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200 1 _aRational design of cobalt catalysts embedded in N-Doped carbon for the alcohol dehydrogenation to carboxylic acids
_fCheng Chen, Hang Jing, Zhi-Qin Wang [et al.]
203 _aText
_celectronic
300 _aTitle screen
320 _a[References.: 87 tit.]
330 _aIn this work, a series of Co catalysts (namely Co@NC) was designed and developed from the thermal treatment of ZIF-67. Through extensive screening of various parameters, Co@NC700-H2/Ar exhibited the best catalytic performance in the acceptorless alcohol dehydrogenation to carboxylic acids. It was worth noting that Co@NC700-H2/Ar enabled the efficient synthesis of various aromatic and aliphatic carboxylic acids in moderate to high yields. Besides, it was recyclable for 9 consecutive cycles without activity decay. Moreover, the effects of pyrolysis conditions on the catalytic performance of the resulting materials were thoroughly examined, and the rationale for the superiority of Co@NC700-H2/Ar over the other prepared materials was also provided. Specifically, the pyrolysis atmosphere applying 95% of Ar gas and 5% of H2 gas (H2/Ar) resulted in the generation of ideal porosity and carbon nanotubes (CNTs), while utilizing 700 °C as the optimized pyrolysis temperature was ascribed to the comprehensive evaluation of materials crystallinity and defective structures. Furthermore, additional insights were gained by systematically exploring the oxidation states of Co in different catalysts. It was proposed that the Co–N species played a crucial role in this catalysis, while the contribution of other Co species, including Co0 and Co–O, could not be neglected. Finally, a plausible reaction mechanism was proposed based on the above observations and related literature reports.
333 _aРежим доступа: по договору с организацией-держателем ресурса
461 _tMolecular Catalysis
463 _tVol. 535
_v[112891, 12 p.]
_d2023
610 1 _aэлектронный ресурс
610 1 _aтруды учёных ТПУ
701 0 _aCheng Chen
701 0 _aHang Jing
701 0 _aZhi-Qin Wang
701 0 _aZheng Zhong-Hui
701 0 _aGu Jun-Fei
701 0 _aWei Sang
701 0 _aYuan Ye
701 0 _aChaemchuen Somboon
701 1 _aVerpoort
_bF. V. K.
_cChemical Engineer
_cProfessor of Tomsk Polytechnic University, doctor of chemical Sciences
_f1963-
_gFrensis Valter Kornelius
_2stltpush
_3(RuTPU)RU\TPU\pers\35059
712 0 2 _aНациональный исследовательский Томский политехнический университет
_bИсследовательская школа химических и биомедицинских технологий
_c(2017- )
_h8120
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856 4 _uhttps://doi.org/10.1016/j.mcat.2022.112891
942 _cCF