Boosting the activity of PdAg2/Al2O3 supported catalysts towards the selective acetylene hydrogenation by means of CO-induced segregation: A combined NAP XPS and mass-spectrometry study

被引:13
作者
Bukhtiyarov, A. V. [1 ,4 ]
Panafidin, M. A. [1 ]
Prosvirin, I. P. [1 ]
Mashkovsky, I. S. [2 ]
Markov, P. V. [1 ,2 ]
Rassolov, A. V. [2 ]
Smirnova, N. S. [1 ,2 ]
Baeva, G. N. [2 ]
Rameshan, C. [3 ]
Rameshan, R. [3 ]
Zubavichus, Y. V. [1 ]
Bukhtiyarov, V. I. [1 ]
Stakheev, A. Yu. [2 ]
机构
[1] Boreskov Inst Catalysis, Lavrentieva ave 5, Novosibirsk 630090, Russia
[2] ND Zelinskii Inst Organ Chem, Leninsky Prospect 47, Moscow 119991, Russia
[3] Tech Univ Wien, Inst Mat Chem, Getreidemarkt 9-BC-01, A-1060 Vienna, Austria
[4] RAS, Boreskov Inst Catalysis SB, Lavrentieva Ave 5, Novosibirsk 630090, Russia
基金
俄罗斯科学基金会;
关键词
Near-ambient pressure X-ray photoelectron; spectroscopy; CO adsorption-induced segregation; Pd-Ag bimetallic catalysts; Acetylene hydrogenation; In situ measurements; SURFACE SEGREGATION; AG/HOPG CATALYSTS; IN-SITU; PD; PERFORMANCE; AG; DEACTIVATION; ADSORPTION; OXIDATION; ETHYLENE;
D O I
10.1016/j.apsusc.2022.154497
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
Selective hydrogenation (or semi-hydrogenation) of acetylene into ethylene is an important industrial process. The aim of the present work is thus to learn regularities governing the CO-induced segregation and elaborate practical procedures for tuning the surface structure of Pd-Ag nanoparticles to improve their catalytic performance towards the selective hydrogenation of acetylene to ethylene. Utilizing NAP XPS the CO adsorption-induced Pd atoms segregation in supported PdAg2/Al2O3 catalysts already at room temperature has been shown. The surface enrichment with Pd further increases if the treatment temperature is increased up to 250 ?. This specific configuration with a redistributed Pd/Ag surface atomic ratio is appreciably stable and self -sustained even at the absence of CO at moderately elevated temperatures. Nevertheless, a reductive treatment in hydrogen at 450 ? reverts the nanoparticle surface structure to the pristine state. Catalytic properties of this peculiar CO-induced configuration of PdAg2/Al2O3 towards the selective acetylene hydrogenation was investigated using a combination of NAP XPS and MS techniques. The PdAg2/Al2O3 catalyst with the surface enriched with Pd due to the CO-induced segregation manifests improved activity with 100 % selectivity under the conditions used. The results obtained clearly demonstrate that CO adsorption-induced segregation is a powerful tool that can be used to optimize the surface composition and catalytic performance of bimetallic nanoparticles.
引用
收藏
页数:7
相关论文
共 49 条
[1]   High catalytic performance of Al-Pd-(Ru, Fe) icosahedral approximants for acetylene semi-hydrogenation [J].
Abe, Keishi ;
Tsukuda, Ryota ;
Fujita, Nobuhisa ;
Kameoka, Satoshi .
RSC ADVANCES, 2021, 11 (25) :15296-15300
[2]  
[Anonymous], XPSPEAK
[3]   AgPd and CuPd Catalysts for Selective Hydrogenation of Acetylene [J].
Ball, Madelyn R. ;
Rivera-Dones, Keishla R. ;
Gilcher, Elise B. ;
Ausman, Samantha F. ;
Hullfish, Cole W. ;
Lebron, Edgard A. ;
Dumesic, James A. .
ACS CATALYSIS, 2020, 10 (15) :8567-8581
[4]   Selective electrocatalytic semihydrogenation of acetylene impurities for the production of polymer-grade ethylene [J].
Bu, Jun ;
Liu, Zhenpeng ;
Ma, Wenxiu ;
Zhang, Lei ;
Wang, Tao ;
Zhang, Hepeng ;
Zhang, Qiuyu ;
Feng, Xinliang ;
Zhang, Jian .
NATURE CATALYSIS, 2021, 4 (07) :557-564
[5]   In situ formation of the active sites in Pd-Au bimetallic nanocatalysts for CO oxidation: NAP (near ambient pressure) XPS and MS study [J].
Bukhtiyarov, A. V. ;
Prosvirin, I. P. ;
Saraev, A. A. ;
Klyushin, A. Yu. ;
Knop-Gericke, A. ;
Bukhtiyarov, V. I. .
FARADAY DISCUSSIONS, 2018, 208 :255-268
[6]  
Bukhtiyarov VI, 2001, USP KHIM+, V70, P167
[7]   Characterization by CO/FTIR spectroscopy of Pd/silica catalysts and its correlation with syn-gas conversion [J].
Cabilla, GC ;
Bonivardi, AL ;
Baltanás, MA .
CATALYSIS LETTERS, 1998, 55 (3-4) :147-156
[8]   Surface Segregation of Pd from TiO2-Supported AuPd Nanoalloys under CO Oxidation Conditions Observed Insitu by ETEM and DRIFTS [J].
Delannoy, Laurent ;
Giorgio, Suzanne ;
Mattei, Jean Gabriel ;
Henry, Claude R. ;
El Kolli, Nadia ;
Methivier, Christophe ;
Louis, Catherine .
CHEMCATCHEM, 2013, 5 (09) :2707-2716
[9]   Model Ag/HOPG catalysts: preparation and STM/XPS study [J].
Demidov, Demid V. ;
Prosvirin, Igor P. ;
Sorokin, Alexei M. ;
Bukhtiyarov, Valerii I. .
CATALYSIS SCIENCE & TECHNOLOGY, 2011, 1 (08) :1432-1439
[10]   A study on structural features of bimetallic Pd-M/C (M: Zn, Ga, Ag) catalysts for liquid-phase selective hydrogenation of acetylene [J].
Glyzdova, Dania V. ;
Vedyagin, Aleksey A. ;
Tsapina, Anna M. ;
Kaichev, Vasily V. ;
Trigub, Alexander L. ;
Trenikhin, Mikhail V. ;
Shlyapin, Dmitry A. ;
Tsyrulnikov, Pavel G. ;
Lavrenov, Alexander V. .
APPLIED CATALYSIS A-GENERAL, 2018, 563 :18-27