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

doi:10.3390/molecules28052017

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^*

^*此作品的通讯作者

化学与化工学院

Beijing Institute of Technology

科研成果: 期刊稿件 › 文章 › 同行评审

1 引用（Scopus）

摘要

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.

源语言	英语
文章编号	2017
期刊	Molecules
卷	28
期	5
DOI	https://doi.org/10.3390/molecules28052017
出版状态	已出版 - 3月 2023

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title = "Structurally-New Hexadecanuclear Ni-Containing Silicotungstate with Catalytic Hydrogen Generation Activity",

abstract = "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.",

keywords = "Ni substitution, hydrogen production, photocatalysis, polyoxometalates",

author = "Yequn Wang and Xing Xin and Yeqin Feng and Manzhou Chi and Ruijie Wang and Tianfu Liu and Hongjin Lv",

note = "Publisher Copyright: {\textcopyright} 2023 by the authors.",

year = "2023",

month = mar,

doi = "10.3390/molecules28052017",

language = "English",

volume = "28",

journal = "Molecules",

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T1 - Structurally-New Hexadecanuclear Ni-Containing Silicotungstate with Catalytic Hydrogen Generation Activity

AU - Wang, Yequn

AU - Xin, Xing

AU - Feng, Yeqin

AU - Chi, Manzhou

AU - Wang, Ruijie

AU - Liu, Tianfu

AU - Lv, Hongjin

PY - 2023/3

Y1 - 2023/3

N2 - 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.

AB - 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.

KW - Ni substitution

KW - hydrogen production

KW - photocatalysis

KW - polyoxometalates

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U2 - 10.3390/molecules28052017

DO - 10.3390/molecules28052017

M3 - Article

C2 - 36903264

AN - SCOPUS:85149862854

SN - 1420-3049

VL - 28

JO - Molecules

JF - Molecules

IS - 5

M1 - 2017

ER -

Structurally-New Hexadecanuclear Ni-Containing Silicotungstate with Catalytic Hydrogen Generation Activity

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