Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2)...Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2) solar reduction due to its excellent visible light response,suitable conduction band position,and good cost-effectiveness.However,the amorphous nature and low conductivity of PCN limit its photocatalytic efficiency by leading to low carrier concentrations and facile electron–hole recombination during photocatalysis.Addressing this bottleneck,in this study,potassium-doped PCN(KPCN)/copper(Ⅱ)-complexed bipyridine hydroxyquinoline carboxylic acid(Cu(Ⅱ)(bpy)(H_(2)hqc))composite catalysts were synthesized through a multistep microwave heating process.In the composite,the formation of an S-scheme junction facilitates the enrichment of more negative electrons on the conduction band of KPCN via intermolecular electron–hole recombination between Cu(Ⅱ)(bpy)(H_(2)hqc)(CuPyQc)and KPCN,thereby promoting efficient photoreduction of CO_(2) to CO.Microwave heating enhances the amidation reaction between these two components,achieving the immobilization of homogeneous molecular catalysts and forming amidation chemical bonds that serve as key channels for the S-scheme charge transfer.This work not only presents a new PCN-based catalytic system for CO_(2) reduction applications,but also offers a novel microwave-practical approach for immobilizing homogeneous catalysts.展开更多
Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photo...Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.展开更多
Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine...Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) evolution.The multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through H-bonds.In addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme heterojunction.The optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1)·h^(-1),which is 2.69 and 1.23 times higher than that of CN and OCN,respectively.This work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.展开更多
Artificial photosynthesis is deemed as an efficient protocol for transforming abundant solar energy into valuable fuel. In this paper, the well-defined one-dimensional(1D) core–shell MnO_(2)@CdS hybrids were construc...Artificial photosynthesis is deemed as an efficient protocol for transforming abundant solar energy into valuable fuel. In this paper, the well-defined one-dimensional(1D) core–shell MnO_(2)@CdS hybrids were constructed by employing MnO_(2) nanotubes and CdS nanoparticles as nano-building blocks via a chemical coprecipitation route. The rationally designed core–shell structure provided an intimate heterojunction interface between the CdS shell and MnO_(2) core. All the MnO_(2)@CdS core–shell nanocomposites possess higher H_(2) evolution rate through visible light irradiation contrary to pristine CdS, and the optimal MnO_(2)@CdS hybrid exhibits the utmost H_(2) evolution rate of 3.94 mmol·g^(-1)·h^(-1), which is2.8-fold higher compared with that of CdS. Appertaining to XPS and Mott-Schottky(M-S) analysis, such enhanced photocatalytic H_(2) generation of MnO_(2)@CdS heterojunction was ascribed to an S-scheme mechanism, which suppressed the charge recombination along with a fast detachment of electron–hole pairs(e^(-)–h^(+)) and significantly improved the severance of carriers, thus improved H_(2) evolution performance. These findings envision a new insight into the development of S-scheme heterostructure for photocatalytic H_(2) generation.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22106105 and 22201180)the Innovation Program of Shanghai Municipal Education Commission(No.2019-01-07-00-E00015)+2 种基金Shanghai Science and Technology Innovation Program(No.21DZ1206300)the Central Local Science and Technology Development Guidance Fund(No.YDZX20213100003002)Shanghai Science and Technology Commission Program(No.20060502200).
文摘Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2) solar reduction due to its excellent visible light response,suitable conduction band position,and good cost-effectiveness.However,the amorphous nature and low conductivity of PCN limit its photocatalytic efficiency by leading to low carrier concentrations and facile electron–hole recombination during photocatalysis.Addressing this bottleneck,in this study,potassium-doped PCN(KPCN)/copper(Ⅱ)-complexed bipyridine hydroxyquinoline carboxylic acid(Cu(Ⅱ)(bpy)(H_(2)hqc))composite catalysts were synthesized through a multistep microwave heating process.In the composite,the formation of an S-scheme junction facilitates the enrichment of more negative electrons on the conduction band of KPCN via intermolecular electron–hole recombination between Cu(Ⅱ)(bpy)(H_(2)hqc)(CuPyQc)and KPCN,thereby promoting efficient photoreduction of CO_(2) to CO.Microwave heating enhances the amidation reaction between these two components,achieving the immobilization of homogeneous molecular catalysts and forming amidation chemical bonds that serve as key channels for the S-scheme charge transfer.This work not only presents a new PCN-based catalytic system for CO_(2) reduction applications,but also offers a novel microwave-practical approach for immobilizing homogeneous catalysts.
基金financially supported by the National Natural Science Foundation of China(No.51302061)Natural Science Foundation of Hebei Province(No.E2020201021 and E2023201019)+4 种基金Industry-University-Research Cooperation Major Projects of Shijiazhuang(No.241130477A)Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(No.hxkytd2102)Industry-University-research Cooperation Project of Colleges and Universities in Hebei Province(No.CXZX2025016)Hebei Province Innovation Capability Enhancement Plan Project(No.22567620H)Bintuan Science and Technology Program(Nos.2020DB002 and 2022DB009)。
文摘Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.
基金financially supported by the National Natural Science Foundation of China (Nos.21906072, 21906039, 21908115 and 22006057)Hebei Province 333 Talents Project (No.A202101020)+3 种基金the Science and Technology Project of Hebei Education Department (No.BJ2021010)the Graduate Student Innovation Ability Training Funding Project of Hebei Province (No.CXZZSS2023129)the Open Fund for Hebei Province Key Laboratory of Sustained Utilization & Development of Water Recourse (No.HSZYL2022002)Instrumental Analysis Center, Jiangsu University of Science and Technology。
文摘Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific research.Herein,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) evolution.The multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through H-bonds.In addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme heterojunction.The optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1)·h^(-1),which is 2.69 and 1.23 times higher than that of CN and OCN,respectively.This work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.
基金financially supported by the National Natural Science Foundation of China(Nos.51672113,21975110 and 21972058)。
文摘Artificial photosynthesis is deemed as an efficient protocol for transforming abundant solar energy into valuable fuel. In this paper, the well-defined one-dimensional(1D) core–shell MnO_(2)@CdS hybrids were constructed by employing MnO_(2) nanotubes and CdS nanoparticles as nano-building blocks via a chemical coprecipitation route. The rationally designed core–shell structure provided an intimate heterojunction interface between the CdS shell and MnO_(2) core. All the MnO_(2)@CdS core–shell nanocomposites possess higher H_(2) evolution rate through visible light irradiation contrary to pristine CdS, and the optimal MnO_(2)@CdS hybrid exhibits the utmost H_(2) evolution rate of 3.94 mmol·g^(-1)·h^(-1), which is2.8-fold higher compared with that of CdS. Appertaining to XPS and Mott-Schottky(M-S) analysis, such enhanced photocatalytic H_(2) generation of MnO_(2)@CdS heterojunction was ascribed to an S-scheme mechanism, which suppressed the charge recombination along with a fast detachment of electron–hole pairs(e^(-)–h^(+)) and significantly improved the severance of carriers, thus improved H_(2) evolution performance. These findings envision a new insight into the development of S-scheme heterostructure for photocatalytic H_(2) generation.
