Renewable and economical generation of hydrogen via electrochemical methods shows great potential in addressing the energy crisis.In this study,an emerging molten salt method was adopted for the synthesis of a cerium-...Renewable and economical generation of hydrogen via electrochemical methods shows great potential in addressing the energy crisis.In this study,an emerging molten salt method was adopted for the synthesis of a cerium-modifi ed rhenium disulfi de nanosheet for electrical hydrogen evolution reactions.The prepared 1%Ce-doped rhenium disulfi de(ReS_(2))sample showed promoted hydrogen evolution performance in both acid and alkaline electrolytes compared to bare ReS_(2).Generating of abundant defects in ReS_(2)exposed more reaction active sites.Moreover,adding cerium accelerated the hydrogen evolution dynamics.Hopefully,this work will off er new insight into developing ReS_(2)-based electrocatalysts for hydrogen evolution reactions.展开更多
One of the critical problems in bladder cancer(BC)management is the local recurrence of disease.However,achieving the accurate delineation of tumor margins intraoperatively remains extremely difficult due to the lack ...One of the critical problems in bladder cancer(BC)management is the local recurrence of disease.However,achieving the accurate delineation of tumor margins intraoperatively remains extremely difficult due to the lack of effective tumor margin recognition technology.Herein,survivin molecular beacon(MB)and R11 peptide-linked spherical nucleic acids(SNAs)were synthesized as nanoprobes(AuNP-MB@R11)for sensitive detection of BC margins.Physicochemical properties proved that R11 peptides and survivin MB were successfully loaded onto the surface of SNAs.AuNP-MB@R11 had good stability against nuclease activity and high sensitivity and specificity to detect survivin single strand DNA(ssDNA)in vitro.According to cytology,R11 peptides could increase the BC targeting ability and membrane penetrability of SNAs.Notably,R11 peptides significantly promoted the disintegration of lysosomes and the release of SNAs to enhance fluorescence imaging quality.Further RNA sequencing proved that some genes and pathways related to endocytosis and lysosomes were significantly regulated,such as AGPAT5,GPD1L,and GRB2.In orthotopic BC models and a clinical sample from a patient with BC,AuNP-MB@R11 showed a more legible cancerous fluorescence margin and offered remarkably improved detection compared to those achieved by SNAs.R11 peptide-linked SNAs present promising potential to identify BC margin,which may help to improve the R0 resection rate in surgery and improve patients’quality of life.展开更多
Recently,surface-enhanced Raman scattering(SERS)has been successfully used in the non-invasive detection of bladder tumor(BCa).The internal standard method was considered as an effective ratiometric strategy for calib...Recently,surface-enhanced Raman scattering(SERS)has been successfully used in the non-invasive detection of bladder tumor(BCa).The internal standard method was considered as an effective ratiometric strategy for calibrating signal fluctuation originated from the interference of measurement conditions and samples.However,it is still difficult to detect the target mRNA quantitatively using the current ratiometric SERS nanosensors.In this study,we developed an internal reference based ratiometric SERS assay.Two kinds of molecular beacons(MB)carrying Raman reporter molecules were anchored on sea-urchinlike Au nanoclusters(AuNCs).Thymidine kinase1(TK1)MBs with hexachlorofluorescein(HEX)were used to capture tumor biomarker TK1 mRNA,and glyceraldehyde 3-phosphate dehydrogenase(GAPDH)MBs with 5(6)-carboxyfluorescein(FAM)were used to offer internal standard signals.The internal reference GAPDH MB can reflect the consistent content of the GAPDH mRNA in single cells.The ratiometric method(I745/I645)can more accurately reflect the content of target mRNA in single cells.The ratiometric nanoprobes had excellent stability(coefficient of variation:0.3%),high sensitivity(detection limit:3.4 pM),high specificity(capable of single-base mismatch recognition)and ribozyme-resistant stability.Notably,the nanoprobes can effectively distinguish BCa cells from normal cells,and it was easy to contour the single BCa cell using the ratiometric method.By combining asymmetric polymerase chain reaction(PCR)and ratiometric nanoprobes,it was easy to distinguish the SERS ratio(I_(745)/I_(645))as low concentration as 10-14 M.Further clinical detection in urine samples from patients with BCa confirmed its potential for early noninvasive diagnosis of BCa with the sensitivity of 80%and specificity of 100%,which is superior to the current urine cytological method.展开更多
基金supported by Talent Program of Huangshan University(No.2020xkjq010)Bureau of Huangshan Ecological Environment(No.hkxt2021212)+1 种基金Key Project of Natural Science Research in Anhui Universities(No.KJ2020A0690)Major Project of Natural Science Research in Anhui Universities(No.KJ2019ZD42).
文摘Renewable and economical generation of hydrogen via electrochemical methods shows great potential in addressing the energy crisis.In this study,an emerging molten salt method was adopted for the synthesis of a cerium-modifi ed rhenium disulfi de nanosheet for electrical hydrogen evolution reactions.The prepared 1%Ce-doped rhenium disulfi de(ReS_(2))sample showed promoted hydrogen evolution performance in both acid and alkaline electrolytes compared to bare ReS_(2).Generating of abundant defects in ReS_(2)exposed more reaction active sites.Moreover,adding cerium accelerated the hydrogen evolution dynamics.Hopefully,this work will off er new insight into developing ReS_(2)-based electrocatalysts for hydrogen evolution reactions.
基金the National Natural Science Foundation of China(No.81901838)Key research and development plan in Shaanxi province(Nos.2020SF-123 and 2020SF-195)+1 种基金Medical Technology Plan of Zhejiang Province(No.2021KY042)Medical research program of department of science and technology of Xi’an,Shaanxi Province(No.2019115713YX012SF048(4)).
文摘One of the critical problems in bladder cancer(BC)management is the local recurrence of disease.However,achieving the accurate delineation of tumor margins intraoperatively remains extremely difficult due to the lack of effective tumor margin recognition technology.Herein,survivin molecular beacon(MB)and R11 peptide-linked spherical nucleic acids(SNAs)were synthesized as nanoprobes(AuNP-MB@R11)for sensitive detection of BC margins.Physicochemical properties proved that R11 peptides and survivin MB were successfully loaded onto the surface of SNAs.AuNP-MB@R11 had good stability against nuclease activity and high sensitivity and specificity to detect survivin single strand DNA(ssDNA)in vitro.According to cytology,R11 peptides could increase the BC targeting ability and membrane penetrability of SNAs.Notably,R11 peptides significantly promoted the disintegration of lysosomes and the release of SNAs to enhance fluorescence imaging quality.Further RNA sequencing proved that some genes and pathways related to endocytosis and lysosomes were significantly regulated,such as AGPAT5,GPD1L,and GRB2.In orthotopic BC models and a clinical sample from a patient with BC,AuNP-MB@R11 showed a more legible cancerous fluorescence margin and offered remarkably improved detection compared to those achieved by SNAs.R11 peptide-linked SNAs present promising potential to identify BC margin,which may help to improve the R0 resection rate in surgery and improve patients’quality of life.
基金This work was supported by the National Natural Science Foundation of China(No.81901838)the Key Research and Development Plan in Shaanxi Province(Nos.2020SF-123 and 2020SF-195)+1 种基金the Natural Science Foundation of Zhejiang Province(No.LQ21H160041)the Medical Research Program of Department of Science and Technology of Xi’an,Shaanxi Province(No.2019115713YX012SF048(4)).
文摘Recently,surface-enhanced Raman scattering(SERS)has been successfully used in the non-invasive detection of bladder tumor(BCa).The internal standard method was considered as an effective ratiometric strategy for calibrating signal fluctuation originated from the interference of measurement conditions and samples.However,it is still difficult to detect the target mRNA quantitatively using the current ratiometric SERS nanosensors.In this study,we developed an internal reference based ratiometric SERS assay.Two kinds of molecular beacons(MB)carrying Raman reporter molecules were anchored on sea-urchinlike Au nanoclusters(AuNCs).Thymidine kinase1(TK1)MBs with hexachlorofluorescein(HEX)were used to capture tumor biomarker TK1 mRNA,and glyceraldehyde 3-phosphate dehydrogenase(GAPDH)MBs with 5(6)-carboxyfluorescein(FAM)were used to offer internal standard signals.The internal reference GAPDH MB can reflect the consistent content of the GAPDH mRNA in single cells.The ratiometric method(I745/I645)can more accurately reflect the content of target mRNA in single cells.The ratiometric nanoprobes had excellent stability(coefficient of variation:0.3%),high sensitivity(detection limit:3.4 pM),high specificity(capable of single-base mismatch recognition)and ribozyme-resistant stability.Notably,the nanoprobes can effectively distinguish BCa cells from normal cells,and it was easy to contour the single BCa cell using the ratiometric method.By combining asymmetric polymerase chain reaction(PCR)and ratiometric nanoprobes,it was easy to distinguish the SERS ratio(I_(745)/I_(645))as low concentration as 10-14 M.Further clinical detection in urine samples from patients with BCa confirmed its potential for early noninvasive diagnosis of BCa with the sensitivity of 80%and specificity of 100%,which is superior to the current urine cytological method.
