Single layer graphene encapsulating non-precious metals as high-performance electrocatalysts for water oxidation

被引:743
作者
Cui, Xiaoju [1 ]
Ren, Pengju [1 ]
Deng, Dehui [1 ]
Deng, Jiao [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, iChEM, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
CORE-SHELL ELECTROCATALYSTS; CARBON NITRIDE SHELL; OXYGEN REDUCTION; ELECTROCHEMICAL PERFORMANCE; IRON NANOPARTICLES; COBALT OXIDE; EVOLUTION; NANOTUBES; CATALYSTS; MORPHOLOGY;
D O I
10.1039/c5ee03316k
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The oxygen evolution reaction (OER) is recognized as a key half-reaction in water electrolysis for clean hydrogen energy, which is kinetically not favored and usually requires precious metal catalysts such as IrO2 and RuO2 to reduce the overpotential. The major challenge in using non-precious metals in place of these precious metal catalysts for OER is their low efficiency and poor stability, which urgently demand new concepts and strategies to tackle this issue. Herein, we report a universal strategy to directly synthesize single layer graphene encapsulating uniform earth-abundant 3d transition-metal nanoparticles such as Fe, Co, Ni and their alloys in a confined channel of mesoporous silica. The single atomic thickness of the graphene shell immensely promotes the electron transfer from the encapsulated metals to the graphene surface, which efficiently optimizes the electronic structure of the graphene surface and thereby triggers the OER activity of the inert graphene surface. We investigated a series of non-precious 3d metals encapsulated within single layer graphene, and found that the encapsulated FeNi alloy showed the best OER activity in alkaline solutions with only 280 mV overpotential at 10 mA cm(-2), and also possessed a high durability after 10000 cycles. Both the activity and durability of the non-precious catalyst even exceed that of the commercial IrO2 catalyst, showing great potential to replace precious metal catalysts in the OER.
引用
收藏
页码:123 / 129
页数:7
相关论文
共 44 条
[1]  
[Anonymous], ANGEW CHEM INT ED
[2]  
Barnett SM, 2012, NAT CHEM, V4, P498, DOI [10.1038/NCHEM.1350, 10.1038/nchem.1350]
[3]   A class of non-precious metal composite catalysts for fuel cells [J].
Bashyam, Rajesh ;
Zelenay, Piotr .
NATURE, 2006, 443 (7107) :63-66
[4]   Three-Dimensional N-Doped Graphene Hydrogel/NiCo Double Hydroxide Electrocatalysts for Highly Efficient Oxygen Evolution [J].
Chen, Sheng ;
Duan, Jingjing ;
Jaroniec, Mietek ;
Qiao, Shi Zhang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (51) :13567-13570
[5]   Visualizing electronic interactions between iron and carbon by X-ray chemical imaging and spectroscopy [J].
Chen, Xiaoqi ;
Xiao, Jianping ;
Wang, Jian ;
Deng, Dehui ;
Hu, Yongfeng ;
Zhou, Jigang ;
Yu, Liang ;
Heine, Thomas ;
Pan, Xiulian ;
Bao, Xinhe .
CHEMICAL SCIENCE, 2015, 6 (05) :3262-3267
[6]   Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction [J].
Chung, Hoon T. ;
Won, Jong H. ;
Zelenay, Piotr .
NATURE COMMUNICATIONS, 2013, 4
[7]   Iron Encapsulated within Pod-like Carbon Nanotubes for Oxygen Reduction Reaction [J].
Deng, Dehui ;
Yu, Liang ;
Chen, Xiaoqi ;
Wang, Guoxiong ;
Jin, Li ;
Pan, Xiulian ;
Deng, Jiao ;
Sun, Gongquan ;
Bao, Xinhe .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (01) :371-375
[8]   Enhanced Electron Penetration through an Ultrathin Graphene Layer for Highly Efficient Catalysis of the Hydrogen Evolution Reaction [J].
Deng, Jiao ;
Ren, Pengju ;
Deng, Dehui ;
Bao, Xinhe .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (07) :2100-2104
[9]   Highly active and durable non-precious-metal catalysts encapsulated in carbon nanotubes for hydrogen evolution reaction [J].
Deng, Jiao ;
Ren, Pengju ;
Deng, Dehui ;
Yu, Liang ;
Yang, Fan ;
Bao, Xinhe .
ENERGY & ENVIRONMENTAL SCIENCE, 2014, 7 (06) :1919-1923
[10]   Highly active reduction of oxygen on a FeCo alloy catalyst encapsulated in pod-like carbon nanotubes with fewer walls [J].
Deng, Jiao ;
Yu, Liang ;
Deng, Dehui ;
Chen, Xiaoqi ;
Yang, Fan ;
Bao, Xinhe .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (47) :14868-14873