Solvent Engineering of Oxygen-Enriched Carbon Dots for Efficient Electrochemical Hydrogen Peroxide Production

被引:67
作者
Shen, Xiaoyu [1 ]
Wang, Zeming [1 ]
Guo, Huazhang [1 ]
Lei, Zhendong [2 ]
Liu, Zheng [2 ]
Wang, Liang [1 ,2 ]
机构
[1] Shanghai Univ, Inst Nanochem & Nanobiol, Sch Environm & Chem Engn, 99 Shangda Rd, Baoshan 200444, Shanghai, Peoples R China
[2] Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore
基金
中国国家自然科学基金;
关键词
electrochemical generations; flow cells; hydrogen peroxide; metal-free carbon materials; selectivity; MICROWAVE-ASSISTED SYNTHESIS; GRAPHENE QUANTUM DOTS; H2O2; PRODUCTION; REDUCTION; ELECTROSYNTHESIS; SELECTIVITY; GENERATION;
D O I
10.1002/smll.202303156
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of cost-effective and reliable metal-free carbon-based electrocatalysts has gained significant attention for electrochemical hydrogen peroxide (H2O2) generation through a two-electron oxygen reduction reaction. In this study, a scalable solvent engineering strategy is employed to fabricate oxygen-doped carbon dots (O-CDs) that exhibit excellent performance as electrocatalysts. By adjusting the ratio of ethanol and acetone solvents during the synthesis, the surface electronic structure of the resulting O-CDs can be systematically tuned. The amount of edge active C-O group was strongly correlated with the selectivity and activity of the O-CDs. The optimum O-CDs-3 exhibited extraordinary H2O2 selectivity of up to 96.55% (n = 2.06) at 0.65 V (vs RHE) and achieved a remarkably low Tafel plot of 64.8 mV dec(-1). Furthermore, the realistic H2O2 productivity yield of flow cell is measured to be as high as 111.18 mg h(-1) cm(-2) for a duration of 10 h. The findings highlight the potential of universal solvent engineering approach for enabling the development of carbon-based electrocatalytic materials with improved performance. Further studies will be undertaken to explore the practical implications of the findings for advancing the field of carbon-based electrocatalysis.
引用
收藏
页数:9
相关论文
共 59 条
[1]   Two-Electron Oxygen Reduction on Carbon Materials Catalysts: Mechanisms and Active Sites [J].
Chai, Guo-Liang ;
Hou, Zhufeng ;
Ikeda, Takashi ;
Terakura, Kiyoyuki .
JOURNAL OF PHYSICAL CHEMISTRY C, 2017, 121 (27) :14524-14533
[2]   Oxygen Reduction Reaction on Graphene in an Electro-Fenton System: In Situ Generation of H2O2 for the Oxidation of Organic Compounds [J].
Chen, Chen-Yu ;
Tang, Cheng ;
Wang, Hao-Fan ;
Chen, Cheng-Meng ;
Zhang, Xiaoyuan ;
Huang, Xia ;
Zhang, Qiang .
CHEMSUSCHEM, 2016, 9 (10) :1194-1199
[3]   Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity [J].
Chen, Jinxing ;
Ma, Qian ;
Zheng, Xiliang ;
Fang, Youxing ;
Wang, Jin ;
Dong, Shaojun .
NATURE COMMUNICATIONS, 2022, 13 (01)
[4]   Chemical Identification of Catalytically Active Sites on Oxygen-doped Carbon Nanosheet to Decipher the High Activity for Electro-synthesis Hydrogen Peroxide [J].
Chen, Shanyong ;
Luo, Tao ;
Chen, Kejun ;
Lin, Yiyang ;
Fu, Junwei ;
Liu, Kang ;
Cai, Chao ;
Wang, Qiyou ;
Li, Huangjingwei ;
Li, Xiaoqing ;
Hu, Junhua ;
Li, Hongmei ;
Zhu, Mingshan ;
Liu, Min .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (30) :16607-16614
[5]   Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide [J].
Chen, Shucheng ;
Chen, Zhihua ;
Siahrostami, Samira ;
Kim, Taeho Roy ;
Nordlund, Dennis ;
Sokaras, Dimosthenis ;
Nowak, Stanislaw ;
To, John W. F. ;
Higgins, Drew ;
Sinclair, Robert ;
Norskov, Jens K. ;
Jaramillo, Thomas F. ;
Bao, Zhenan .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2018, 6 (01) :311-317
[6]   Oxygen-Doped Hierarchical Porous Carbon with Improved Selectivity of Hydrogen Peroxide in an Oxygen Reduction Reaction [J].
Chen, Zixi ;
Li, Yizhao ;
Wu, Ming ;
Cao, Yali .
ENERGY & FUELS, 2021, 35 (03) :2665-2673
[7]   Hydrogen peroxide generation in microbial fuel cells using graphene-based air-cathodes [J].
Dong, Heng ;
Liu, Xiaowan ;
Xu, Ting ;
Wang, Qiuying ;
Chen, Xianghao ;
Chen, Shuning ;
Zhang, Helan ;
Liang, Peng ;
Huang, Xia ;
Zhang, Xiaoyuan .
BIORESOURCE TECHNOLOGY, 2018, 247 :684-689
[8]   Carbon-based dots for the electrochemical production of hydrogen peroxide [J].
Dong, Yongqiang ;
Su, Juanxia ;
Zhou, Shuqing ;
Wang, Min ;
Huang, Shuping ;
Lu, Chun-Hua ;
Yang, Hongbin ;
Fu, Fengfu .
CHEMICAL COMMUNICATIONS, 2020, 56 (55) :7609-7612
[9]   N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production [J].
Fan, Mengmeng ;
Wang, Zeming ;
Sun, Kang ;
Wang, Ao ;
Zhao, Yuying ;
Yuan, Qixin ;
Wang, Ruibin ;
Raj, Jithu ;
Wu, Jingjie ;
Jiang, Jianchun ;
Wang, Liang .
ADVANCED MATERIALS, 2023, 35 (17)
[10]   CO2 Laser-Induced Graphene with an Appropriate Oxygen Species as an Efficient Electrocatalyst for Hydrogen Peroxide Synthesis [J].
Fan, Mengmeng ;
Xu, Jing ;
Wang, Yan ;
Yuan, Qixin ;
Zhao, Yuying ;
Wang, Zeming ;
Jiang, Jianchun .
CHEMISTRY-A EUROPEAN JOURNAL, 2022, 28 (60)