Multi-functional Ni3C cocatalyst/g-C3N4 nanoheterojunctions for robust photocatalytic H2 evolution under visible light

被引:270
作者
He, Kelin [1 ,2 ]
Xie, Jun [1 ,2 ]
Liu, Zhao-Qing [3 ]
Li, Neng [4 ]
Chen, Xiaobo [5 ]
Hu, Jun [6 ]
Li, Xin [1 ,2 ]
机构
[1] South China Agr Univ, Key Lab Energy Plants Resource & Utilizat, Coll Forestry & Landscape Architecture, Minist Agr, Guangzhou 510642, Guangdong, Peoples R China
[2] South China Agr Univ, Coll Mat & Energy, Guangzhou 510642, Guangdong, Peoples R China
[3] Guangzhou Univ, Sch Chem & Chem Engn,Minist Educ, Guangzhou Key Lab Environm Funct Mat & Technol, Key Lab Water Qual & Conservat Pearl River Delta, Guangzhou 510006, Guangdong, Peoples R China
[4] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Hubei, Peoples R China
[5] Univ Missouri Kansas City, Dept Chem, Kansas City, MO 64110 USA
[6] Northwest Univ, Sch Chem Engn, Xian 710069, Shaanxi, Peoples R China
基金
中国国家自然科学基金; 美国国家科学基金会;
关键词
MOLYBDENUM CARBIDE NANOPARTICLES; GRAPHITIC CARBON NITRIDE; HYDROGEN-EVOLUTION; METAL-FREE; G-C3N4; NANOSHEETS; TUNGSTEN CARBIDE; EFFICIENT ELECTROCATALYSTS; CDS NANOSHEETS; DOPED G-C3N4; GENERATION;
D O I
10.1039/c8ta03048k
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 highly active, non-noble-metal H-2 evolution co-catalysts is appealing yet still remains a great challenge in the promising field of visible-light-driven photocatalytic solar fuel H-2 production. In this work, high quality hexagonal Ni3C nanoparticles were facilely fabricated through the low-temperature thermolysis of nickel acetylacetonate in oleylamine under a nitrogen atmosphere and were then coupled with g-C3N4 by a simple grinding method. The photocatalytic performances of g-C3N4/Ni3C nanoheterojunctions were tested under visible light irradiation using triethanolamine (TEOA) as a hole scavenger. The optimal H-2-production rate of 15.18 mol h(-1) over 15 wt% Ni3C nanoparticle decorated g-C3N4, corresponding to an apparent quantum yield (AQY) of 0.40% at 420 nm, is approximately 116.7 times higher than that of pure g-C3N4 and is even larger than that of the 0.5 wt% Pt/g-C3N4 sample. Well resolved density functional theory (DFT) calculation reveals that the TOP site of Ni3C(113) with a H adsorption energy of -0.97 eV is likely the dominant reaction site for H-2 evolution, rather than the Hollow and Bridge sites. It was also demonstrated by the polarization curves that the Ni3C nanoparticles could act as multi-functional electrocatalysts to improve the kinetics for water oxidation, the oxidation of TEOA, and hydrogen evolution in both acidic and basic media. Therefore, the loading of multi-functional Ni3C cocatalyst nanoparticles onto g-C3N4 can fundamentally promote the rapid transportation/separation of charge carriers, enhance the oxidation kinetics of TEOA, and decrease the overpotential of H-2-evolution, thus favoring significantly enhanced photocatalytic activity. It is highly expected that this work will provide new ideas to develop robust metal carbides as noble-metal-free cocatalysts for high-efficiency and low-cost g-C3N4-based photocatalytic water splitting.
引用
收藏
页码:13110 / 13122
页数:13
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