The development of metal sulfide catalysts with remarkable activity toward efficient overall photocatalytic water splitting remains challenging owing to the dominant charge recombination and deficient catalytic active...The development of metal sulfide catalysts with remarkable activity toward efficient overall photocatalytic water splitting remains challenging owing to the dominant charge recombination and deficient catalytic active sites.Moreover,in the process of water oxidation catalysis,the inhibition of severe photocorrosion is an immense task,requiring effective photogenic hole-transfer kinetics.Herein,stratified Co-MnO_(2)@CdS/CoS hollow cubes with spatially separated catalytic sites were rationally designed and fabricated as highly efficient controllable catalysts for photocatalytic overall water splitting.The unique self-templated method,including a continuous anion/cation-exchange reaction,integrates a Co-doped oxidation co-catalyst(Co-MnO_(2))and a reduction co-catalyst(CoS)on the nanocubes with uniform interface contact and ultrathin two-dimensional(2D)nanometer sheets.We demonstrate that the stratified Co-MnO_(2)@CdS/CoS hollow cubes can provide an abundance of active sites for surface redox reactions and contribute to the separation and migration of the photoionization charge carriers.In particular,CoS nanoparticles dispersed on the walls of CdS hollow cubes were identified as reduction co-catalysts accelerating hydrogen generation,while Co-MnO_(2) nanosheets attached to the inner walls of the CdS hollow cube were oxidation co-catalysts,promoting oxygen evolution dynamics.Benefiting from the desirable structural and compositional advantages,optimized stratification of Co-MnO_(2)@CdS/CoS nanocubes provided a catalytic system devoid of precious metals,which exhibited a remarkable overall photocatalytic water-splitting rate(735.4(H_(2))and 361.1(O_(2))μmol h^(−1) g^(−1)),being among the highest values reported thus far for CdS-based catalysts.Moreover,an apparent quantum efficiency(AQE)of 1.32%was achieved for hydrogen evolution at 420 nm.This study emphasizes the importance of rational design on the structure and composition of photocatalysts for overall water splitting.展开更多
Objective: To evaluate the efficacy and safety of irinotecan (CPT-11) plus cisplatin (DDP) in patients with small cell lung cancer (SCLC) as second-line chemotherapy. Methods: Patients received irinotecan 60 m...Objective: To evaluate the efficacy and safety of irinotecan (CPT-11) plus cisplatin (DDP) in patients with small cell lung cancer (SCLC) as second-line chemotherapy. Methods: Patients received irinotecan 60 mg/m^2 on days 1, 8, 15, and cisplatin 25 mg/m^2 on days 1-3, every 28 days one cycle. Response was evaluated every two cycles and patients were follow-up for two years or until death. Results: Among the 28 evaluable patients, there were 1 CR, 7 PR, 8 SD and 12 PD. The response rate was 28.6% (8/28). Median time to progression (TTP) was 3.2 (0.8-5.6) months. Median survival after second-line treatment was 7.5 (1.5-31) months and overall survival was 15 (2.3-43.5) months. The most common adverse effect was hematological toxicity with 36.7% (11/30), grades Ⅲ-Ⅳ neutroperia. Hepatic toxicity was another major side effect. Only one patient developed grade Ⅲ diarrhea. Conclusion: The combination of irinotecan and cisplatin is feasible, effective, and safe for SCLC as second-line treatment.展开更多
A copper-catalyzed highly stereoselective cyclopropanation of 1,2-disubstituted olefins with α-nitrodiazo acetates has been developed, giving the desired products in up to 97 % yields, up to 〉99/1 dr and up to 98 % ...A copper-catalyzed highly stereoselective cyclopropanation of 1,2-disubstituted olefins with α-nitrodiazo acetates has been developed, giving the desired products in up to 97 % yields, up to 〉99/1 dr and up to 98 % ee, which provides an efficient access to the synthesis of optical active cyclopropane α-amino acids and unnatural α-amino acid derivatives.展开更多
文摘The development of metal sulfide catalysts with remarkable activity toward efficient overall photocatalytic water splitting remains challenging owing to the dominant charge recombination and deficient catalytic active sites.Moreover,in the process of water oxidation catalysis,the inhibition of severe photocorrosion is an immense task,requiring effective photogenic hole-transfer kinetics.Herein,stratified Co-MnO_(2)@CdS/CoS hollow cubes with spatially separated catalytic sites were rationally designed and fabricated as highly efficient controllable catalysts for photocatalytic overall water splitting.The unique self-templated method,including a continuous anion/cation-exchange reaction,integrates a Co-doped oxidation co-catalyst(Co-MnO_(2))and a reduction co-catalyst(CoS)on the nanocubes with uniform interface contact and ultrathin two-dimensional(2D)nanometer sheets.We demonstrate that the stratified Co-MnO_(2)@CdS/CoS hollow cubes can provide an abundance of active sites for surface redox reactions and contribute to the separation and migration of the photoionization charge carriers.In particular,CoS nanoparticles dispersed on the walls of CdS hollow cubes were identified as reduction co-catalysts accelerating hydrogen generation,while Co-MnO_(2) nanosheets attached to the inner walls of the CdS hollow cube were oxidation co-catalysts,promoting oxygen evolution dynamics.Benefiting from the desirable structural and compositional advantages,optimized stratification of Co-MnO_(2)@CdS/CoS nanocubes provided a catalytic system devoid of precious metals,which exhibited a remarkable overall photocatalytic water-splitting rate(735.4(H_(2))and 361.1(O_(2))μmol h^(−1) g^(−1)),being among the highest values reported thus far for CdS-based catalysts.Moreover,an apparent quantum efficiency(AQE)of 1.32%was achieved for hydrogen evolution at 420 nm.This study emphasizes the importance of rational design on the structure and composition of photocatalysts for overall water splitting.
文摘Objective: To evaluate the efficacy and safety of irinotecan (CPT-11) plus cisplatin (DDP) in patients with small cell lung cancer (SCLC) as second-line chemotherapy. Methods: Patients received irinotecan 60 mg/m^2 on days 1, 8, 15, and cisplatin 25 mg/m^2 on days 1-3, every 28 days one cycle. Response was evaluated every two cycles and patients were follow-up for two years or until death. Results: Among the 28 evaluable patients, there were 1 CR, 7 PR, 8 SD and 12 PD. The response rate was 28.6% (8/28). Median time to progression (TTP) was 3.2 (0.8-5.6) months. Median survival after second-line treatment was 7.5 (1.5-31) months and overall survival was 15 (2.3-43.5) months. The most common adverse effect was hematological toxicity with 36.7% (11/30), grades Ⅲ-Ⅳ neutroperia. Hepatic toxicity was another major side effect. Only one patient developed grade Ⅲ diarrhea. Conclusion: The combination of irinotecan and cisplatin is feasible, effective, and safe for SCLC as second-line treatment.
基金supported by the National Natural Science Foundation of China(21421091,21432011 and21272250)the Chinese Academy of Sciences
文摘A copper-catalyzed highly stereoselective cyclopropanation of 1,2-disubstituted olefins with α-nitrodiazo acetates has been developed, giving the desired products in up to 97 % yields, up to 〉99/1 dr and up to 98 % ee, which provides an efficient access to the synthesis of optical active cyclopropane α-amino acids and unnatural α-amino acid derivatives.