Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 22, Pages 7169-7177Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b02688
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Funding
- Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001015]
- Pre-973 Program [2010CB635114]
- National Natural Science Foundation of China [21371099, 21401021, 21403033]
- China Postdoctoral Science Foundation [2014M551154]
- Science and Technology Development Planning of Jilin Province [20140520089JH, 20140203006GX]
- NSF of Jiangsu Province of China [BK20130043]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials
- Fundamental Research Funds for the Central Universities [14QNJJ013]
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Two novel polyoxometalate (POM)-based metal-organic frameworks (MOFs), [TBA](3)[epsilon-PMo(V)8Mo(4)(VI)O(36)(OH)(4)Zn-4][BTB](4/3).xGuest (NENU-500, BTB = benzene tribenzoate, TBA(+) = tetrabutylammonium ion) and [TBA](3)[epsilon-(PMo8Mo4O37)-Mo-V-O-VI(OH)(3)Zn-4][BPT] (NENU-501, BPT = [1,1'-biphenyl]-3,4',5-tricarboxylate), were isolated. In these compounds, the POM fragments serving as nodes were directly connected with organic ligands giving rise to three-dimensional (3D) open frameworks. The two anionic frameworks were balanced by TBA(+) ions residing inside the open channels. They exhibit not only good stability in air but also tolerance to acidic and basic media. Furthermore, they were employed as electrocatalysts for the hydrogen evolution reaction (HER) owing to the combination of the redox activity of a POM unit and the porosity of a MOF. Meanwhile, the HER activities of epsilon(trim)(4/3), NENU-5, and HKUST-1 were also studied for comparison. Remarkably, as a 3D hydrogen-evolving cathode operating in acidic electrolytes, NENU-500 exhibits the highest activity among all MOF materials. It shows an onset overpotential of 180 mV and a Tafel slope of 96 mV.dec(-1), and the catalytic current density can approach 10 mA.cm(-2) at an overpotential of 237 mV. Moreover, NENU-500 and NENU-501 maintain their electrocatalytic activities after 2000 cycles.
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