To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(...To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(2)reduction pretreatment.The NH_(3)-SCO activity of the adjusted 2Co/Al_(2)O_(3)catalyst was substantially improved,outperforming other catalysts with higher Co-loading.Fresh Co/Al_(2)O_(3)catalysts exhibited multitemperature reduction processes,enabling the control of the valence state of the Co-active centers by adjusting the reduction temperature.Changes in the state of the Co-active centers also led to differences in redox capacity of the catalysts,resulting in different reaction mechanisms for NH_(3)-SCO.However,in situ diffuse reflectance infrared Fourier transform spectra revealed that an excessive O_(2)activation capacity caused overoxidation of NH_(3)to NO and NO_(2).The NH_(3)-SCO activity of the 2Co/Al_(2)O_(3)catalyst with low redox capacity was successfully increased while controlling and optimizing the N_(2)selectivity by modulating the active centers via H_(2)pretreatment,which is a universalmethod used for enhancing the redox properties of catalysts.Thus,this method has great potential for application in the design of inexpensive and highly active catalysts.展开更多
NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Cont...NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Controlling NH_(3) emissions caused by ammonia escaping from mobile and industrial sources can effectively reduce the NH_(3) content in ambient air. Among the various NH_(3) removal methods, the selective catalytic oxygen method (NH_(3)-SCO) is committed to oxidizing NH_(3) to environmentally harmless H_(2)O and N_(2);therefore, it is the most valuable and ideal ammonia removal method. In this review, the characteristics of loaded and core-shell catalysts in NH_(3)-SCO have been reviewed in the context of catalyst structure-activity relationships, and the H_(2)O resistance and SO2 resistance of the catalysts are discussed in the context of practical application conditions. Then the effects of the valence state of the active center, oxygen species on the catalyst surface, dispersion of the active center and acidic sites on the catalyst performance are discussed comprehensively. Finally, the shortcomings of the existing catalysts are summarized and the catalyst development is discussed based on the existing studies.展开更多
Background Cervical cancer(CC)is the fourth most common cancer in women worldwide.Although immunotherapy has been applied in clinical practice,its therapeutic efficacy remains far from satisfactory,necessitating furth...Background Cervical cancer(CC)is the fourth most common cancer in women worldwide.Although immunotherapy has been applied in clinical practice,its therapeutic efficacy remains far from satisfactory,necessitating further investigation of the mechanism of CC immune remodeling and exploration of novel treatment targets.This study aimed to investigate the mechanism of CC immune remodeling and explore potential therapeutic targets.Methods We conducted single-cell RNA sequencing on a total of 17 clinical specimens,including normal cervical tissues,high-grade squamous intraepithelial lesions,and CC tissues.To validate our findings,we conducted multicolor immunohistochemical staining of CC tissues and constructed a subcutaneous tumorigenesis model in C57BL/6 mice using murine CC cell lines(TC1)to evaluate the effectiveness of combination therapy involving indoleamine 2,3-dioxygenase 1(IDO1)inhibition and immune checkpoint blockade(ICB).We used the unpaired two-tailed Student's t-test,Mann-Whitney test,or Kruskal-Wallis test to compare continuous data between two groups and one-way ANOVA with Tukey's post hoc test to compare data between multiple groups.Results Malignant cervical epithelial cells did not manifest noticeable signs of tumor escape,whereas lysosomal-associated membrane protein 3-positive(LAMP3^(+))dendritic cells(DCs)in a mature state with immunoregulatory roles were found to express IDO1 and affect tryptophan metabolism.These cells interacted with both tumor-reactive exhausted CD8^(+)T cells and CD4^(+) regulatory T cells,synergistically forming a vicious immunosuppressive cycle and mediating CC immune escape.Further validation through multicolor immunohistochemical staining showed co-localization of neoantigen-reactive T cells(CD3^(+),CD4^(+)/CD8^(+),and PD-1^(+))and LAMP3+DCs(CD80^(+) and PD-L1^(+)).Additionally,a combination of the IDO1 inhibitor with an ICB agent significantly reduced tumor volume in the mouse model of CC compared with an ICB agent alone.Conclusions Our study suggested that a combination treatment consisting of targeting IDO1 and ICB agent could improve the therapeutic efficacy of current CC immunotherapies.Additionally,our results provided crucial insights for designing drugs and conducting future clinical trials for CC.展开更多
基金supported by the National Natural Science Foundation of China(No.52260013)Yunnan Major Scientific and Technological Projects(No.202202AG050005).
文摘To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(2)reduction pretreatment.The NH_(3)-SCO activity of the adjusted 2Co/Al_(2)O_(3)catalyst was substantially improved,outperforming other catalysts with higher Co-loading.Fresh Co/Al_(2)O_(3)catalysts exhibited multitemperature reduction processes,enabling the control of the valence state of the Co-active centers by adjusting the reduction temperature.Changes in the state of the Co-active centers also led to differences in redox capacity of the catalysts,resulting in different reaction mechanisms for NH_(3)-SCO.However,in situ diffuse reflectance infrared Fourier transform spectra revealed that an excessive O_(2)activation capacity caused overoxidation of NH_(3)to NO and NO_(2).The NH_(3)-SCO activity of the 2Co/Al_(2)O_(3)catalyst with low redox capacity was successfully increased while controlling and optimizing the N_(2)selectivity by modulating the active centers via H_(2)pretreatment,which is a universalmethod used for enhancing the redox properties of catalysts.Thus,this method has great potential for application in the design of inexpensive and highly active catalysts.
基金the National Natural Science Foundation of China(No.52000093)Yunnan Fundamental Research Projects(No.202101BE070001-001)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019B03).
文摘NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Controlling NH_(3) emissions caused by ammonia escaping from mobile and industrial sources can effectively reduce the NH_(3) content in ambient air. Among the various NH_(3) removal methods, the selective catalytic oxygen method (NH_(3)-SCO) is committed to oxidizing NH_(3) to environmentally harmless H_(2)O and N_(2);therefore, it is the most valuable and ideal ammonia removal method. In this review, the characteristics of loaded and core-shell catalysts in NH_(3)-SCO have been reviewed in the context of catalyst structure-activity relationships, and the H_(2)O resistance and SO2 resistance of the catalysts are discussed in the context of practical application conditions. Then the effects of the valence state of the active center, oxygen species on the catalyst surface, dispersion of the active center and acidic sites on the catalyst performance are discussed comprehensively. Finally, the shortcomings of the existing catalysts are summarized and the catalyst development is discussed based on the existing studies.
基金supported by funding from Medical Innovation Research of Shanghai Science and Technology(21Y11906900 and 22Y3190050)Shanghai Hospital Development Center(SHDC2020CR1045B,SHDC2020CR6009,SHDC2020CR4087,and SHDC22021307)+2 种基金Shanghai Municipal Health Commission(202040498)National Natural Science Foundation of China(81971361 and 82173188)Program for Zhuoxue of Fudan University(JIF157600).
文摘Background Cervical cancer(CC)is the fourth most common cancer in women worldwide.Although immunotherapy has been applied in clinical practice,its therapeutic efficacy remains far from satisfactory,necessitating further investigation of the mechanism of CC immune remodeling and exploration of novel treatment targets.This study aimed to investigate the mechanism of CC immune remodeling and explore potential therapeutic targets.Methods We conducted single-cell RNA sequencing on a total of 17 clinical specimens,including normal cervical tissues,high-grade squamous intraepithelial lesions,and CC tissues.To validate our findings,we conducted multicolor immunohistochemical staining of CC tissues and constructed a subcutaneous tumorigenesis model in C57BL/6 mice using murine CC cell lines(TC1)to evaluate the effectiveness of combination therapy involving indoleamine 2,3-dioxygenase 1(IDO1)inhibition and immune checkpoint blockade(ICB).We used the unpaired two-tailed Student's t-test,Mann-Whitney test,or Kruskal-Wallis test to compare continuous data between two groups and one-way ANOVA with Tukey's post hoc test to compare data between multiple groups.Results Malignant cervical epithelial cells did not manifest noticeable signs of tumor escape,whereas lysosomal-associated membrane protein 3-positive(LAMP3^(+))dendritic cells(DCs)in a mature state with immunoregulatory roles were found to express IDO1 and affect tryptophan metabolism.These cells interacted with both tumor-reactive exhausted CD8^(+)T cells and CD4^(+) regulatory T cells,synergistically forming a vicious immunosuppressive cycle and mediating CC immune escape.Further validation through multicolor immunohistochemical staining showed co-localization of neoantigen-reactive T cells(CD3^(+),CD4^(+)/CD8^(+),and PD-1^(+))and LAMP3+DCs(CD80^(+) and PD-L1^(+)).Additionally,a combination of the IDO1 inhibitor with an ICB agent significantly reduced tumor volume in the mouse model of CC compared with an ICB agent alone.Conclusions Our study suggested that a combination treatment consisting of targeting IDO1 and ICB agent could improve the therapeutic efficacy of current CC immunotherapies.Additionally,our results provided crucial insights for designing drugs and conducting future clinical trials for CC.
