Superassembly of Surface-Enriched Ru Nanoclusters from Trapping-Bonding Strategy for Efficient Hydrogen Evolution

被引:99
作者
Liang, Qirui [1 ]
Li, Qizhen
Xie, Lei [1 ]
Zeng, Hui [1 ]
Zhou, Shan [1 ]
Huang, Yanan [1 ]
Yan, Miao [1 ]
Zhang, Xin [1 ]
Liu, Tianyi [1 ]
Zeng, Jie [1 ]
Liang, Kang [2 ]
Terasaki, Osamu [3 ]
Zhao, Dongyuan [1 ]
Jiang, Lei [4 ,5 ]
Kong, Biao [1 ]
机构
[1] Fudan Univ, Adv Mat Lab, Shanghai Key Lab Mol Catalysis & Innovat Mat iChE, Dept Chem,Collaborat Innovat Ctr Chem Energy Mat, Shanghai 200438, Peoples R China
[2] Univ New South Wales, Sch Chem Engn, Sydney, NSW, Australia
[3] ShanghaiTech Univ, Sch Phys Sci & Technol, Ctr High Resolut Elect Microscopy, Shanghai 201210, Peoples R China
[4] Chinese Acad Sci, CAS Key Lab Bio Inspired Mat, Beijing 100190, Peoples R China
[5] Chinese Acad Sci, Interfacial Sci Tech Inst Phys & Chem, Beijing 100190, Peoples R China
基金
上海市自然科学基金; 中国国家自然科学基金;
关键词
electrocatalyst; hydrogenation; metal-organic frameworks; ruthenium; clusters; HIGH-PERFORMANCE; PH; ELECTROCATALYSTS; CATALYSTS; ENERGY; NANOCATALYST; DESIGN; COP;
D O I
10.1021/acsnano.2c00901
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Hydrogen evolution reaction (HER) through water splitting is a potential technology to realize the sustainable production of hydrogen, yet the tardy water dissociation and costly Pt-based catalysts inhibit its development. Here, a trapping-bonding strategy is proposed to realize the superassembly of surface-enriched Ru nanoclusters on a phytic acid modified nitrogen-doped carbon framework (denoted as NCPO-Ru NCs). The modified framework has a high affinity to metal cations and can trap plenty of Ru ions. The trapped Ru ions are mainly distributed on the surface of the framework and can form Ru nanoclusters at 50 degrees C with the synergistic effect of vacancies and phosphate groups. By adjusting the content of phytic acid, surface-enriched Ru nanoclusters with adjustable distribution and densities can be obtained. Benefiting from the adequate exposure of the active sites and dense distribution of ultrasmall Ru nanoclusters, the obtained NCPO-Ru NCs catalyst can effectively drive HER in alkaline electrolytes and show an activity (at overpotential of 50 mV) about 14.3 and 9.6 times higher than that of commercial Ru/C and Pt/C catalysts, respectively. Furthermore, the great performance in solar to hydrogen generation through water splitting provides more flexibility for wide applications of NCPO-Ru NCs.
引用
收藏
页码:7993 / 8004
页数:12
相关论文
共 58 条
[1]   Multifunctional Mo-N/C@MoS2 Electrocatalysts for HER, OER, ORR, and Zn-Air Batteries [J].
Amiinu, Ibrahim Saana ;
Pu, Zonghua ;
Liu, Xiaobo ;
Owusu, Kwadwo Asare ;
Monestel, Hellen Gabriela Rivera ;
Boakye, Felix Ofori ;
Zhang, Haining ;
Mu, Shichun .
ADVANCED FUNCTIONAL MATERIALS, 2017, 27 (44)
[2]   A Self-Standing High-Performance Hydrogen Evolution Electrode with Nanostructured NiCo2O4/CuS Heterostructures [J].
An, Li ;
Huang, Liang ;
Zhou, Panpan ;
Yin, Jie ;
Liu, Hongyan ;
Xi, Pinxian .
ADVANCED FUNCTIONAL MATERIALS, 2015, 25 (43) :6814-6822
[3]   Carbon capture and storage update [J].
Boot-Handford, M. E. ;
Abanades, J. C. ;
Anthony, E. J. ;
Blunt, M. J. ;
Brandani, S. ;
Mac Dowell, N. ;
Fernandez, J. R. ;
Ferrari, M. -C. ;
Gross, R. ;
Hallett, J. P. ;
Haszeldine, R. S. ;
Heptonstall, P. ;
Lyngfelt, A. ;
Makuch, Z. ;
Mangano, E. ;
Porter, R. T. J. ;
Pourkashanian, M. ;
Rochelle, G. T. ;
Shah, N. ;
Yao, J. G. ;
Fennell, P. S. .
ENERGY & ENVIRONMENTAL SCIENCE, 2014, 7 (01) :130-189
[4]   The path towards sustainable energy [J].
Chu, Steven ;
Cui, Yi ;
Liu, Nian .
NATURE MATERIALS, 2017, 16 (01) :16-22
[5]   Opportunities and challenges for a sustainable energy future [J].
Chu, Steven ;
Majumdar, Arun .
NATURE, 2012, 488 (7411) :294-303
[6]   Defective Metal-Organic Frameworks [J].
Dissegna, Stefano ;
Epp, Konstantin ;
Heinz, Werner R. ;
Kieslich, Gregor ;
Fischer, Roland A. .
ADVANCED MATERIALS, 2018, 30 (37)
[7]   Wavelet analysis of extended x-ray absorption fine structure data [J].
Funke, H ;
Scheinost, AC ;
Chukalina, M .
PHYSICAL REVIEW B, 2005, 71 (09)
[8]   A new FEFF-based wavelet for EXAFS data analysis [J].
Funke, Harald ;
Chukalina, Marina ;
Scheinost, Andreas C. .
JOURNAL OF SYNCHROTRON RADIATION, 2007, 14 :426-432
[9]   Co-Ni-B nanocatalyst for efficient hydrogen evolution reaction in wide pH range [J].
Gupta, S. ;
Patel, N. ;
Fernandes, R. ;
Kadrekar, R. ;
Dashora, Alpa ;
Yadav, A. K. ;
Bhattacharyya, D. ;
Jha, S. N. ;
Miotello, A. ;
Kothari, D. C. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 192 :126-133
[10]   Identification of active edge sites for electrochemical H2 evolution from MoS2 nanocatalysts [J].
Jaramillo, Thomas F. ;
Jorgensen, Kristina P. ;
Bonde, Jacob ;
Nielsen, Jane H. ;
Horch, Sebastian ;
Chorkendorff, Ib .
SCIENCE, 2007, 317 (5834) :100-102