Comparison of Methodologies of Activation Barrier Measurements for Reactions with Deactivation

Xie, Zhenhua; Yan, Binhang; Zhang, Li; Chen, Jingguang G.

doi:10.1021/acs.iecr.6b04626

Title: Comparison of Methodologies of Activation Barrier Measurements for Reactions with Deactivation

Journal Article · Wed Jan 25 00:00:00 EST 2017 · Industrial and Engineering Chemistry Research

DOI:https://doi.org/10.1021/acs.iecr.6b04626· OSTI ID:1358017

^[1]; Yan, Binhang ^[2]; Zhang, Li ^[3]; Chen, Jingguang G. ^[4]

Chongqing University (China). College of Power Engineering; Columbia Univ., New York, NY (United States). Department of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
Chongqing University (China). College of Power Engineering
Columbia Univ., New York, NY (United States). Department of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department

In this work, methodologies of activation barrier measurements for reactions with deactivation were theoretically analyzed. Reforming of ethane with CO₂ was introduced as an example for reactions with deactivation to experimentally evaluate these methodologies. Both the theoretical and experimental results showed that due to catalyst deactivation, the conventional method would inevitably lead to a much lower activation barrier, compared to the intrinsic value, even though heat and mass transport limitations were excluded. In this work, an optimal method was identified in order to provide a reliable and efficient activation barrier measurement for reactions with deactivation.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1358017

Report Number(s):: BNL-113829-2017-JA; R&D Project: CO035; KC0302010

Journal Information:: Industrial and Engineering Chemistry Research, Vol. 56, Issue 5; ISSN 0888-5885

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 10 works

Citation information provided by
Web of Science

References (13)

Handbook of Heterogeneous Catalysis https://doi.org/10.1002/9783527610044	book	March 2008
Tests for Transport Limitations in Experimental Catalytic Reactors Mears, D. E. Industrial & Engineering Chemistry Process Design and Development, Vol. 10, Issue 4 https://doi.org/10.1021/i260040a020	journal	October 1971
A review of dry (CO ₂ ) reforming of methane over noble metal catalysts Pakhare, Devendra; Spivey, James Chem. Soc. Rev., Vol. 43, Issue 22 https://doi.org/10.1039/C3CS60395D	journal	January 2014
Identifying Different Types of Catalysts for CO ₂ Reduction by Ethane through Dry Reforming and Oxidative Dehydrogenation Porosoff, Marc D.; Myint, Myat Noe Zin; Kattel, Shyam Angewandte Chemie International Edition, Vol. 54, Issue 51 https://doi.org/10.1002/anie.201508128	journal	November 2015
Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina Peterson, Eric J.; DeLaRiva, Andrew T.; Lin, Sen Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5885	journal	September 2014
Catalyst deactivation Forzatti, P. Catalysis Today, Vol. 52, Issue 2-3 https://doi.org/10.1016/S0920-5861(99)00074-7	journal	September 1999
A review of multiscale modeling of metal-catalyzed reactions: Mechanism development for complexity and emergent behavior Salciccioli, M.; Stamatakis, M.; Caratzoulas, S. Chemical Engineering Science, Vol. 66, Issue 19 https://doi.org/10.1016/j.ces.2011.05.050	journal	October 2011
Toward Benchmarking in Catalysis Science: Best Practices, Challenges, and Opportunities Bligaard, Thomas; Bullock, R. Morris; Campbell, Charles T. ACS Catalysis, Vol. 6, Issue 4 https://doi.org/10.1021/acscatal.6b00183	journal	March 2016
Linear Least Squares Regression Watson, Geoffrey S. The Annals of Mathematical Statistics, Vol. 38, Issue 6 https://doi.org/10.1214/aoms/1177698603	journal	December 1967
A diagnostic test of the kinetic regime in a packed bed reactor Koros, R. M.; Nowak, E. J. Chemical Engineering Science, Vol. 22, Issue 3 https://doi.org/10.1016/0009-2509(67)80134-9	journal	March 1967
Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts Matsubu, John C.; Zhang, Shuyi; DeRita, Leo Nature Chemistry, Vol. 9, Issue 2 https://doi.org/10.1038/nchem.2607	journal	September 2016
Isolated Metal Active Site Concentration and Stability Control Catalytic CO ₂ Reduction Selectivity Matsubu, John C.; Yang, Vanessa N.; Christopher, Phillip Journal of the American Chemical Society, Vol. 137, Issue 8 https://doi.org/10.1021/ja5128133	journal	February 2015
Review of Pt-Based Bimetallic Catalysis: From Model Surfaces to Supported Catalysts Yu, Weiting; Porosoff, Marc D.; Chen, Jingguang G. Chemical Reviews, Vol. 112, Issue 11, p. 5780-5817 https://doi.org/10.1021/cr300096b	journal	August 2012

Similar Records

Evaluation of Catalyst Deactivation during Catalytic Steam Reforming of Biomass-Derived Syngas

Journal Article · Sat Jan 01 00:00:00 EST 2005 · Industrial and Engineering Chemistry Research · OSTI ID:1358017

Bain, R L; Dayton, D C; Carpenter, D L; +5 more

Reforming of methane with carbon dioxide to synthesis gas over supported rhodium catalysts: I. Effects of support and metal crystallite size on reaction activity and deactivation characteristics

Journal Article · Mon Jan 01 00:00:00 EST 1996 · Journal of Catalysis · OSTI ID:1358017

Zhang, Z L; Tsipouriari, V A; Efstathiou, A M

Bench- and Pilot-Scale Studies of Reaction and Regeneration of Ni-Mg-K/Al2O3 for Catalytic Conditioning of Biomass-Derived Syngas

Journal Article · Tue May 01 00:00:00 EDT 2012 · Topics in Catalysis · OSTI ID:1358017

Magrini-Bair, K A; Jablonski, W S; Parent, Y O; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Comparison of Methodologies of Activation Barrier Measurements for Reactions with Deactivation

Citation Formats

References (13)

Similar Records

Related Subjects