Covalent immobilization of molecular complexes on metal-organic frameworks towards robust and highly efficient heterogeneous water oxidation catalysts

被引：24

作者：

Liang, Xiangming ^{[1
,2
]}

Yang, Sizhuo ^{[3
]}

Yang, Junyi ^{[1
,2
]}

Sun, Wanjun ^{[1
,2
]}

Li, Xiangyang ^{[1
,2
]}

Ma, Baochun ^{[1
,2
]}

Huang, Jier ^{[3
]}

Zhang, Jiangwei ^{[4
,5
]}

Duan, Lele ^{[6
,7
]}

Ding, Yong ^{[1
,2
]}

机构：

[1] Lanzhou Univ, State Key Lab Appl Organ Chem, Key Lab Nonferrous Met Chem & Resources Utilizat, 222 Tianshui South Rd, Lanzhou 730000, Peoples R China

[2] Lanzhou Univ, Coll Chem & Chem Engn, 222 Tianshui South Rd, Lanzhou 730000, Peoples R China

[3] Marquette Univ, Dept Chem, Milwaukee, WI 53201 USA

[4] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

[5] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

[6] Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China

[7] Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Guangdong, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2021年 / 291卷

基金：

中国国家自然科学基金;

关键词：

Covalent immobilization; Water oxidation; Metal-organic framework; Molecular complex; RUTHENIUM CATALYST; CHALLENGES; EVOLUTION; INSIGHT; SURFACE; LIGAND; DOTS; PH;

D O I：

10.1016/j.apcatb.2021.120070

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The major challenges to practical implementation of efficient noble metal based molecular water oxidation catalysts are their stability and recycle ability. Herein, noble metal Ru based molecular water oxidation catalysts were covalently anchored in MOFs through "amide bond" as bridges, which leads to the formation of highefficiency and robust heterogeneous catalysts for water oxidation reaction. We show that the efficiency for CeIV-driven water oxidation was significantly enhanced by 120 times when the Ru molecules were immobilized on the frameworks of MIL-101(Cr). The relationship between recycle stability and the structure of the Ru complexes covalently anchored in MOFs was carefully studied by recycle tests and various characterization methods. [Ru(terpy)(pic)2(H2O)]2+ was directly certified as real catalytic species instead of the original complex [Ru(terpy)(pic)2Cl]+ by the X-ray absorption spectroscopy and control experiments. The synthetic method of hybrid catalysts offers a good strategy for enhancing water oxidation activity and stability of molecular catalysts.

引用

页数：12

共 76 条

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