NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the mic...NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature（80 ℃） impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups（such as-OH and-C0NH-） to the surface of g-C3N4.Then,the Ni^2＋ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2＋ ions upon the addition of Ni（NO3）2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate（116.343 μmol h^-1 g^-1）,which is significantly higher than that of the pure g-C3N4（3 μmol h^-1 g^-1）.Moreover,the results of a recycling test for the NiS2/g-C3N4（3 wt%）sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.展开更多
Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid i...Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid interfacial charge transfer. However,the present preparation methods usually include complicated and multistep procedures,which can cause damage to the hollow nanostructures. In this paper,a facile template-induced synthesis,based on a template-directed deposition and in situ template-sacrificial dissolution,was employed to prepare Ag-modified TiO 2（Ag/TiO 2） hollow octahedra using Ag2 O octahedra as templates and TiF 4 as the precursor. In the synthetic strategy,the shells of TiO 2 hollow octahedra were formed by coating TiO 2 nanoparticles on the surface of Ag2 O templates based on the template-directed deposition. Simultaneously,the Ag2 O templates can be in situ removed by dissolving the Ag2 O octahedral template in HF solution produced via the hydrolysis reaction of TiF 4 in the reaction system. In addition,Ag nanoparticles were deposited on the inside and outside surfaces of TiO 2 shells by effectively using the photosensitive properties of Ag2 O and Ag＋ ions under light irradiation,along with the formation of TiO 2 hollow octahedra. The Ag/TiO 2 hollow octahedra exhibited high photocatalytic activity because of their（1） short diffusion distances between photogenerated electrons and holes because of the thin shells of Ag/TiO 2 hollow octahedral,（2） deposition of Ag nanoparticles on the inside and outside surfaces of TiO 2 shells,and（3） rapid interfacial charge transfer between TiO 2 shells and Ag nanoparticles. This work may also provide new insights into preparing other Ag-modified and hollow nanostructured photocatalysts.展开更多
基金supported by the National Natural Science Foundation of China (21277107, 21477094, 51672203, 51472192)the Program for New Century Excellent Talents in University (NCET-13-0944)the Fundamental Research Funds for the Central Universities (WUT 2015IB002)~~
文摘NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature（80 ℃） impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups（such as-OH and-C0NH-） to the surface of g-C3N4.Then,the Ni^2＋ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2＋ ions upon the addition of Ni（NO3）2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate（116.343 μmol h^-1 g^-1）,which is significantly higher than that of the pure g-C3N4（3 μmol h^-1 g^-1）.Moreover,the results of a recycling test for the NiS2/g-C3N4（3 wt%）sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.
文摘通过对混凝土拌合物工作性能、浆体黏度与含气量、硬化试件表面气孔分布与外观色泽研究,探讨了机制砂中石粉含量对混凝土外观质量的影响规律。同时,通过SEM观测了硬化试件28 d龄期时的水化产物形貌特征。试验表明:石粉含量低于5%时,试件表面气孔较多,局部有色差。石粉含量不超过10%时,浆体旋转黏度值在2 000 M Pa·s以内,含气量小于2.0%,浆体黏度适中,工作性能好,试件表面色泽均匀、气孔少,能达到清水混凝土外观效果。石粉含量超过15%后,混凝土较黏稠,流动性差,试件表面易出现麻面、气孔等缺陷。适量石粉可增加混凝土微结构的致密性,细化CH晶粒,提高混凝土的力学性能和耐久性能。
基金supported by the National Natural Science Foundation of China(5120839621277107+5 种基金21477094and 51472192)the Program for New Century Excellent Talents in University(NCET-13-0944)the Fundamental Research Funds for the Central Universities(WUT 2014-1a-0032014-VII-037and 2015IB002)~~
文摘Noble metal/titania hollow nanomaterials usually exhibit excellent photocatalytic activity because of their high specific surface area,low density,good surface permeability,strong light-harvesting capacity,and rapid interfacial charge transfer. However,the present preparation methods usually include complicated and multistep procedures,which can cause damage to the hollow nanostructures. In this paper,a facile template-induced synthesis,based on a template-directed deposition and in situ template-sacrificial dissolution,was employed to prepare Ag-modified TiO 2（Ag/TiO 2） hollow octahedra using Ag2 O octahedra as templates and TiF 4 as the precursor. In the synthetic strategy,the shells of TiO 2 hollow octahedra were formed by coating TiO 2 nanoparticles on the surface of Ag2 O templates based on the template-directed deposition. Simultaneously,the Ag2 O templates can be in situ removed by dissolving the Ag2 O octahedral template in HF solution produced via the hydrolysis reaction of TiF 4 in the reaction system. In addition,Ag nanoparticles were deposited on the inside and outside surfaces of TiO 2 shells by effectively using the photosensitive properties of Ag2 O and Ag＋ ions under light irradiation,along with the formation of TiO 2 hollow octahedra. The Ag/TiO 2 hollow octahedra exhibited high photocatalytic activity because of their（1） short diffusion distances between photogenerated electrons and holes because of the thin shells of Ag/TiO 2 hollow octahedral,（2） deposition of Ag nanoparticles on the inside and outside surfaces of TiO 2 shells,and（3） rapid interfacial charge transfer between TiO 2 shells and Ag nanoparticles. This work may also provide new insights into preparing other Ag-modified and hollow nanostructured photocatalysts.
