Density functional theory calculations demonstrate that the adsorption mechanism of phenol within GO channel is energetically oriented by hydrogen bonds, which is dominated by oxygen-containing groups compared to amino groups. Particularly, the interfaces which facilitate strong π-π interaction and hydrogen bonds maybe the most active regions. Moreover, the as-prepared PG8 membrane showed outstanding performance for other contaminants such as methyl orange and Cr(VI). It is anticipated that this study will have implications for design of GO-related environmental materials with enhanced efficiency.

Key words: Graphene oxide, Multichannel, Adsorptive behavior, Phenol, DFT calculations

Jian Tian, Gen Li, Wang He, Kok Bing Tan, Daohua Sun, Junfu Wei, Qingbiao Li. Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants[J]. 中国化学工程学报, 2023, 53(1): 124-132.

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Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants

Insight into the dynamic adsorption behavior of graphene oxide multichannel architecture toward contaminants

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