A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loa...A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI,but also can significantly promote the catalytic performance.By employing NHPI/h-BN as the catalyst,azodiisobutyronitrile(AIBN)as the metal-free initiator,a 95%conversion of dibenzothiophene(DBT)can be acquired under the reaction conditions of 120°C and atmospheric pressure with molecular oxygen(O_(2))as oxidant.Moreover,the heterogenization is convenient for the regeneration of the catalyst with>94%DBT conversion after being recycled seven times.Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN.The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical(O_(2)^(·-)),which oxidize DBT to DBTO2 for desulfurization.展开更多
A series of basic nitrogen doped carbon hollow spheres(p-N-C) catalysts derived from waste tires were prepared by a green, facile and environmental “leavening” strategy for the catalytic oxidation of pentanethiol. C...A series of basic nitrogen doped carbon hollow spheres(p-N-C) catalysts derived from waste tires were prepared by a green, facile and environmental “leavening” strategy for the catalytic oxidation of pentanethiol. Compared to pristine carbon, the p-N-C has a higher surface curvature conducive to the enrichment of substrates, leading to an excellent catalytic performance. This increased surface curvature of p-N-C was fabricated on the synergistic effect of two foaming agents((NH4)2 C2 O4 and NaHCO3), and the released gas also endows the spherical shell of p-N-C with a hierarchical porous structure, promoting the accessibility of active sites with pentanethiol. Pyridine-like and pyrrolic-like nitrogen atoms were investigated as reactive sites on the p-N-C to accelerate the electron transfer from sulfur to active surface oxygen and enhance the adsorption/oxidation process. As a result, the optimal p-N-C catalyst exhibits superior adsorption and oxidation performance(99.9%) of pentanethiol, outperforming the “unleavened”catalyst(20.8%). This work offers a new avenue for the fabrication of highly efficient materials for the desulfurization of fuel.展开更多
The development of high-efficient adsorbents for the treatment of antibiotics from contaminated water has been of great concern.This work introduced an alcohol-solvent mediated strategy to increase the specific surfac...The development of high-efficient adsorbents for the treatment of antibiotics from contaminated water has been of great concern.This work introduced an alcohol-solvent mediated strategy to increase the specific surface area(SSA)and porosity of hexagonal boron nitride nanosheets(BNNSs)for improving tetracycline(TC)removal efficiency.The BNNSs synthesized with the mediation of n-propanol solvent(BN-P)exhibited the largest pore volume and relatively high SSA(increased by 34%and 64%,respectively,compared with that synthesized under the mediation of water)in its structure,which in turn facilitated the mass transfer of TC molecules onto BN-P framework.The remarkable adsorption performance of BN-P,with 20%increase in equilibrium adsorption capacity and Langmuir maximum adsorption capacity of 556 mg·g^(-1),was achieved for capturing TC within just 3 h,which is mainly through p-p interaction and electrostatic force.Pseudo-second kinetics equation can well illustrate the adsorption process,while Freundlich and Langmuir isotherm models fitted the equilibrium data well.Thermodynamics study demonstrated a spontaneous exothermal adsorption process.Furthermore,the strong environmental suitability and notable recycling performance of BN-P revealed its good application prospect in removing antibiotic TC from wastewater.展开更多
基金the financial support from the National Key R&D Program of China(No.2017YFB0306504)National Natural Science Foundation of China(No.22008094,22178154 and 21878133)+2 种基金Chinese Postdoctoral Science Foundation(No.2019M651743,2020M671364 and 2020M673039)Natural Science Foundation of Jiangsu Province(No.BK20190852)Natural Science Foundation for Jiangsu Colleges and Universities(No.19KJB530005)
文摘A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI,but also can significantly promote the catalytic performance.By employing NHPI/h-BN as the catalyst,azodiisobutyronitrile(AIBN)as the metal-free initiator,a 95%conversion of dibenzothiophene(DBT)can be acquired under the reaction conditions of 120°C and atmospheric pressure with molecular oxygen(O_(2))as oxidant.Moreover,the heterogenization is convenient for the regeneration of the catalyst with>94%DBT conversion after being recycled seven times.Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN.The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical(O_(2)^(·-)),which oxidize DBT to DBTO2 for desulfurization.
基金financially supported by the National Natural Science Foundation of China (Nos. 21722604, 21878133, and22002050)China Postdoctoral Science Foundation (No.2020M671365)Postgraduate Research&Practice Innovation Program of Jiangsu Province (No. KYCX20_3039)。
文摘A series of basic nitrogen doped carbon hollow spheres(p-N-C) catalysts derived from waste tires were prepared by a green, facile and environmental “leavening” strategy for the catalytic oxidation of pentanethiol. Compared to pristine carbon, the p-N-C has a higher surface curvature conducive to the enrichment of substrates, leading to an excellent catalytic performance. This increased surface curvature of p-N-C was fabricated on the synergistic effect of two foaming agents((NH4)2 C2 O4 and NaHCO3), and the released gas also endows the spherical shell of p-N-C with a hierarchical porous structure, promoting the accessibility of active sites with pentanethiol. Pyridine-like and pyrrolic-like nitrogen atoms were investigated as reactive sites on the p-N-C to accelerate the electron transfer from sulfur to active surface oxygen and enhance the adsorption/oxidation process. As a result, the optimal p-N-C catalyst exhibits superior adsorption and oxidation performance(99.9%) of pentanethiol, outperforming the “unleavened”catalyst(20.8%). This work offers a new avenue for the fabrication of highly efficient materials for the desulfurization of fuel.
基金This work was financially supported by Hainan Natural Science Foundation Innovation Research Team project(No.220CXTD436)the National Natural Science Foundation of China(No.21766007,21878133).
文摘The development of high-efficient adsorbents for the treatment of antibiotics from contaminated water has been of great concern.This work introduced an alcohol-solvent mediated strategy to increase the specific surface area(SSA)and porosity of hexagonal boron nitride nanosheets(BNNSs)for improving tetracycline(TC)removal efficiency.The BNNSs synthesized with the mediation of n-propanol solvent(BN-P)exhibited the largest pore volume and relatively high SSA(increased by 34%and 64%,respectively,compared with that synthesized under the mediation of water)in its structure,which in turn facilitated the mass transfer of TC molecules onto BN-P framework.The remarkable adsorption performance of BN-P,with 20%increase in equilibrium adsorption capacity and Langmuir maximum adsorption capacity of 556 mg·g^(-1),was achieved for capturing TC within just 3 h,which is mainly through p-p interaction and electrostatic force.Pseudo-second kinetics equation can well illustrate the adsorption process,while Freundlich and Langmuir isotherm models fitted the equilibrium data well.Thermodynamics study demonstrated a spontaneous exothermal adsorption process.Furthermore,the strong environmental suitability and notable recycling performance of BN-P revealed its good application prospect in removing antibiotic TC from wastewater.