4.7 Article

Mineral-modulated Co catalyst with enhanced adsorption and dissociation of BH4- for hydrogenation of p-nitrophenol to p-aminophenol

Journal

CHEMOSPHERE
Volume 291, Issue -, Pages -

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2021.132871

Keywords

Mineral material; Hydrogenation; p-nitrophenol; Magnetic separation; Electron transfer mechanism

Funding

  1. National Natural Science Foundation of China [51674293]
  2. Fundamental Research Funds for the Central Universities of Central South University [1053320183883]
  3. Opening Project of Engineering Research Center of Nano-Geo Materials of Ministry of Education of China Uni-versity of Geosciences [NGM2020KF001]

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By using a mineral-modulated catalyst, the hydrogenation reduction process of p-nitrophenol was facilitated, leading to fast reaction rate and high conversion. The designed Co/EAtp@C catalyst showed good electron transfer mechanism and stability, as well as magnetic separability.
Slow adsorption and dissociation kinetics of NaBH4 onto the catalyst surface limit the hydrogenation reduction of hazardous p-nitrophenol to worthy p-aminophenol. Herein, we design a mineral-modulated catalyst to facilitate the rate-limiting step. Carbon-coated etched attapulgite (EAtp@C) is obtained by HF treatment. Co/EAtp@C is fabricated via anchoring cobalt nanoparticles (CoNPs) on the carrier EAtp@C. Compared to pure Co, the anchored CoNPs are more electronegative and stable, which provides abundant and stable active sites and ac-celerates the BH4- adsorption and dissociation. Therefore, Co/EAtp@C leads to nearly 100% reduction of p-nitrophenol to p-aminophenol within 8 min and its apparent rate constant Kapp (0.69 min(-1)) is 4 times higher than that of pure Co. Thermodynamic calculations show a lower activation energy (37.92 kJ mol(-1)) of Co/ EAtp@C catalyst than that of pure Co. Co/EAtp@C also shows magnetic separability and good stability by remaining 98.6% of catalytic conversion rate after six cycles. Significantly, we detect the active species Co-H, and reveal the electron transfer mechanism between catalysts, BH4-, and p-nitrophenol by electrochemical method. These results offer a fundamental insight into the catalytic mechanism of p-nitrophenol hydrogenation for rational design of efficient catalysts.

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