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It has been widely documented that the oxygen-containing functionalities, especially carboxyl groups, on carbon surfaces play crucial roles in the catalytic wet air oxidation (CWAO) reactions. Herein, the CWAO of phenol with molecular O 2 as terminal oxidant using cylindrical and herringbone carbon nanotubes (CNTs) underwent different treatments as catalysts were conducted in batch mode. It was uncovered that the catalytic function of carboxyl groups strongly depended on the structure of CNTs. Parallel CNTs ( p -CNTs) with cylindrical graphitic walls displayed the highest catalytic activity after nitric acid oxidation, due to the carboxylated carbon debris (CDs) coating on surfaces. For herringbone CNTs ( h- CNTs), carboxyl groups are mostly linked to its sidewalls, where abundant edge carbons were exposed, providing an enhanced CWAO activity. The positively synergistic effect of carboxyl groups and adjacent edge carbons was responsible for the activation of O 2 , leading to the improved CWAO activity. This study provides a new insight into the structural effect of carbon materials on the CWAO of phenol. [ABSTRACT FROM AUTHOR]

Novel nitrogen doped magnetic carbons (NMC), in-situ synthesized through facile pyrolysis-carbonization processes using Fe(NO 3 ) 3 and melamine as precursors, were demonstrated as excellent nanoadsorbents to remove Cr(VI) effectively. The achieved removal capacity in both neutral and acidic solution was 29.4 and 2001.4 mg g −1 respectively, much higher than the reported adsorbents so far. The unprecedented high adsorption performance can be attributed to the incorporation of the nitrogen dopant, which increased the negative charge density on the surface of adsorbent and thereby enhanced the interaction between the adsorbents and Cr(VI) ions. The density functional theory (DFT) calculation demonstrated that the nitrogen dopants can decrease the adsorption energy between the Cr(VI) ions and NMC (−3.456 kJ mol −1 ), lower than the undoped sample (−3.344 kJ mol −1 ), which boosted the adsorption behavior. Chemical rather than physical adsorption was followed for these magnetic nanoadsorbents as revealed from the pseudo-second-order kinetic study. Furthermore, the NMC showed high stability with recycling tests for the Cr(VI) removal. [ABSTRACT FROM AUTHOR]

Abstract: Nitrogen-, phosphorous- and boron-doped carbon nanotubes (N-CNTs, P-CNTs and B-CNTs) were prepared by a chemical vapor deposition method using xylene as carbon source and aniline-NH3, triphenyl phosphine and triethyl borate as nitrogen, phosphorous and boron precursors, respectively. By tailoring the composition of reactants and reaction atmosphere, N-CNTs with nitrogen contents from 0% to 4.36% and P-CNTs with phosphorous contents from 0.55% to 5.14% were synthesized. N- and P-CNTs are active for the oxidation of cyclohexane in the liquid phase with molecular oxygen as oxidant. The highest mass-normalized activity, 761mmolg−1 h−1, was achieved over N-CNTs synthesized from aniline in an NH3 atmosphere, while the highest surface-area-normalized activity, 28mmolm−2 h−1, was observed over P-CNTs. B-doping does not improve the activity of CNTs. The effect of the number of nitrogen functionalities and defects was investigated to reveal the structure–activity relationship of the doped CNTs. By using the work function as an indicator of the electron donation of carbon, an exponential dependence of specific activity on work function was discovered for N- and P-CNTs, suggesting that the electron transfer on the surfaces of CNTs plays a central role in the CNT-catalyzed oxidation of cyclohexane. [Copyright &y& Elsevier]