Metal Nanoparticle/Carbon Quantum Dot Composite as a Photocatalyst for High-Efficiency Cyclohexane Oxidation

被引：300

作者：

Liu, Ruihua ^{[1
,2
]}

Huang, Hui ^{[1
,2
]}

Li, Haitao ^{[1
,2
]}

Liu, Yang ^{[1
,2
]}

Zhong, Jun ^{[1
,2
]}

Li, Youyong ^{[1
,2
]}

Zhang, Shuo ^{[3
]}

Kang, Zhenhui ^{[1
,2
]}

机构：

[1] Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Suzhou, Peoples R China

[2] Soochow Univ, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou, Peoples R China

[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China

来源：

ACS CATALYSIS | 2014年 / 4卷 / 01期

基金：

中国国家自然科学基金;

关键词：

carbon quantum dots; composites; cyclohexane oxidation; photocatalysis; selective oxidation; SELECTIVE OXIDATION; GOLD NANOPARTICLES; CATALYTIC-OXIDATION; CARBON NANODOTS; HYDROGEN-PEROXIDE; LOW-TEMPERATURE; ADIPIC ACID; X-RAY; HYDROXYLATION; HYDROCARBONS;

D O I：

10.1021/cs400913h

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：

High-efficiency and high-selectivity catalytic oxidation of alkanes under mild conditions is a major objective of current catalysis chemistry and chemical production. Despite extensive development efforts on new catalysts for cyclohexane oxidation, current commercial processes still suffer from low conversion, poor selectivity, and excessive production of waste. We demonstrate the design and synthesis of composites made from metal nanoparticles and carbon quantum dots (CQDs) for high-efficiency and high-selectivity photocatalyst systems for the green oxidation of cyclohexane. Remarkably, the present Au nanoparticles/CQDs composite photocatalyst yields 63.8% conversion efficiency and 99.9% selectivity for the green oxidation of cyclohexane to cyclohexanone, using H2O2 under visible light at room temperature. Given its diversity and versatility of structural and composition design, metal nanoparticles/CQDs composites may provide a powerful pathway for the development of high-performance catalysts and production processes for green chemical industry.

引用

页码：328 / 336

页数：9

共 35 条

[1] Luminescent Carbon Nanodots: Emergent Nanolights [J].

Baker, Sheila N. ;

Baker, Gary A. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (38) :6726-6744

[2] One-Phase Synthesis of Surface Modified Gold Nanoparticles and Generation of SERS Substrate by Seed Growth Method [J].

Baruah, Bharat ;

Craighead, Carl ;

Abolarin, Caleb .

LANGMUIR, 2012, 28 (43) :15168-15176

[3] Innovative direct synthesis of adipic acid by air oxidation of cyclohexane [J].

Bonnet, Didier ;

Ireland, Tania ;

Fache, Eric ;

Simonato, Jean-Pierre .

GREEN CHEMISTRY, 2006, 8 (06) :556-559

[4] The mechanism of a C-H bond activation reaction in room-temperature alkane solution [J].

Bromberg, SE ;

Yang, H ;

Asplund, MC ;

Lian, T ;

McNamara, BK ;

Kotz, KT ;

Yeston, JS ;

Wilkens, M ;

Frei, H ;

Bergman, RG ;

Harris, CB .

SCIENCE, 1997, 278 (5336) :260-263

[5] Nitrogen-, phosphorous- and boron-doped carbon nanotubes as catalysts for the aerobic oxidation of cyclohexane [J].

Cao, Yonghai ;

Yu, Hao ;

Tan, Jun ;

Peng, Feng ;

Wang, Hongjuan ;

Li, Jing ;

Zheng, Wenxu ;

Wong, Ning-Bew .

CARBON, 2013, 57 :433-442

[6] Synthesis, properties, and structure of a stable cobalt(III) alkyl peroxide complex and its role in the oxidation of cyclohexane [J].

Chavez, FA ;

Nguyen, CV ;

Olmstead, MM ;

Mascharak, PK .

INORGANIC CHEMISTRY, 1996, 35 (21) :6282-6291

[7] Oxidation of Cyclohexane by High-Valent Iron Bispidine Complexes: Tetradentate versus Pentadentate Ligands [J].

Comba, Peter ;

Maurer, Martin ;

Vadivelu, Prabha .

INORGANIC CHEMISTRY, 2009, 48 (21) :10389-10396

[8] CATALYTIC-OXIDATION OF HYDROCARBONS WITH O2 OR H2O2 USING A STERICALLY HINDERED RUTHENIUM COMPLEX [J].

GOLDSTEIN, AS ;

BEER, RH ;

DRAGO, RS .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (06) :2424-2429

[9] Highly Dispersed Copper Species within SBA-15 Introduced by the Hydrophobic Core of a Surfactant Micelle as a Carrier and Their Enhanced Catalytic Activity for Cyclohexane Oxidation [J].

Gu, Jinlou ;

Huang, Ying ;

Elangovan, S. P. ;

Li, Yongsheng ;

Zhao, Wenru ;

Toshio, Iijima ;

Yamazaki, Yasuo ;

Shi, Jianlin .

JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (43) :21211-21217

[10] Co-TUD-1: A ketone-selective catalyst for cyclohexane oxidation [J].

Hamdy, MS ;

Ramanathan, A ;

Maschmeyer, T ;

Hanefeld, U ;

Jansen, JC .

CHEMISTRY-A EUROPEAN JOURNAL, 2006, 12 (06) :1782-1789

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