This study aimed to prepare and apply a novel Pt/CdMoO_(4) composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO_(4) composite was subjected to comprehensive investigation o...This study aimed to prepare and apply a novel Pt/CdMoO_(4) composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO_(4) composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO_(4) surface. Close contact between CdMoO_(4) and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO_(4), resulting in electron drift from CdMoO_(4) to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO_(4) composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO_(4) catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒^(1)·g‒^(1)·h‒^(1), which is 3.2 times higher than that of pure CdMoO_(4). In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.展开更多
In this paper,Cu-doped Bi_(2)WO_(6)was synthesized via a solvothermal method and applied it in photocatalytic N_(2)immobilization.Characterization results showed the presence of a small amount of metallic Bi in the ph...In this paper,Cu-doped Bi_(2)WO_(6)was synthesized via a solvothermal method and applied it in photocatalytic N_(2)immobilization.Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst,indicating that the synthesized photocatalyst is actually Bi/Cu-Bi_(2)WO_(6)composite.The doped Cu had a valence state of+2 and most likely substituted the position of Bi^(3+).The introduced Cu did not affect the metallic Bi content,but mainly influenced the energy band structure of Bi_(2)WO_(6).The band gap was slightly narrowed,the conduction band was elevated,and the work function was reduced.The reduced work function improved the transfer and separation of charge carriers,which mainly caused the increased photoactivity.The optimized NH_(3)generation rates of Bi/Cu-Bi_(2)WO_(6)reached 624 and 243μmol·L^(-1)·g^(-1)·h^(-1)under simulated solar and visible light,and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi_(2)WO_(6),respectively.This research provides a method for improving the photocatalytic N_(2)fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N_(2)-to-NH_(3)conversion.展开更多
Side chain engineering with fluorine substitution is widely used to enhance photovoltaic performance of polymer donors in the research field of polymer solar cells(PSCs).However,fluorine substitution has disadvantages...Side chain engineering with fluorine substitution is widely used to enhance photovoltaic performance of polymer donors in the research field of polymer solar cells(PSCs).However,fluorine substitution has disadvantages of complicated synthesis and high cost.Herein,we synthesized a novel D-A copolymer donor PBQ9 based on difluoroquinoxaline A-unit with chlorine substitution on its alkyl-thiophene side chains instead of fluorine substitution in the polymer donor PBQ6,which greatly shortens the synthetic route and reduces the cost.Interestingly,the optimized binary PSC with PBQ9 as polymer donor and m-TEH as acceptor demonstrated a high power conversion efficiency(PCE)of 18.81%(certified PCE of 18.33%by National Institute of Metrology,China)with a high fill factor of 80.59%,and the photovoltaic performance of the PSCs is insensitive to the different batches of the polymer donor.The results indicate that PBQ9 is a high-performance polymer donor and that chlorine substitution is an effective strategy to improve photovoltaic performance and reduce the cost of polymer donors.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.22172144).
文摘This study aimed to prepare and apply a novel Pt/CdMoO_(4) composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO_(4) composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO_(4) surface. Close contact between CdMoO_(4) and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO_(4), resulting in electron drift from CdMoO_(4) to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO_(4) composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO_(4) catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒^(1)·g‒^(1)·h‒^(1), which is 3.2 times higher than that of pure CdMoO_(4). In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.
基金The work was financially supported by National Natural Science Foundation of China(Grant No.22172144)Natural Science Foundation of Zhejiang Province(Grant No.LY20B030004).
文摘In this paper,Cu-doped Bi_(2)WO_(6)was synthesized via a solvothermal method and applied it in photocatalytic N_(2)immobilization.Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst,indicating that the synthesized photocatalyst is actually Bi/Cu-Bi_(2)WO_(6)composite.The doped Cu had a valence state of+2 and most likely substituted the position of Bi^(3+).The introduced Cu did not affect the metallic Bi content,but mainly influenced the energy band structure of Bi_(2)WO_(6).The band gap was slightly narrowed,the conduction band was elevated,and the work function was reduced.The reduced work function improved the transfer and separation of charge carriers,which mainly caused the increased photoactivity.The optimized NH_(3)generation rates of Bi/Cu-Bi_(2)WO_(6)reached 624 and 243μmol·L^(-1)·g^(-1)·h^(-1)under simulated solar and visible light,and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi_(2)WO_(6),respectively.This research provides a method for improving the photocatalytic N_(2)fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N_(2)-to-NH_(3)conversion.
基金supported by National Key Research and Development Program of China(grant no.2019YFA0705900)funded by MOST,the National Natural Science Foundation of China(grant nos.51820105003,21734008,61904181,and 52173188)the Key Research Program of the Chinese Academy of Sciences(grant no.XDPB13)+2 种基金the Basic and Applied Basic Research Major Program of Guangdong Province(grant no.2019B030302007)Y.W.acknowledges financial support from the Office of Naval Research(award no.N00014-19-1-2453)the use of the Stanford Synchrotron Radiation Light-source,SLAC National Accelerator Laboratory,which is supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences(contract no.DE-AC02-76SF00515).
文摘Side chain engineering with fluorine substitution is widely used to enhance photovoltaic performance of polymer donors in the research field of polymer solar cells(PSCs).However,fluorine substitution has disadvantages of complicated synthesis and high cost.Herein,we synthesized a novel D-A copolymer donor PBQ9 based on difluoroquinoxaline A-unit with chlorine substitution on its alkyl-thiophene side chains instead of fluorine substitution in the polymer donor PBQ6,which greatly shortens the synthetic route and reduces the cost.Interestingly,the optimized binary PSC with PBQ9 as polymer donor and m-TEH as acceptor demonstrated a high power conversion efficiency(PCE)of 18.81%(certified PCE of 18.33%by National Institute of Metrology,China)with a high fill factor of 80.59%,and the photovoltaic performance of the PSCs is insensitive to the different batches of the polymer donor.The results indicate that PBQ9 is a high-performance polymer donor and that chlorine substitution is an effective strategy to improve photovoltaic performance and reduce the cost of polymer donors.
基金the National Key Research and Development Program of China(2019YFA0705900)the National Natural Science Foundation of China(51820105003,21734008,61904181,52173188 and 52103243)+1 种基金the Key Research Program of the Chinese Academy of Sciences(XDPB13)the Basic and Applied Basic Research Major Program of Guangdong Province(2019B030302007).
文摘降低电压损失(V_(loss))是有机光伏电池未来商业化应用面临的关键挑战之一.V_(loss)一般由活性层材料的光学带隙和器件的开路电压(V_(oc))之差定义,而V_(oc)则由给受体之间的最低未占据分子轨(LUMO)和最高占据分子轨道(HOMO)之间的能级差决定.本文通过引入苯并三唑(BTz)π-桥单元,利用末端调控策略合成了两种A-π-D-π-A型小分子给体SMBTz-1和SM-BTz-2.结果显示,BTzπ-桥单位显著降低了小分子给体的HOMO能级,使其具有较高的Voc和载流子迁移率,实现了高效率与低能量损失(小于0.5 eV)之间的平衡.最终,以SM-BTz-2为给体,Y6为受体的全小分子有机太阳能电池V_(o c)为0.91 V,短路电流密度(J_(sc))为22.8 mA cm^(−2),填充因子为68%,能量转化效率为14.12%.此外,该工作也进一步说明了苯并三唑π-桥单元是提高载流子迁移率,降低能量损失的有效构建单元.
