Synthesizing large-area ultrathin two-dimensional(2D)nanostructures in aqueous media has received considerable increasing attention but remains a big challenge.Herein,we report a facile method for the synthesis of two...Synthesizing large-area ultrathin two-dimensional(2D)nanostructures in aqueous media has received considerable increasing attention but remains a big challenge.Herein,we report a facile method for the synthesis of two unprecedented large-area ultrathin 2D supramolecular nanosheets via ionic self-assembly in water.Upon consideration of electrostatic interaction and repulsive effect,deprotonated tetrakis(4-carboxyphenyl)porphyrin(TCPP)or Fe(III)tetra(4-carboxyphenyl)porphine chloride(TCPP(Fe))as connection vertex and protonated bis(2-dimethylaminoethyl)ether(BDMAEE)unit as bridging edge connect with each other to form few-layer 2D nanosheet with a thickness of^1.8–1.9 nm,while the lateral size can close to one hundred micrometers.Moreover,the well-dispersed 2D TCPP(Fe)-BDMAEE with heme-like active center displays intrinsic peroxidase-like catalytic activity,which can be used to detect hydrogen peroxide.The present facile strategy highlights new opportunities in constructing large-area ultrathin 2D supramolecular nanomaterials and paves the avenue to expand their potential applications.展开更多
Graphitic carbon nitride(g-C3N4,CN)has attracted increasing interests in the field of photocatalysis due to its high visible-light-response.However,its photocatalytic activity is still lower for degradation of refract...Graphitic carbon nitride(g-C3N4,CN)has attracted increasing interests in the field of photocatalysis due to its high visible-light-response.However,its photocatalytic activity is still lower for degradation of refractory contaminants such as Cr(Ⅵ)and Rhodamine B(RhB)etc.Herein,we report a facile method to synthesize a novel sulfur(S)-doped CN/reduced graphene oxide(rGO)porous nanosheet(S-CN/rGO PNs)via a supramolecular self-assembling followed by a solvothermal treatment.The as-prepared porous SCN/rGO PNs are stable with high specific surface area^188.5 m2 g-1 and exhibit a significantly enhanced photocatalytic activity of^17-fold and 15-fold higher than that of bulk CN for the degradation of RhB and Cr(Ⅵ)under visible light irradiation,respectively.Typically,50 mL of 15 mg/mL RhB can be degraded within 20 min by 10 mg S-CN/rGO PNs.The mechanism can be explained by the synergistic effect of S doping and porous structure which can effectively reduce the band gap of CN and increase the specific surface area to promote the separation and transfer of photo-generated charge carriers.The results have provided a new way to significantly enhance the photocatalytic activity of g-C3N4 for degradation of refractory contaminants.展开更多
基金support from the National Natural Science Foundation of China(NSFC)(No.51733003).
文摘Synthesizing large-area ultrathin two-dimensional(2D)nanostructures in aqueous media has received considerable increasing attention but remains a big challenge.Herein,we report a facile method for the synthesis of two unprecedented large-area ultrathin 2D supramolecular nanosheets via ionic self-assembly in water.Upon consideration of electrostatic interaction and repulsive effect,deprotonated tetrakis(4-carboxyphenyl)porphyrin(TCPP)or Fe(III)tetra(4-carboxyphenyl)porphine chloride(TCPP(Fe))as connection vertex and protonated bis(2-dimethylaminoethyl)ether(BDMAEE)unit as bridging edge connect with each other to form few-layer 2D nanosheet with a thickness of^1.8–1.9 nm,while the lateral size can close to one hundred micrometers.Moreover,the well-dispersed 2D TCPP(Fe)-BDMAEE with heme-like active center displays intrinsic peroxidase-like catalytic activity,which can be used to detect hydrogen peroxide.The present facile strategy highlights new opportunities in constructing large-area ultrathin 2D supramolecular nanomaterials and paves the avenue to expand their potential applications.
基金the Science and Technology Major Project of Shanxi Province(Grant Numbers MC2016-06)National Natural Science Foundation of China(21173041)the Opening Project of Jiangsu Key Laboratory of Advanced Metallic Materials,China.
文摘Graphitic carbon nitride(g-C3N4,CN)has attracted increasing interests in the field of photocatalysis due to its high visible-light-response.However,its photocatalytic activity is still lower for degradation of refractory contaminants such as Cr(Ⅵ)and Rhodamine B(RhB)etc.Herein,we report a facile method to synthesize a novel sulfur(S)-doped CN/reduced graphene oxide(rGO)porous nanosheet(S-CN/rGO PNs)via a supramolecular self-assembling followed by a solvothermal treatment.The as-prepared porous SCN/rGO PNs are stable with high specific surface area^188.5 m2 g-1 and exhibit a significantly enhanced photocatalytic activity of^17-fold and 15-fold higher than that of bulk CN for the degradation of RhB and Cr(Ⅵ)under visible light irradiation,respectively.Typically,50 mL of 15 mg/mL RhB can be degraded within 20 min by 10 mg S-CN/rGO PNs.The mechanism can be explained by the synergistic effect of S doping and porous structure which can effectively reduce the band gap of CN and increase the specific surface area to promote the separation and transfer of photo-generated charge carriers.The results have provided a new way to significantly enhance the photocatalytic activity of g-C3N4 for degradation of refractory contaminants.