Structurally-New Hexadecanuclear Ni-Containing Silicotungstate with Catalytic Hydrogen Generation Activity
Yequn Wang,
Xing Xin,
Yeqin Feng,
Manzhou Chi,
Ruijie Wang,
Tianfu Liu,
Hongjin Lv
Affiliations
Yequn Wang
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Xing Xin
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Yeqin Feng
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Manzhou Chi
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Ruijie Wang
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Tianfu Liu
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
Hongjin Lv
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
A structurally-new, carbon-free hexadecanuclear Ni-containing silicotungstate, [Ni16(H2O)15(OH)9(PO4)4(SiW9O34)3]19-, has been facilely synthesized using a one-pot, solution-based synthetic method systematically characterized by single-crystal X-ray diffraction and several other techniques. The resulting complex works as a noble-metal-free catalyst for visible-light-driven catalytic generation of hydrogen, by coupling with a [Ir(coumarin)2(dtbbpy)][PF6] photosensitizer and a triethanolamine (TEOA) sacrificial electron donor. Under minimally optimized conditions, a turnover number (TON) of 842 was achieved for TBA-Ni16P4(SiW9)3-catalyzed hydrogen evolution system. The structural stability of TBA-Ni16P4(SiW9)3 catalyst under photocatalytic conditions was evaluated by the mercury-poisoning test, FT-IR, and DLS measurements. The photocatalytic mechanism was elucidated by both time-solved luminescence decay and static emission quenching measurements.
