Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide

Abstract With the rapid development of graphene industry, low-cost sustainable synthesis of monolayer graphene oxide (GO) has become more and more important for many applications such as water desalination, thermal management, energy storage and functional composites. Compared to the conventional ch...

Full description

Saved in:
Bibliographic Details
Main Authors: Jiaqi Guo, Songfeng Pei, Kun Huang, Qing Zhang, Xizhong Zhou, Jinmeng Tong, Zhibo Liu, Hui-Ming Cheng, Wencai Ren
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56121-4
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1832594568150777856
author Jiaqi Guo
Songfeng Pei
Kun Huang
Qing Zhang
Xizhong Zhou
Jinmeng Tong
Zhibo Liu
Hui-Ming Cheng
Wencai Ren
author_facet Jiaqi Guo
Songfeng Pei
Kun Huang
Qing Zhang
Xizhong Zhou
Jinmeng Tong
Zhibo Liu
Hui-Ming Cheng
Wencai Ren
author_sort Jiaqi Guo
collection DOAJ
description Abstract With the rapid development of graphene industry, low-cost sustainable synthesis of monolayer graphene oxide (GO) has become more and more important for many applications such as water desalination, thermal management, energy storage and functional composites. Compared to the conventional chemical oxidation methods, water electrolytic oxidation of graphite-intercalation-compound (GIC) shows significant advantages in environmental-friendliness, safety and efficiency, but suffers from non-uniform oxidation, typically ~50 wt.% yield with ~50% monolayers. Here, we show that water-induced deintercalation of GIC is responsible for the non-uniform oxidation of the water electrolytic oxidation method. Using in-situ experiments, the control principles of water diffusion governing electrochemical oxidation and deintercalation of GIC are revealed. Based on these principles, a liquid membrane electrolysis method was developed to precisely control the water diffusion to achieve a dynamic equilibrium between oxidation and deintercalation, enabling industrial sustainable synthesis of uniform monolayer GO with a high yield (~180 wt.%) and a very low cost (~1/7 of Hummers’ methods). Moreover, this method allows precise control on the structure of GO and the synthesis of GO by using pure water. This work provides new insights into the role of water in electrochemical reaction of graphite and paves the way for the industrial applications of GO.
format Article
id doaj-art-b5a837a12f1141dbb38974d7f69d9b31
institution Kabale University
issn 2041-1723
language English
publishDate 2025-01-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-b5a837a12f1141dbb38974d7f69d9b312025-01-19T12:31:15ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-025-56121-4Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxideJiaqi Guo0Songfeng Pei1Kun Huang2Qing Zhang3Xizhong Zhou4Jinmeng Tong5Zhibo Liu6Hui-Ming Cheng7Wencai Ren8Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua RoadAbstract With the rapid development of graphene industry, low-cost sustainable synthesis of monolayer graphene oxide (GO) has become more and more important for many applications such as water desalination, thermal management, energy storage and functional composites. Compared to the conventional chemical oxidation methods, water electrolytic oxidation of graphite-intercalation-compound (GIC) shows significant advantages in environmental-friendliness, safety and efficiency, but suffers from non-uniform oxidation, typically ~50 wt.% yield with ~50% monolayers. Here, we show that water-induced deintercalation of GIC is responsible for the non-uniform oxidation of the water electrolytic oxidation method. Using in-situ experiments, the control principles of water diffusion governing electrochemical oxidation and deintercalation of GIC are revealed. Based on these principles, a liquid membrane electrolysis method was developed to precisely control the water diffusion to achieve a dynamic equilibrium between oxidation and deintercalation, enabling industrial sustainable synthesis of uniform monolayer GO with a high yield (~180 wt.%) and a very low cost (~1/7 of Hummers’ methods). Moreover, this method allows precise control on the structure of GO and the synthesis of GO by using pure water. This work provides new insights into the role of water in electrochemical reaction of graphite and paves the way for the industrial applications of GO.https://doi.org/10.1038/s41467-025-56121-4
spellingShingle Jiaqi Guo
Songfeng Pei
Kun Huang
Qing Zhang
Xizhong Zhou
Jinmeng Tong
Zhibo Liu
Hui-Ming Cheng
Wencai Ren
Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
Nature Communications
title Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
title_full Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
title_fullStr Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
title_full_unstemmed Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
title_short Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
title_sort control of water for high yield and low cost sustainable electrochemical synthesis of uniform monolayer graphene oxide
url https://doi.org/10.1038/s41467-025-56121-4
work_keys_str_mv AT jiaqiguo controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT songfengpei controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT kunhuang controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT qingzhang controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT xizhongzhou controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT jinmengtong controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT zhiboliu controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT huimingcheng controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide
AT wencairen controlofwaterforhighyieldandlowcostsustainableelectrochemicalsynthesisofuniformmonolayergrapheneoxide