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Atom-scale dispersed palladium in a conductive Pd0.1TaS2lattice with a unique electronic structure for efficient hydrogen evolution
Wang, Dong1; Wang, Xin2; Lu, Yue3; Song, Changsheng1; Pan, Jie1; Li, Chilin1; Sui, Manling3; Zhao, Wei1; Huang, Fuqiang1,2
2017
发表期刊Journal of Materials Chemistry A
ISSN20507488
卷号5期号:43页码:22618-22624
摘要Noble metal catalysts have extraordinary catalytic activity but suffer from high cost; therefore single atom catalysis attracts tremendous attention. Here, we propose atom-scale dispersed palladium (Pd) in a layered TaS2lattice to form new compounds of PdxTaS2, whose crystal structure was resolved by powder X-ray diffraction. The electrical conductivity of metallic Pd0.1TaS2(1.36 × 104S m-1) is twice as large as that of TaS2(6.18 × 103S m-1). This compound applied as a new electrocatalyst for the hydrogen evolution reaction (HER) exhibits excellent catalytic performance with an onset overpotential of 77 mV, superior to those of other catalysts such as TaS2(295 mV) and Pd-loaded TaS2(114 mV). Density functional theory calculations reveal that the interaction of Pd-4d and Ta-5d orbitals results in the upshift of the Fermi level (TaS2versus Pd0.1TaS2) to decrease the barrier height for the HER. Furthermore, the hybridization of Pd-4d and S-3p orbitals builds up pathways along the c axis to improve the conductivity and promote HER performance. It is noted that the amount of Pd used in Pd0.1TaS2is only 4 wt%, compared with 20 wt% in commercial Pd/C catalysts, which is beneficial for its practical application. © 2017 The Royal Society of Chemistry.
DOI10.1039/c7ta06447k
EI入藏号20174604384427
EI主题词Tantalum compounds
EI分类号547.1 Precious Metals - 803 Chemical Agents and Basic Industrial Chemicals - 804 Chemical Products Generally - 931.3 Atomic and Molecular Physics
引用统计
被引频次:2[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.sic.ac.cn/handle/331005/25688
专题中国科学院上海硅酸盐研究所
作者单位1.State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai; 200050, China;
2.State Key Laboratory of Rare Earth Materials Chemistry and Applications, National Laboratory, College of Chemistry and Molecular Engineering, Peking University, No. 5 Yiheyuan Road,Haidian District, Beijing; 100871, China;
3.Institute of Microstructure and Properties of Advanced Materials, Beijing University of Technology, No. 100, Pingleyuan, Chaoyang District, Beijing; 100124, China
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GB/T 7714
Wang, Dong,Wang, Xin,Lu, Yue,et al. Atom-scale dispersed palladium in a conductive Pd0.1TaS2lattice with a unique electronic structure for efficient hydrogen evolution[J]. Journal of Materials Chemistry A,2017,5(43):22618-22624.
APA Wang, Dong.,Wang, Xin.,Lu, Yue.,Song, Changsheng.,Pan, Jie.,...&Huang, Fuqiang.(2017).Atom-scale dispersed palladium in a conductive Pd0.1TaS2lattice with a unique electronic structure for efficient hydrogen evolution.Journal of Materials Chemistry A,5(43),22618-22624.
MLA Wang, Dong,et al."Atom-scale dispersed palladium in a conductive Pd0.1TaS2lattice with a unique electronic structure for efficient hydrogen evolution".Journal of Materials Chemistry A 5.43(2017):22618-22624.
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