Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most de...Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.展开更多
Developing efficient,stable,and low-cost novel electron-cocatalysts is crucial for photocatalytic hydrogen evolution reaction.Herein,amorphous Ni-P alloy particles were successfully modified onto g-C3N4 to construct t...Developing efficient,stable,and low-cost novel electron-cocatalysts is crucial for photocatalytic hydrogen evolution reaction.Herein,amorphous Ni-P alloy particles were successfully modified onto g-C3N4 to construct the Ni-P/g-C3N4 photocatalyst through a simple and green triethanolamine(TEOA)-mediated photodeposition method.It was found that the TEOA could serve as an excellent complexing agent to coordinate with Ni2+to form[Ni(TEOA)]^2+complex,which can promote the rapid and effective deposition of amorphous Ni-P alloy on the g-C3N4 surface.Photocatalytic tests suggest that the hydrogen-evolution performance of gC3N4 can be greatly promoted through integrating amorphous Ni-P alloy.Especially,the Ni-P/g-C3N4(5 wt%)exhibits the superior H2-generation activity(118.2μmol h^-1g^-1),which is almost 35.8 times that of bare g-C3N4.Furthermore,the amorphous Ni-P alloy cocatalyst can also serve as the general hydrogen-production cocatalyst to greatly enhance the photocatalytic performance of traditional semiconductor materials such as Ti O2 and Cd S.Based on the present results,the mechanism of the amorphous Ni-P alloy as the high-efficiency electron transfer medium was proposed for the boosted H2-generation rate.The present facile route may broaden the horizons for the efficient development of highly active cocatalysts in photocatalytic field.展开更多
基金supported by the National Natural Science Foundation of China(51672113,51602132)the Six Talent Peaks Project in Jiangsu Province(2015-XCL-026)+2 种基金the Natural Science Foundation of Jiangsu Province(BK20171299)the Training Project of Jiangsu University for Young Cadre Teachers(5521220009)the Youth Research Project of Jiangsu Health and Family Planning Commission in 2016(Q201609)~~
文摘Accelerating the separation efficiency of photoexcited electron-hole pairs with the help of highly active co-catalysts has proven to be a promising approach for improving photocatalytic activity. Thus far, the most developed co-catalysts for semiconductor-based photocatalysis are inorganic materials;the employment of a specific organic molecule as a co-catalyst for photocatalytic hydrogen evolution and pollutant photodegradation is rare and still remains a challenging task. Herein, we report on the use of an organic molecule, oxamide (OA), as a novel co-catalyst to enhance electron- hole separation, photocatalytic H2 evolution, and dye degradation over TiO2 nanosheets. OA-modified TiO2 samples were prepared by a wet chemical route and demonstrated improved light absorption in the visible-light region and more efficient charge transport. The photocatalytic performance of H2 evolution from water splitting and rhodamine B (RhB) degradation for an optimal OA-modified TiO2 photocatalyst reached 2.37 mmol g^–1 h^–1 and 1.43 × 10^-2 min^-1, respectively, which were 2.4 and 3.8 times higher than those of pristine TiO2, respectively. A possible mechanism is proposed, in which the specific π-conjugated structure of OA is suggested to play a key role in the enhancement of the charge transfer and catalytic capability of TiO2. This work may provide advanced insight into the development of a variety of metal-free organic molecules as functional co-catalysts for improved solar-to-fuel conversion and environmental remediation.
基金supported by the National Natural Science Foundation of China(21771142 and 51672203)the Fun-damental Research Funds for the Central Universities(WUT 2019IB002)。
文摘Developing efficient,stable,and low-cost novel electron-cocatalysts is crucial for photocatalytic hydrogen evolution reaction.Herein,amorphous Ni-P alloy particles were successfully modified onto g-C3N4 to construct the Ni-P/g-C3N4 photocatalyst through a simple and green triethanolamine(TEOA)-mediated photodeposition method.It was found that the TEOA could serve as an excellent complexing agent to coordinate with Ni2+to form[Ni(TEOA)]^2+complex,which can promote the rapid and effective deposition of amorphous Ni-P alloy on the g-C3N4 surface.Photocatalytic tests suggest that the hydrogen-evolution performance of gC3N4 can be greatly promoted through integrating amorphous Ni-P alloy.Especially,the Ni-P/g-C3N4(5 wt%)exhibits the superior H2-generation activity(118.2μmol h^-1g^-1),which is almost 35.8 times that of bare g-C3N4.Furthermore,the amorphous Ni-P alloy cocatalyst can also serve as the general hydrogen-production cocatalyst to greatly enhance the photocatalytic performance of traditional semiconductor materials such as Ti O2 and Cd S.Based on the present results,the mechanism of the amorphous Ni-P alloy as the high-efficiency electron transfer medium was proposed for the boosted H2-generation rate.The present facile route may broaden the horizons for the efficient development of highly active cocatalysts in photocatalytic field.
