Stabilization of Super Electrophilic Pd+2 Cations in Small-Pore SSZ-13 Zeolite

Khivantsev, Konstantin; Jaegers, Nicholas R.; Koleva, Iskra Z.; Aleksandrov, Hristiyan A.; Kovarik, Libor; Engelhard, Mark; Gao, Feng; Wang, Yong; Vayssilov, Georgi N.; Szanyi, Janos

doi:10.1021/acs.jpcc.9b06760

Title: Stabilization of Super Electrophilic Pd⁺² Cations in Small-Pore SSZ-13 Zeolite

Journal Article · Wed Dec 04 00:00:00 EST 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.9b06760· OSTI ID:1617560

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Univ. of Sofia (Bulgaria)

We offer the first observation and characterization of super electrophilic metal cations on a solid support. For Pd/SSZ-13, the results of our combined experimental (Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, high-angle annular dark-field scanning transmission electron microscopy) and density functional theory study reveal that Pd ions in zeolites, previously identified as Pd⁺³ and Pd⁺⁴, are, in fact, present as super electrophilic Pd⁺² species (charge-transfer complex/ion pair with the negatively charged framework oxygens). In this contribution, we reassign the spectroscopic signatures of these species, discuss the unusual coordination environment of “naked” (ligand-free) super electrophilic Pd⁺² in SSZ-13, and their complexes with CO and NO. With CO, nonclassical, highly positive [Pd(CO)₂]²⁺ ions are formed with the zeolite framework acting as a weakly coordinating anion (ion pairs). Nonclassical carbonyl complexes also form with Pt⁺² and Ag⁺ in SSZ-13. The Pd⁺²(CO)₂ complex is remarkably stable in zeolite cages even in the presence of water. Dicarbonyl and nitrosyl Pd⁺² complexes, in turn, serve as precursors to the synthesis of previously inaccessible Pd⁺²–carbonyl–olefin [Pd(CO)(C₂H₄)] and Pd⁺²–nitrosyl–olefin [Pd(NO)(C₂H₄)] complexes. In general, we show that the zeolite framework can stabilize super electrophilic metal (Pd) cations and show the new chemistry of the Pd/SSZ-13 system with implications for adsorption and catalysis.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1617560

Report Number(s):: PNNL-SA-148282

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 1; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 58 works

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Title: Stabilization of Super Electrophilic Pd⁺² Cations in Small-Pore SSZ-13 Zeolite