Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation

被引:688
作者
Zhang, Zailei [1 ]
Zhu, Yihan [2 ]
Asakura, Hiroyuki [3 ,4 ]
Zhang, Bin [1 ]
Zhang, Jiaguang [1 ]
Zhou, Maoxiang [5 ]
Han, Yu [2 ,6 ]
Tanaka, Tsunehiro [3 ,4 ]
Wang, Aiqin [5 ]
Zhang, Tao [5 ]
Yan, Ning [1 ]
机构
[1] Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore
[2] King Abdullah Univ Sci & Technol, Phys Sci & Engn Div, Adv Membranes & Porous Mat Ctr, Thuwal 239556900, Saudi Arabia
[3] Kyoto Univ, Grad Sch Engn, Dept Mol Engn, Kyoto 6158510, Japan
[4] Kyoto Univ, ESICB, Kyoto 6158245, Japan
[5] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[6] King Abdullah Univ Sci & Technol, Phys Sci & Engn Div, KAUST Catalysis Ctr, Thuwal 239556900, Saudi Arabia
关键词
ATOMICALLY DISPERSED PALLADIUM; WATER-GAS SHIFT; PLATINUM NANOPARTICLES; CERIA CATALYSTS; ACTIVE-SITES; METAL; TRANSFORMATION; SPECTROSCOPY; GENERATION; ZEOLITE;
D O I
10.1038/ncomms16100
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Single-atom metal catalysts offer a promising way to utilize precious noble metal elements more effectively, provided that they are catalytically active and sufficiently stable. Herein, we report a synthetic strategy for Pt single-atom catalysts with outstanding stability in several reactions under demanding conditions. The Pt atoms are firmly anchored in the internal surface of mesoporous Al2O3, likely stabilized by coordinatively unsaturated pentahedral Al3+ centres. The catalyst keeps its structural integrity and excellent performance for the selective hydrogenation of 1,3-butadiene after exposure to a reductive atmosphere at 200 degrees C for 24 h. Compared to commercial Pt nanoparticle catalyst on Al2O3 and control samples, this system exhibits significantly enhanced stability and performance for n-hexane hydro-reforming at 550 degrees C for 48 h, although agglomeration of Pt single-atoms into clusters is observed after reaction. In CO oxidation, the Pt single-atom identity was fully maintained after 60 cycles between 100 and 400 degrees C over a one-month period.
引用
收藏
页数:10
相关论文
共 52 条
[1]   Designed Catalysts from Pt Nanoparticles Supported on Macroporous Oxides for Selective Isomerization of n-Hexane [J].
An, Kwangjin ;
Alayoglu, Selim ;
Musselwhite, Nathan ;
Na, Kyungsu ;
Somorjai, Gabor A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (19) :6830-6833
[2]  
[Anonymous], 2015, FORECAST PLATINUM SU
[3]   Furfuraldehyde Hydrogenation on Titanium Oxide-Supported Platinum Nanoparticles Studied by Sum Frequency Generation Vibrational Spectroscopy: Acid-Base Catalysis Explains the Molecular Origin of Strong Metal-Support Interactions [J].
Baker, L. Robert ;
Kennedy, Griffin ;
Van Spronsen, Matthijs ;
Hervier, Antoine ;
Cai, Xiaojun ;
Chen, Shiyou ;
Wang, Lin-Wang ;
Somorjai, Gabor A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (34) :14208-14216
[4]   Ligand-capped Pt nanocrystals as oxide-supported catalysts:: FTIR spectroscopic investigations of the adsorption and oxidation of CO [J].
Borchert, Holger ;
Tenske, Daniela ;
Kolny-Olesiak, Joanna ;
Parisi, Juergen ;
Al-Shamery, Katharina ;
Baeumer, Marcus .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (16) :2923-2926
[5]   Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum [J].
Bruix, Albert ;
Lykhach, Yaroslava ;
Matolinova, Iva ;
Neitzel, Armin ;
Skala, Tomas ;
Tsud, Nataliya ;
Vorokhta, Mykhailo ;
Stetsovych, Vitalii ;
Sevcikova, Klara ;
Myslivecek, Josef ;
Fiala, Roman ;
Vaclavu, Michal ;
Prince, Kevin C. ;
Bruyere, Stephanie ;
Potin, Valerie ;
Illas, Francesc ;
Matolin, Vladimir ;
Libuda, Joerg ;
Neyman, Konstantin M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (39) :10525-10530
[6]   Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts [J].
Cargnello, Matteo ;
Doan-Nguyen, Vicky V. T. ;
Gordon, Thomas R. ;
Diaz, Rosa E. ;
Stach, Eric A. ;
Gorte, Raymond J. ;
Fornasiero, Paolo ;
Murray, Christopher B. .
SCIENCE, 2013, 341 (6147) :771-773
[7]   Study of selective hydrogenation of acetophenone on Pt/SiO2 [J].
Chen, CS ;
Chen, HW ;
Cheng, WH .
APPLIED CATALYSIS A-GENERAL, 2003, 248 (1-2) :117-128
[8]   Molecular Insight into Pt-Catalyzed Chemoselective Hydrogenation of an Aromatic Ketone by In Situ Modulation-Excitation IR Spectroscopy [J].
Chen, Mengmeng ;
Maeda, Nobutaka ;
Baiker, Alfons ;
Huang, Jun .
ACS CATALYSIS, 2012, 2 (09) :2007-2013
[9]   Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst [J].
Choi, Chang Hyuck ;
Kim, Minho ;
Kwon, Han Chang ;
Cho, Sung June ;
Yun, Seongho ;
Kim, Hee-Tak ;
Mayrhofer, Karl J. J. ;
Kim, Hyungjun ;
Choi, Minkee .
NATURE COMMUNICATIONS, 2016, 7
[10]   A NONPOROUS SUPPORTED-PLATINUM CATALYST FOR AROMATIZATION OF N-HEXANE [J].
DAVIS, RJ ;
DEROUANE, EG .
NATURE, 1991, 349 (6307) :313-315