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Title: Adsorption of sulfur on bimetallic surfaces: Formation of copper sulfides on Pt(111) and Ru(001)

Abstract

It has been found that by making specific bimetallic systems (in this case a noble metal deposited on a transition metal surface) one can change the catalytic activity and selectivity of the metals for reactions that lead to the conversion of hydrocarbons. A major problem associated with these catalysts is sulfur poisoning. The interaction of sulfur and copper on Pt(111) and Ru(001) has been examined using X-ray photoelectron spectroscopy (XPS) and thermal desorption mass spectroscopy (TDS). Cu/Pt (111) and Cu/Ru(001) surfaces were exposed to S{sub 2} gas at 300 K. It was found that for both substrates stable copper-sulfide films were formed, of which the Cu-S/Ru(001) system was the more stable. The decomposition of the Cu{sub 2}S films on Pt(111) occurred at 600--850 K and on Ru(001) at 900--1,000 K. Breakdown of the films led to evolution into the gas phase of sulfur (mainly as S{sub 2}) without desorption of copper or the sulfur chemisorbed on the substrate. This chemisorbed sulfur desorbed in a broad feature from 1,000--1,500 K. For the Ru(001) substrate the Cu atoms remained on the surface until they desorbed at 1080 K, while on Pt(111) the Cu atoms migrated into the Pt(111) surface to form amore » subsurface Cu-Pt alloy and no Cu desorption features were seen at temperatures as high as 1,300 K. On Pt(111), copper-sulfide promoted the formation of a bulk-like platinum sulfide. No sulfidation of ruthenium was detected in the presence of copper-sulfide films. For both substrates the sulfur atoms were found to highly perturb the copper sites, decreasing the ability of the noble-metal ad atoms to adsorb CO.« less

Authors:
;
Publication Date:
Research Org.:
Brookhaven National Lab., Upton, NY (United States)
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10191271
Report Number(s):
BNL-60952; CONF-941001-4
ON: DE95001994; TRN: AHC29428%%6
DOE Contract Number:
AC02-76CH00016
Resource Type:
Technical Report
Resource Relation:
Conference: 41. annual American Vacuum Society symposium,Denver, CO (United States),24-28 Oct 1994; Other Information: PBD: [1994]
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 02 PETROLEUM; CATALYSTS; POISONING; COPPER; SORPTIVE PROPERTIES; PLATINUM; RUTHENIUM; SULFUR; ADSORPTION; CARBON MONOXIDE; BIMETALS; CHEMISORPTION; EXPERIMENTAL DATA; 400201; 020400; CHEMICAL AND PHYSICOCHEMICAL PROPERTIES; PROCESSING

Citation Formats

Kuhn, M., and Rodriguez, J.A.. Adsorption of sulfur on bimetallic surfaces: Formation of copper sulfides on Pt(111) and Ru(001). United States: N. p., 1994. Web. doi:10.2172/10191271.
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Kuhn, M., & Rodriguez, J.A.. Adsorption of sulfur on bimetallic surfaces: Formation of copper sulfides on Pt(111) and Ru(001). United States. doi:10.2172/10191271.
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Kuhn, M., and Rodriguez, J.A.. Tue . "Adsorption of sulfur on bimetallic surfaces: Formation of copper sulfides on Pt(111) and Ru(001)". United States. doi:10.2172/10191271. https://www.osti.gov/servlets/purl/10191271.
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@article{osti_10191271,
title = {Adsorption of sulfur on bimetallic surfaces: Formation of copper sulfides on Pt(111) and Ru(001)},
author = {Kuhn, M. and Rodriguez, J.A.},
abstractNote = {It has been found that by making specific bimetallic systems (in this case a noble metal deposited on a transition metal surface) one can change the catalytic activity and selectivity of the metals for reactions that lead to the conversion of hydrocarbons. A major problem associated with these catalysts is sulfur poisoning. The interaction of sulfur and copper on Pt(111) and Ru(001) has been examined using X-ray photoelectron spectroscopy (XPS) and thermal desorption mass spectroscopy (TDS). Cu/Pt (111) and Cu/Ru(001) surfaces were exposed to S{sub 2} gas at 300 K. It was found that for both substrates stable copper-sulfide films were formed, of which the Cu-S/Ru(001) system was the more stable. The decomposition of the Cu{sub 2}S films on Pt(111) occurred at 600--850 K and on Ru(001) at 900--1,000 K. Breakdown of the films led to evolution into the gas phase of sulfur (mainly as S{sub 2}) without desorption of copper or the sulfur chemisorbed on the substrate. This chemisorbed sulfur desorbed in a broad feature from 1,000--1,500 K. For the Ru(001) substrate the Cu atoms remained on the surface until they desorbed at 1080 K, while on Pt(111) the Cu atoms migrated into the Pt(111) surface to form a subsurface Cu-Pt alloy and no Cu desorption features were seen at temperatures as high as 1,300 K. On Pt(111), copper-sulfide promoted the formation of a bulk-like platinum sulfide. No sulfidation of ruthenium was detected in the presence of copper-sulfide films. For both substrates the sulfur atoms were found to highly perturb the copper sites, decreasing the ability of the noble-metal ad atoms to adsorb CO.},
doi = {10.2172/10191271},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Nov 01 00:00:00 EST 1994},
month = {Tue Nov 01 00:00:00 EST 1994}
}
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Technical Report:
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DOI:  10.2172/10191271
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  • ; - Journal of Vacuum Science and Technology, A
    The interaction of sulfur and copper on Pt(111) and Ru(001) has been examined using x-ray photoelectron spectroscopy and thermal desorption mass spectroscopy. Cu/Pt(111) and Cu/Ru(001) surfaces were exposed to S{sub 2} gas at 300 K. It was found that for both substrates stable copper--sulfide films were formed, of which the Cu--S/Ru(001) system was the more stable. The decomposition of the Cu{sub 2}S films on Pt(111) occurred at 600--850 K and on Ru(001) at 900--1000 K. Breakdown of the films led to evolution into the gas phase of sulfur (mainly as S{sub 2}) without desorption of copper or the sulfur chemisorbedmore » on the substrate. This chemisorbed sulfur desorbed in a broad feature from 1000 to 1500 K. For the Ru(001) substrate the Cu atoms remained on the surface until they desorbed at 1080 K, while on Pt(111) the Cu atoms migrated into the Pt(111) surface to form a subsurface Cu--Pt alloy; no Cu desorption features were seen at temperatures as high as 1300 K. On Pt(111), copper sulfide {ital promoted} the formation of a bulklike platinum sulfide. No sulfidation of ruthenium was detected in the presence of copper--sulfide films. For both substrates the sulfur atoms were found to highly perturb the copper sites, decreasing the ability of the noble-metal adatoms to adsorb CO. {copyright} {ital 1995} {ital American} {ital Vacuum} {ital Society}« less

  • ; - Journal of Physical Chemistry; (United States)
    The coadsorption of S with Cu or Ag on Ru(001) has been investigated using TDS, XPS, XAES, and CO chemisorption. At 300 K, copper and silver atoms in contact with Ru(001) react with S[sub 2] to form noble-metal sulfides. The Cu-S and Ag-S bonds in these surface compounds break at high temperatures (> 800 K) producing sulfur and noble-metal adatoms that compete for the ruthenium electrons. This competition leads to a weakening of 5-6 kcal/mol in the strength of the Ru-Cu and Ru-Ag bonds. A sulfur adatom produces long-range perturbations on the surface, diminishing the ability for bimetallic bonding ofmore » several (5-10) adjacent ruthenium atoms. At [theta][sub s] = 0.2 ML (ML = monolayer), all the ruthenium sites show a strong weakening in their bonding interactions with copper or silver adatoms. Photoemission experiments examining the interaction of S[sub 2] with copper and silver multilayers at 300 K show the formation of thick films of Cu[sub 2]S and Ag[sub 2]S at a fast rate. The decomposition pathways for these films are similar: evolution of S[sub 2] into gas phase, with the noble metal remaining solid. For Ag[sub 2]S films the decomposition process starts around 800 K, whereas Cu[sub 2]S films are stable up to 950 K. 55 refs., 13 figs.« less

  • ; ; - Surface Science
    No abstract prepared.

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  • ; ; ; ... - Journal of American Chemical Society
    No abstract prepared.