Citation: Hao Wang, Xiaohao Liu, Guangyue Xu, Ziwei Guo, Ying Zhang. In situ synthesis of Fe-N-C catalysts from cellulose for hydrogenation of nitrobenzene to aniline[J]. Chinese Journal of Catalysis, ;2019, 40(10): 1557-1565. doi: S1872-2067(19)63416-9 shu

In situ synthesis of Fe-N-C catalysts from cellulose for hydrogenation of nitrobenzene to aniline

Hao Wang ^a, ,
Xiaohao Liu ^a ,
Guangyue Xu ^a ,
Ziwei Guo ^a ,
Ying Zhang ^a,b

a Department of Chemistry, University of Science and Technology of China, Hefei 230026, Anhui, China;
b Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

Received Date: 28 April 2019
Revised Date: 27 May 2019

Fund Project: This work was supported by the National Natural Science Foundation of China (51876200, 21572213), and the DNL Cooperation Fund, CAS (DNL180301).

Owing to Fe being the most abundant and least expensive transition metal on the earth, the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention. In this work, a series of N-doped C supported Fe catalysts (Fe-N-C) were prepared by co-pyrolysis of cellulose and ferric chloride under ammonia atmosphere. Characterization methods such as elemental analysis, atomic absorption spectroscopy, nitrogen adsorption-desorption isotherms, transmission electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were carried out to explore the physicochemical properties of the catalysts. Using hydrogenation of nitrobenzene as a model reaction, the catalysts prepared at different pyrolysis temperatures displayed different activities. Fe-N-C-700 exhibited the best activity among these catalysts, with the yield of aniline being up to 98.0% under 5 MPa H₂ at 120℃ after 12 h. Combined with the results of catalyst characterization and comparative tests, the transformation of Fe species and the generation of N-doped C, especially graphitized N-doped C, in the catalyst may be the main factors affecting the activity. A kinetic study was carried out and the apparent activation energy was obtained as 31.53 kJ/mol. The stability of the catalyst was also tested and no significant decrease in the activity was observed after 5 runs.
- Co-pyrolysis,
- Iron,
- Nitrogen-doped,
- Carbon,
- Hydrogenation
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