Citation: Zhou Ren, Yuan Lyu, Siquan Feng, Xiangen Song, Yunjie Ding. Acid-promoted Ir-La-S/AC-catalyzed methanol carbonylation on single atomic active sites[J]. Chinese Journal of Catalysis, ;2018, 39(6): 1060-1069. doi: 10.1016/S1872-2067(18)63019-0 shu

Acid-promoted Ir-La-S/AC-catalyzed methanol carbonylation on single atomic active sites

Zhou Ren ^a,c, ,
Yuan Lyu ^a ,
Siquan Feng ^a,c ,
Xiangen Song ^a ,
Yunjie Ding ^a,b

a Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b State Key Laboratory of catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c University of Chinese Academy of Sciences, Beijing 100049, China

Received Date: 19 January 2018
Revised Date: 2 March 2018

Fund Project: This work was supported by the National Key R&D Program of China (2017YFB0602203).

Highly active Ir-La-S/AC catalyst was successfully prepared by co-impregnation of an activated carbon (AC) carrier with a sulfuric acid solution of Ir and La species and compared with a traditionally prepared Ir-La/AC catalyst. High angle annular dark-field-scanning transmission electron microscopy (HAADF-STEM) measurement results show that most of the Ir species on Ir-La-S/AC exist as single atomic sites, while those on Ir-La/AC exist as nanoparticles with an average diameter of 1.5 nm. Evaluation of Ir-La-S/AC as a catalyst for heterogeneous carbonylation of methanol to acetyl gave a maximum TOF (turn-over-frequency) of 2760 h^-1, which was distinctly higher than that achieved by the Ir-La/AC catalyst (approximately 1000 h^-1). Temperature-programmed desorption of ammonia (NH₃-TPD) result shows that the addition of sulfuric acid during the preparation procedure results in significantly more acidic sites on Ir-La-S/AC than those on Ir-La/AC, which plays a key role in the enhancement of CO insertion as the rate-determining step. Temperature-programmed reduction (TPR) and in situ X-ray photoelectron spectroscopy reveal that Ir species are more reducible, and that more Ir⁺ might be formed by activation of Ir-La-S/AC than those on the Ir-La/AC catalyst, which is thought to be beneficial for reductive elimination of AcI from Ir³⁺ species as an essential step for CH₃I regeneration and acetyl formation.
- Heterogeneous methanol carbonylation,
- Ir-La-S/AC catalyst,
- Bifunctional catalyst,
- Single-atomic active site,
- Co-impregnation
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