Journal
CCS CHEMISTRY
Volume 4, Issue 8, Pages 2639-2650Publisher
CHINESE CHEMICAL SOC
DOI: 10.31635/ccschem.021.202101454
Keywords
WOx monolayers; metal-acid catalysis; proximity; bifunctional catalysis; acid quantification
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Funding
- Natural Science Foundation of China [21725301, 21932002, 22005007, 21821004]
- National Key R&D Program of China [2017YFB0602200]
- Chinese Post-doctoral Science Foundation [8206300246]
- Junior Fellowship of Beijing National Lab-oratory of Molecular Science
- Tencent Foundation through the XPLORER PRIZE
- OSSO state key lab
- BoyaPostdoctoral Fellowship of Peking University
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Isomerization of paraffins remains a challenge, but mesoporous tungsten-zirconia supported Pt catalysts showed improved initial productivity. Close proximity between Pt and WOx species plays a significant role in isomerization, while acid density and metallicity affect the triggering of isomerization and activation of C-H bonds.
Processes for the isomerization of light alkanes have been commercialized; however, the isomerization of paraffins (CnH2n+2, n >= 7) remains a challenge. On mesoporous tungsten-zirconia catalyst supported Pt catalysts (Pt/WZrOx), initial isomerization productivity of 5249 mol(i-C7)/mol(Pt)/h was obtained for n-heptane reforming at 275 degrees C and 5 bar of hydrogen. The catalyst possessed quasi-monolayer and uniformly distributed WOx clusters ( diameter of similar to 0.5 nm), and Pt nanoparticles were preferentially deposited in close vicinity to these WOx sub-nanometer monolayers. The initial productivity over the best Pt/WZrOx catalyst was 18 times higher than that of a corresponding physical mixture (0.8 wt % Pt/ZrO2 + WZrOx), highlighting the significance of intimacy between the Pt and WOx species. The isomerization could not be triggered until the acid density of the catalysts reached a threshold because of the necessity of close proximity between adequate acid sites and adjacent Pt metal sites. Meanwhile, the adjacency increased the metallicity of the supported Pt; thus, enabling easier activation of C-H bonds of C7H16. [GRAPHICS] .
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