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Catalysis

Solid Rh crystals isomerize butene without dissolving

Chadwick FM, McKay AI, Martinez-Martinez AJ, et al. · Chemical science · 2017

Open access · cc by · source: Europe PMC

A crystalline Rh σ-alkane complex swaps NBA for alkenes in the solid state and the porous ethene polymorph isomerizes 1-butene with high TOF.

Study at a glance

Design
Other — Solid/gas SC-SC organometallic substitutions and polymorphic catalysis of 1-butene isomerization
N
Solid-state organometallic materials — no sample N
Population
Molecular organometallic crystals ([1-NBA]/[BArF4] ethene polymorphs)
Outcome
SC-SC reactivity and TOF differences between porous hexagonal and octahedral polymorphs

Structured fields used in claim comparison tables when every cited study has a complete layer.

Key findings

NBA is a token ligand; SC-SC ethene substitution gives an octahedral anion cage. The hexagonal porous polymorph (25% void) reaches TOF(90%) = 1160 h–1 versus 20–29 h–1 for nonporous crystals.

Methodology

Authors used solid/gas substitution, X-ray, SSNMR, periodic DFT/GIPAW shifts, and compared 1-butene isomerization TOFs of octahedral vs hexagonal ethene polymorphs.

Limitations

Solution lifetimes are minutes; X-ray R-factors are high after SC-SC; industrial TON still far below silica-supported systems.

How this study connects

Role on claims

Each row is a claim on a concept or method page where this paper supports, challenges, or qualifies the statement. Roles are hand-checked — not a model guess.

  • SupportsCatalysisconcept

    This library holds 8 empirical chemistry papers on catalysis with isolated findings, rates or spectra rather than reviews.

    Evidence for the claim as stated.

  • SupportsCatalysisconcept

    A crystalline Rh σ-alkane complex swaps NBA for alkenes in the solid state and the porous ethene polymorph isomerizes 1-butene with high TOF.

    Evidence for the claim as stated.

  • Single-crystal-to-single-crystal XRD can watch a lattice stay crystalline while catalysis turns over. In solid rhodium organometallics, ethene substitution of a token NBA ligand gives an octahedral anion cage; the hexagonal porous polymorph (25% void) reaches TOF(90%) = 1160 h⁻¹ versus 20–29 h⁻¹ for nonporous crystals. Solution lifetimes are minutes, post-substitution R-factors are high, and industrial TON still trails silica-supported systems.

    Evidence for the claim as stated.

  • XRD can show a lattice that is not the working catalyst. The rhodium hexagonal polymorph's 25% void tracks a 1160 versus 20–29 h⁻¹ TOF split, but post-SC-SC R-factors are already high. On carbon-supported Pt, the particles XRD/TEM size (the 6.7 nm mode) are the ORR-active population, not the leftover 1.8 nm primaries. Structure of what was synthesised is not automatically structure of what turns over.

    Evidence for the claim as stated.

Open questions

Tensions this paper is part of

From concept pages' “where studies disagree.” Disagreement means the same question; scope means different assays, populations, or outcomes.

  • Scope difference — different assays, populations, or outcomes

    XRD can show a lattice that is not the working catalyst. The rhodium hexagonal polymorph's 25% void tracks a 1160 versus 20–29 h⁻¹ TOF split, but post-SC-SC R-factors are already high. On carbon-supported Pt, the particles XRD/TEM size (the 6.7 nm mode) are the ORR-active population, not the leftover 1.8 nm primaries. Structure of what was synthesised is not automatically structure of what turns over.

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