Synergistic effect of dual active sites over Ru/a-MoC for accelerating alkaline hydrogen evolution reaction

被引:74
作者
Fan, Xueliang [1 ]
Liu, Cong [2 ]
Wu, Minying [1 ]
Gao, Boxu [1 ]
Zheng, Luyao [1 ]
Zhang, Yahong [1 ]
Zhang, Hongbin [3 ]
Gao, Qingsheng [4 ]
Cao, Xiaoming [2 ]
Tang, Yi [1 ]
机构
[1] Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat,Lab A, Shanghai 200433, Peoples R China
[2] East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China
[3] Fudan Univ, Fudan Univ Lib, Inst Preservat Chinese Ancient Books, Shanghai 200433, Peoples R China
[4] Jinan Univ, Coll Chem & Mat Sci, Guangdong Prov Key Lab Funct Supramol Coordinat Ma, Guangzhou 510632, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 318卷
基金
中国国家自然科学基金;
关键词
Hydrogen evolution reaction; a-MoC; Ruthenium (Ru); Synergistic effect; Dual active sites; EFFICIENT; CARBON; WATER;
D O I
10.1016/j.apcatb.2022.121867
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Developing alkaline hydrogen evolution reaction catalysts with ultra-low overpotential remains a significant challenge. In this paper, a three-dimensional porous Ru/alpha-MoC has been developed, which features the dual active sites of alpha-MoC and Ru. The coexistence of ultrafine Ru nanoparticles and Ru single atoms in Ru/alpha-MoC system is demonstrated by multiple structural characterizations. The fabricated Ru/alpha-MoC exhibits excellent alkaline HER activity with a low overpotential 25 mV at 10 mA cm-2, outperforming commercial 20% Pt/C (45 mV), and robust electrocatalytic stability at an industrial-scale current density of 400 mA cm-2. Particularly, the turnover frequency value reaches 39.2 s-1 at the overpotential of 100 mV. Experiments and theory investigations demonstrate the electron redistribution at the interface of alpha-MoC and Ru. The synergistic effect of dual active sites enables the easy cleavage of H-OH bond and the optimal H adsorption energy simultaneously. This work opens up a feasible way to rationally design high-efficient electrocatalysts with dual active sites for typical multistep reactions.
引用
收藏
页数:10
相关论文
共 52 条
[1]   Single Faceted Two-Dimensional Mo2C Electrocatalyst for Highly Efficient Nitrogen Fixation [J].
Ba, Kun ;
Wang, Ganlin ;
Ye, Tong ;
Wang, Xirui ;
Sun, Yangye ;
Liu, Hanqi ;
Hu, Anqi ;
Li, Zhenyu ;
Sun, Zhengzong .
ACS CATALYSIS, 2020, 10 (14) :7864-7870
[2]   Recent advances in ruthenium-based electrocatalysts for the hydrogen evolution reaction [J].
Bae, Seo-Yoon ;
Mahmood, Javeed ;
Jeon, In-Yup ;
Baek, Jong-Beom .
NANOSCALE HORIZONS, 2020, 5 (01) :43-56
[3]   Ordered Mesoporous Metastable α-MoC1-x with Enhanced Water Dissociation Capability for Boosting Alkaline Hydrogen Evolution Activity [J].
Baek, Du San ;
Jung, Gwan Yeong ;
Seo, Bora ;
Kim, Jin Chul ;
Lee, Hyun-Wook ;
Shin, Tae Joo ;
Jeong, Hu Young ;
Kwak, Sang Kyu ;
Joo, Sang Hoon .
ADVANCED FUNCTIONAL MATERIALS, 2019, 29 (28)
[4]   Coupling of Ru and O-Vacancy on 2D Mo-Based Electrocatalyst Via a Solid-Phase Interface Reaction Strategy for Hydrogen Evolution Reaction [J].
Cai, Jialin ;
Ding, Jie ;
Wei, Donghui ;
Xie, Xin ;
Li, Baojun ;
Lu, Siyu ;
Zhang, Jianmin ;
Liu, Yushan ;
Cai, Qiang ;
Zang, Shuangquan .
ADVANCED ENERGY MATERIALS, 2021, 11 (26)
[5]   Construction of Dual-Site Atomically Dispersed Electrocatalysts with Ru-C5 Single Atoms and Ru-O4 Nanoclusters for Accelerated Alkali Hydrogen Evolution [J].
Cao, Dong ;
Wang, Jiayi ;
Xu, Haoxiang ;
Cheng, Daojian .
SMALL, 2021, 17 (31)
[6]   Tunable Ru-Ru2P heterostructures with charge redistribution for efficient pH-universal hydrogen evolution [J].
Chen, Ding ;
Yu, Ruohan ;
Lu, Ruihu ;
Pu, Zonghua ;
Wang, Pengyan ;
Zhu, Jiawei ;
Ji, Pengxia ;
Wu, Dulan ;
Wu, Jinsong ;
Zhao, Yan ;
Kou, Zongkui ;
Yu, Jun ;
Mu, Shichun .
INFOMAT, 2022, 4 (05)
[7]   Ru-doped 3D flower-like bimetallic phosphide with a climbing effect on overall water splitting [J].
Chen, Ding ;
Lu, Ruihu ;
Pu, Zonghua ;
Zhu, Jiawei ;
Li, Hai-Wen ;
Liu, Fang ;
Hu, Song ;
Luo, Xu ;
Wu, Jinsong ;
Zhao, Yan ;
Mu, Shichun .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 279 (279)
[8]   Ultralow Ru Loading Transition Metal Phosphides as High-Efficient Bifunctional Electrocatalyst for a Solar-to-Hydrogen Generation System [J].
Chen, Ding ;
Pu, Zonghua ;
Lu, Ruihu ;
Ji, Pengxia ;
Wang, Pengyan ;
Zhu, Jiawei ;
Lin, Can ;
Li, Hai-Wen ;
Zhou, Xiangang ;
Hu, Zhiyi ;
Xia, Fanjie ;
Wu, Jingsong ;
Mu, Shichun .
ADVANCED ENERGY MATERIALS, 2020, 10 (28)
[9]   Molecular Engineering toward Pyrrolic N-Rich M-N4 (M = Cr, Mn, Fe, Co, Cu) Single-Atom Sites for Enhanced Heterogeneous Fenton-Like Reaction [J].
Chen, Feng ;
Wu, Xi-Lin ;
Shi, Chenyang ;
Lin, Hongjun ;
Chen, Jianrong ;
Shi, Yanpeng ;
Wang, Shaobin ;
Duan, Xiaoguang .
ADVANCED FUNCTIONAL MATERIALS, 2021, 31 (13)
[10]   Improving alkaline hydrogen evolution reaction kinetics on molybdenum carbide: Introducing Ru dopant [J].
Chen, Jiadong ;
Chen, Chunhong ;
Chen, Yuzhuo ;
Wang, Haiyan ;
Mao, Shanjun ;
Wang, Yong .
JOURNAL OF CATALYSIS, 2020, 392 :313-321