Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
The interfaces between the inorganic metal oxide and organic photoactive layer are of outmost importance for efficiency and stability in organic solar cells(OSCs).Tin oxide(SnO_(2))is one of the promising candidates f...The interfaces between the inorganic metal oxide and organic photoactive layer are of outmost importance for efficiency and stability in organic solar cells(OSCs).Tin oxide(SnO_(2))is one of the promising candidates for the electron transport layer(ETL)in high-performance inverted OSCs.When a solution-processed SnO_(2)ETL is employed,however,the presence of interfacial defects and suboptimal interfacial contact can lower the power conversion efficiency(PCE)and operational stability of OSCs.Herein,highly efficient and stable inverted OSCs by modification of the SnO_(2)surface with ultraviolet(UV)-curable acrylate oligomers(SAR and OCS)are demonstrated.The highest PCEs of 16.6%and 17.0%are achieved in PM6:Y6-BO OSCs with the SAR and OCS,respectively,outperforming a device with a bare SnO_(2)ETL(PCE 13.8%).The remarkable enhancement of PCEs is attributed to the optimized interfacial contact,leading to mitigated surface defects.More strikingly,improved light-soaking and thermal stability strongly correlated with the interfacial defects are demonstrated for OSCs based on SnO_(2)/UV cross-linked resins compared to OSCs utilizing bare SnO_(2).We believe that UV cross-linking oligomers will play a key role as interfacial modifiers in the future fabrication of large-area and flexible OSCs with high efficiency and stability.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金the Partnership for Skills in Applied Sciences,Engineering and Technology(PASET)-Regional Scholarship Innovation Fund(RSIF)(World Bank PASET No.IP22-15)supported by the National Research Foundation(NRF)(NRF-2021R1A2C2091787 and NRF-2022M3H4A1A03076280)+1 种基金the Korea Research Institute of Chemical Technology(KRICT)of the Republic of Korea(No.KS2422-10)the National Research Council of Science and Technology(Grant No.Global-23-007)of Republic of Korea。
文摘The interfaces between the inorganic metal oxide and organic photoactive layer are of outmost importance for efficiency and stability in organic solar cells(OSCs).Tin oxide(SnO_(2))is one of the promising candidates for the electron transport layer(ETL)in high-performance inverted OSCs.When a solution-processed SnO_(2)ETL is employed,however,the presence of interfacial defects and suboptimal interfacial contact can lower the power conversion efficiency(PCE)and operational stability of OSCs.Herein,highly efficient and stable inverted OSCs by modification of the SnO_(2)surface with ultraviolet(UV)-curable acrylate oligomers(SAR and OCS)are demonstrated.The highest PCEs of 16.6%and 17.0%are achieved in PM6:Y6-BO OSCs with the SAR and OCS,respectively,outperforming a device with a bare SnO_(2)ETL(PCE 13.8%).The remarkable enhancement of PCEs is attributed to the optimized interfacial contact,leading to mitigated surface defects.More strikingly,improved light-soaking and thermal stability strongly correlated with the interfacial defects are demonstrated for OSCs based on SnO_(2)/UV cross-linked resins compared to OSCs utilizing bare SnO_(2).We believe that UV cross-linking oligomers will play a key role as interfacial modifiers in the future fabrication of large-area and flexible OSCs with high efficiency and stability.