In-situ studies of oxidation/reduction of copper in Cu-CHA SCR catalysts: Comparison of fresh and SO2-poisoned catalysts

Bergman, Susanna L.Yale NUS College,Yale NUS Coll, Sci Div, Singapore 138527, Singapore. (författare)

QC 20200608
SO2-poisoning results in deactivation of Cu-CHA SCR under standard SCR conditions; however regeneration at 700 °C completely restores the SCR performance. To understand the nature of these effects, Cu-species in the fresh and poisoned catalysts were characterized by in-situ temperature-dependent time-resolved Cu K-edge X-ray absorption spectroscopy using the multivariate curve resolution alternating least squares (MCR-ALS) approach and continuous Cauchy wavelet transforms. The extracted chemically-meaningful reference spectra of Cu-species were analyzed by DFT-assisted XANES calculations. Cu-bisulfates were found as the most energetically favorable poisoned Cu-species. The response of Cu-species to a reducing environment differs in the fresh and SO2-poisoned catalysts. Differences in reducibility are related to the formation of quasi-linear Cu-complexes in the SO2-poisoned catalyst formed during heating in H2/He. Heating in H2/He leads to partial desulfurization of the poisoned catalyst. Cooling in H2/He after heating results in more facile formation of Cu-metal clusters in fresh catalyst than in SO2-poisoned.

Dahlin, SandraKTH,Processteknologi,Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)(Swepub:kth)u1k6111x (författare)
Mesilov, Vitaly V.Yale NUS College,Yale NUS Coll, Sci Div, Singapore 138527, Singapore. (författare)
Xiao, YangYale NUS College,Yale NUS Coll, Sci Div, Singapore 138527, Singapore. (författare)
Englund, Johanna,1988Chalmers tekniska högskola,Chalmers University of Technology,Chalmers Univ Technol, Competence Ctr Catalysis, S-41296 Gothenburg, Sweden.(Swepub:cth)johancar (författare)
Xi, ShiboASTAR, Singapore Synchrotron Light Source, ICES, Singapore 117603, Singapore. (författare)
Tang, ChunhuaUniversiti Kebangsaan Singapura (NUS),National University of Singapore (NUS),Natl Univ Singapore, Mat Sci & Engn, Singapore 117575, Singapore. (författare)
Skoglundh, Magnus,1965Chalmers tekniska högskola,Chalmers University of Technology,Chalmers Univ Technol, Competence Ctr Catalysis, S-41296 Gothenburg, Sweden.(Swepub:cth)skoglund (författare)
Pettersson, Lars J.KTH,Kemiteknik,Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)(Swepub:kth)u1kcgmtv (författare)
Bernasek, Steven L.Yale NUS College,Yale NUS Coll, Sci Div, Singapore 138527, Singapore. (författare)
Yale NUS CollegeYale NUS Coll, Sci Div, Singapore 138527, Singapore. (creator_code:org_t)

Av författaren/redakt...: Bergman, Susanna ...; Dahlin, Sandra; Mesilov, Vitaly ...; Xiao, Yang; Englund, Johanna ...; Xi, Shibo; visa fler...; Tang, Chunhua; Skoglundh, Magnu ...; Pettersson, Lars ...; Bernasek, Steven ...; visa färre...

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