A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nan...A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nanoparticles on the surface of sheet cobalt-based metal-organic framework(Co-MOF)and graphitic carbon nitride(g-C_(3)N_(4),CN).The structure and properties of the obtained catalysts were systematically analyzed.NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region.The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254μmol/(g·h)at pH=9.At the same time,NSCQDs synergy Co-MOF/CN composites have good stability.After four cycles of hydrogen production,the performance remains relatively stable.The tran sient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts.The semiconductor type(n-type semico nductor)of the single-phase catalyst was determined by the Mott-Schottky test,and the band structure was analyzed.The conductive and valence bands of CN are-0.99 and 1.72 eV,respectively,and the conduction and valence bands of Co-MOF are-1.85 and 1.33 eV,respectively.Th e mechanism of the photocatalytic reaction can be inferred,that is,Z-type heterojunction is formed between CN an d Co-MOF,and NSCQDs was used as cocatalyst.展开更多
Nanozyme antibacterial agents with high enzyme-like catalytic activity and strong bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism.Herein,the carbon n...Nanozyme antibacterial agents with high enzyme-like catalytic activity and strong bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism.Herein,the carbon nitride quantum dots(CNQDs)nanozymes with high nitrogen vacancies(NVs)were mass-productively prepared by a simple ultrasonic-crushing method assisted by propylene glycol.It was found that the NVs of CNQDs were stemmed from the selective breaking of surface N-(C)_(2)sites,accounting for 6.2%.Experiments and density functional theory(DFT)simulations have demonstrated that the presence of NVs can alter the local electron distribution and extend theπ-electron delocalization to enhance the peroxidase-like activity.Biocompatible CNQDs could enter inside microorganisms by diffusion and elevate the bacteria-binding ability,which enhanced the accurate and rapid attack of·OH to the microorganisms.The sterilization rate of CNQDs against Gram-negative bacteria(E.coli),Gram-positive bacteria(S.aureus,B.subtilis),fungi(R.solani)reaches more than 99%.Thus,this work showed great potential for engineered nanozymes for broad-spectrum antibacterial in biomedicine and environmental protection.展开更多
Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,w...Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,we prepared two kinds of CDs with solvatochromic emissions:green emission CDs(G-CDs)and multicolor emission CDs(M-CDs).G-CDs synthesized from o-phenylenediamine exhibited weak photoluminescence emission(quantum yield 2.8%-6.1%)and 39 nm solvatochromic shifts(492-531 nm).In contrast,M-CDs prepared from o-phenylenediamine and 4-aminophenol showed 87 nm solvatochromic shift range(505-592 nm)and much higher photoluminescence quantum yield(18.4%-32.5%).The two CDs exhibited different emission,absorption,and photoluminescence lifetime.The origin of solvatochromic shifts and the formation mechanism of CDs were demonstrated by analyzing the structures and compositions of two CDs.High percentages of pyrrolic nitrogen and amino nitrogen make wider solvatochromic shifts and higher quantum yields.The results were well supported by density functional theory calculations.This effective strategy to expand solvatochromic shift range and improve quantum yields could open a new window to prepare satisfied solvatochromic carbon dots.展开更多
A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W...A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W Xe lamp light(with optical filter,λ≥420nm),the performanceof N‐CQDs/Ag2CO3in photocatalytic degradation of phenol was evaluated.The as‐preparedsamples were analyzed by XRD,SEM,TEM,BET,element mapping,UV‐vis DRS,FT‐IR,XPS,transientphotocurrent response and EIS testing.The results showed that after coupling with trace amountsof N‐CQDs,both the photocatalytic activity and stability of Ag2CO3were greatly boosted.The additionof N‐CQDs solution influenced the crystallization of Ag2CO3,resulting in a distinct decrease inAg2CO3crystal size and an obvious increase in surface area.Moreover,the charge transfer resistancewas greatly reduced,and the separation efficiency of photogenerated electrons and holes wasstrongly promoted.The presence of NCQDs on the surface of the catalysts facilitates the transfer ofphotogenerated electrons,slowing the photocorrosion rate of Ag2CO3,and then resulting in higherstability than bare Ag2CO3in degradation.The synergistic effect of the improvement of morphologyand charge transfer rate thus accounted for the superior photocatalytic performance ofN‐CQDs/Ag2CO3.展开更多
基金Project supported by the Ningxia Natural Science Foundation of China(2023AAC03285)National Natural Science Foundation of China(21666001)+1 种基金Innovative Team for Transforming Waste Cooking Oil into Clean Energy and High Value-added Chemicals,ChinaNingxia Low-grade Resource High Value Utilization and Environmental Chemical Integration Technology Innovation Team Project,China。
文摘A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nanoparticles on the surface of sheet cobalt-based metal-organic framework(Co-MOF)and graphitic carbon nitride(g-C_(3)N_(4),CN).The structure and properties of the obtained catalysts were systematically analyzed.NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region.The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254μmol/(g·h)at pH=9.At the same time,NSCQDs synergy Co-MOF/CN composites have good stability.After four cycles of hydrogen production,the performance remains relatively stable.The tran sient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts.The semiconductor type(n-type semico nductor)of the single-phase catalyst was determined by the Mott-Schottky test,and the band structure was analyzed.The conductive and valence bands of CN are-0.99 and 1.72 eV,respectively,and the conduction and valence bands of Co-MOF are-1.85 and 1.33 eV,respectively.Th e mechanism of the photocatalytic reaction can be inferred,that is,Z-type heterojunction is formed between CN an d Co-MOF,and NSCQDs was used as cocatalyst.
基金the National Natural Science Foundation of China(Nos.21876099,22106088,and 22276110)Key Research&Developmental Program of Shandong Province(No.2021CXGC011202)Fundamental Research Funds of Shandong University(No.zy202102).
文摘Nanozyme antibacterial agents with high enzyme-like catalytic activity and strong bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism.Herein,the carbon nitride quantum dots(CNQDs)nanozymes with high nitrogen vacancies(NVs)were mass-productively prepared by a simple ultrasonic-crushing method assisted by propylene glycol.It was found that the NVs of CNQDs were stemmed from the selective breaking of surface N-(C)_(2)sites,accounting for 6.2%.Experiments and density functional theory(DFT)simulations have demonstrated that the presence of NVs can alter the local electron distribution and extend theπ-electron delocalization to enhance the peroxidase-like activity.Biocompatible CNQDs could enter inside microorganisms by diffusion and elevate the bacteria-binding ability,which enhanced the accurate and rapid attack of·OH to the microorganisms.The sterilization rate of CNQDs against Gram-negative bacteria(E.coli),Gram-positive bacteria(S.aureus,B.subtilis),fungi(R.solani)reaches more than 99%.Thus,this work showed great potential for engineered nanozymes for broad-spectrum antibacterial in biomedicine and environmental protection.
基金We appreciate the financial supports from the Board or Regent Supporting Fund(BORSF)Endowed Professorshipthe Lousiana State University Shreveport(LSUS)R&D Funds+1 种基金the Qingdao Municipal Science and Technology Commission(No.16-5-1-86-jch)the Scientific Research Foundation of Qingdao University of Science and Technology(QUST)(No.210/010022914).
文摘Carbon dots(CDs)with solvatochromic emission colors in different solvents have attracted much attention as a new class of luminescent nanomaterial owing to their facile synthesis and low production cost.In this work,we prepared two kinds of CDs with solvatochromic emissions:green emission CDs(G-CDs)and multicolor emission CDs(M-CDs).G-CDs synthesized from o-phenylenediamine exhibited weak photoluminescence emission(quantum yield 2.8%-6.1%)and 39 nm solvatochromic shifts(492-531 nm).In contrast,M-CDs prepared from o-phenylenediamine and 4-aminophenol showed 87 nm solvatochromic shift range(505-592 nm)and much higher photoluminescence quantum yield(18.4%-32.5%).The two CDs exhibited different emission,absorption,and photoluminescence lifetime.The origin of solvatochromic shifts and the formation mechanism of CDs were demonstrated by analyzing the structures and compositions of two CDs.High percentages of pyrrolic nitrogen and amino nitrogen make wider solvatochromic shifts and higher quantum yields.The results were well supported by density functional theory calculations.This effective strategy to expand solvatochromic shift range and improve quantum yields could open a new window to prepare satisfied solvatochromic carbon dots.
基金supported by the National Natural Science Foundation of China(21567008,21607064,21707055)Program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology+2 种基金Program of 5511 Talents in Scientific and Technological Innovation of Jiangxi Province(20165BCB18014)Academic and Technical Leaders of the Main Disciplines in Jiangxi Province(20172BCB22018)Jiangxi Province Natural Science Foundation(20161BAB203090)~~
文摘A series of N‐CQDs/Ag2CO3composite crystals(where N‐CQDs=Nitrogen doped carbon quantumdots)were prepared by adding different volumes of a solution of N‐CQDs during Ag2CO3crystalgrowth.Under irradiation from a350‐W Xe lamp light(with optical filter,λ≥420nm),the performanceof N‐CQDs/Ag2CO3in photocatalytic degradation of phenol was evaluated.The as‐preparedsamples were analyzed by XRD,SEM,TEM,BET,element mapping,UV‐vis DRS,FT‐IR,XPS,transientphotocurrent response and EIS testing.The results showed that after coupling with trace amountsof N‐CQDs,both the photocatalytic activity and stability of Ag2CO3were greatly boosted.The additionof N‐CQDs solution influenced the crystallization of Ag2CO3,resulting in a distinct decrease inAg2CO3crystal size and an obvious increase in surface area.Moreover,the charge transfer resistancewas greatly reduced,and the separation efficiency of photogenerated electrons and holes wasstrongly promoted.The presence of NCQDs on the surface of the catalysts facilitates the transfer ofphotogenerated electrons,slowing the photocorrosion rate of Ag2CO3,and then resulting in higherstability than bare Ag2CO3in degradation.The synergistic effect of the improvement of morphologyand charge transfer rate thus accounted for the superior photocatalytic performance ofN‐CQDs/Ag2CO3.
