TY - JOUR

T1 - Double oxalates of Rh(III) with Ni(II) and Co(II) – Effective precursors of nanoalloys for hydrocarbons steam reforming

AU - Zadesenets, Andrey V.

AU - Garkul, Ilia A.

AU - Filatov, Evgeny Yu

AU - Sukhikh, Aleksandr S.

AU - Plusnin, Pavel E.

AU - Urlukov, Artem S.

AU - Uskov, Sergey I.

AU - Potemkin, Dmitriy I.

AU - Korenev, Sergey V.

N1 - This research was funded by the Russian Science Foundation , grant number 22-23-00672 (in part of synthesis and catalysts characterization), and by the Ministry of Science and Education of the Russian Federation, under the project 121031700315–2 (in part of synthesis and thermal properties investigation of complex salts) and under the project AAAA-A21-121011390009-1 (in part of catalytic activity investigation). Публикация для корректировки.

PY - 2023/7/12

Y1 - 2023/7/12

N2 - Heteronuclear coordination compounds of d-metals are suitable single-source precursors for bimetallic nanoalloys, which often show extraordinary catalytic properties due to synergetic effect. In particular, Ni- and Rh-based catalysts are highly effective in low temperature steam reforming processes. Double oxalates of Rh with Ni and Co of the formula {[Rh(H2O)2(C2O4)μ-(C2O4)]2M(H2O)2}·6H2O (M = Ni, Co) were synthesized and structurally characterized. According to thermogravimetric analysis, the complexes decompose completely in He and H2 atmospheres to form corresponding nanoalloys at ∼300 °C. The calcination in O2 atmosphere leads to formation of spinel type mixed oxide. The supported Co–Rh/Al2O3 and Ni–Rh/Al2O3 catalysts were prepared by impregnation of double oxalate complexes in porous support with subsequent calcination and tested in propane low temperature steam reforming in CH4 excess. The Co-containing catalyst showed comparable activity regarding to pure Rh/Al2O3 sample, while bimetallic Ni–Rh/Al2O3 catalyst revealed to be appreciably more active, than monometallic catalysts with higher active component loadings. Rh–Ni catalyst allowed for complete propane conversion at T ≈ 350 °C, whereas for Rh catalyst the temperature was T ≈ 410 °C, and Rh–Co did not reach complete C3H8 conversion at all.

AB - Heteronuclear coordination compounds of d-metals are suitable single-source precursors for bimetallic nanoalloys, which often show extraordinary catalytic properties due to synergetic effect. In particular, Ni- and Rh-based catalysts are highly effective in low temperature steam reforming processes. Double oxalates of Rh with Ni and Co of the formula {[Rh(H2O)2(C2O4)μ-(C2O4)]2M(H2O)2}·6H2O (M = Ni, Co) were synthesized and structurally characterized. According to thermogravimetric analysis, the complexes decompose completely in He and H2 atmospheres to form corresponding nanoalloys at ∼300 °C. The calcination in O2 atmosphere leads to formation of spinel type mixed oxide. The supported Co–Rh/Al2O3 and Ni–Rh/Al2O3 catalysts were prepared by impregnation of double oxalate complexes in porous support with subsequent calcination and tested in propane low temperature steam reforming in CH4 excess. The Co-containing catalyst showed comparable activity regarding to pure Rh/Al2O3 sample, while bimetallic Ni–Rh/Al2O3 catalyst revealed to be appreciably more active, than monometallic catalysts with higher active component loadings. Rh–Ni catalyst allowed for complete propane conversion at T ≈ 350 °C, whereas for Rh catalyst the temperature was T ≈ 410 °C, and Rh–Co did not reach complete C3H8 conversion at all.

KW - Bimetallic catalysts

KW - Complex precursors

KW - Nickel

KW - Steam reforming

KW - rhodium

UR - https://www.scopus.com/record/display.uri?eid=2-s2.0-85148367364&origin=inward&txGid=e7c9dd5ac55625b95106313bf6993892

UR - https://www.mendeley.com/catalogue/69774db6-8d95-36a6-9517-32668fecce99/

U2 - 10.1016/j.ijhydene.2023.01.365

DO - 10.1016/j.ijhydene.2023.01.365

M3 - Article

VL - 48

SP - 22428

EP - 22438

JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

IS - 59

ER -