The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry.By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)_(2)I andβ-diketiminato Fe^Ⅱch...The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry.By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)_(2)I andβ-diketiminato Fe^Ⅱchloride,the ferrogermylene complexes 3a,3b and 4a were synthesized and structurally characterized.The structural and IR characterizations show the presence of the Ge←Feπbackbonding in molecules 3a,3b and 4a.The computational works on frontier molecular orbitals and their comparison of energy states confirmed thatσdonation andπbackbonding are both weak in these molecules,despite three complexes have longer Ge-Fe bonds,whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a,3b to 4a.展开更多
Nitroaromatic hydrogenation catalysis without precious metals remains a longstanding challenge.The rate of electron transfer is the crucial factor affecting hydrogenation catalysis.Herein,an ionic Cd-based metal-organ...Nitroaromatic hydrogenation catalysis without precious metals remains a longstanding challenge.The rate of electron transfer is the crucial factor affecting hydrogenation catalysis.Herein,an ionic Cd-based metal-organic framework(I-Cd-MOF)exhibiting a unique structure with one-dimensional(1D)opening nanochannels and good electron transfer ability was synthesized for catalyzing hydrogenation of 4-nitrophenol(4-NP).The catalytic activity of the unique I-Cd-MOF without noble metals is detected,which is higher than most reported noble metal catalysts.Remarkably,the reaction rate of I-Cd-MOF(4.28 min^(-1))is about 47.6 times higher than that of the Cd-based neutral MOF(N-Cd-MOF)with the similar crystalline structure.Liquid chromatograph mass spectrometer(LC-MS)and theoretical results demonstrate that 4-NP and five intermediates are stabilized in the channels of I-Cd-MOF,which increases the possibility of contact with H^*and H_(2)g enerated at the Cd sites.The I-Cd-MOF was extended to other nitroaromatic hydrogenation catalysis,which still displays excellent activity.More importantly,the I-MOF@Filter membrane was successfully constructed for continuous hydrogenation catalytic reactions,which maintains a high catalytic performance after 7 cycles of recycling without washing.This work fills in the application of the I-MOFs in hydrogenation catalytic reactions and provides an effective way for the rapid and green degradation of nitroaromatic compounds.展开更多
The hydrogen-bonded(H-bonded)base pairs,double H-bonded A•T and triple H-bonded G•C in DNA,are important units for storing,encoding,and expressing genetic information.Owing to the interference from water,however,the f...The hydrogen-bonded(H-bonded)base pairs,double H-bonded A•T and triple H-bonded G•C in DNA,are important units for storing,encoding,and expressing genetic information.Owing to the interference from water,however,the formation of H-bonded base pairs from short deoxynucleotide fragments such as mono-or di-deoxynucleotide are not easily achieved in aqueous solutions.展开更多
Ovarian cancer(OC)is a lethal threat to females.According to the 2022 Global Cancer Observatory(GLOBOCAN),new cases of OC were estimated to reach 324,398,with mortality figures at 206,839.China,with one-fifth of the w...Ovarian cancer(OC)is a lethal threat to females.According to the 2022 Global Cancer Observatory(GLOBOCAN),new cases of OC were estimated to reach 324,398,with mortality figures at 206,839.China,with one-fifth of the world population,is bearing a heavy OC health burden,accounting for 18.82%of all OC new cases and 15.8%of OC-related deaths worldwide.The OC incidence and mortality in China increased by 6.3%and 20%in the time intervals from 2016 to 2022,with a significant disparity between urban and rural areas in China[Supplementary Figure 1A,http://links.lww.com/CM9/C570].The new cases and deaths will reach 70,822 and 46,845 by 2050,respectively[Supplementary Figure 1B,http://links.lww.com/CM9/C570].Moreover,females are more susceptible to OC at ages above 50 years[Supplementary Figures 1C and D,http://links.lww.com/CM9/C570].Notably,nearly 50–70%of OC patients suffer from disease recurrence and will ultimately develop platinum resistance,causing over 90%of deaths with a median survival of less than 12 months.展开更多
Background:Burkholderia pseudomallei is a tropical pathogen that causes melioidosis.Its intrinsic drug-resistance is a leading cause of treatment failure,and the few available antibiotics require prolonged use to be e...Background:Burkholderia pseudomallei is a tropical pathogen that causes melioidosis.Its intrinsic drug-resistance is a leading cause of treatment failure,and the few available antibiotics require prolonged use to be effective.This study aimed to assess the clinical potential of B.pseudomallei phages isolated from Hainan,China.Methods:Burkholderia pseudomallei strain(HNBPoo1)was used as the isolation host,and phages were recovered from domestic environmental sources,which were submitted to the host range determination,lytic property assays,and stability tests.The best candidate was examined via the transmission electron microscope for classification.With its genome sequenced and analyzed,its protective efficacy against B.pseudomallei infection in A549 cells and Caenorhabditis elegans was evaluated,in which cell viability and survival rates were compared using the one-way ANOVA method and the log-rank test.Results:A phage able to lyse 24/25 clinical isolates was recovered.It was classified in the Podoviridae family and was found to be amenable to propagation.Under the optimal multiplicity of infection(MOl)of o.1,an eclipse period of around 20 min and a high titer(io12 PFU/ml)produced within 1 h were demonstrated.This phage was found stabile at a wide range of temperatures(24,37,40,50,and 60 C)and pH values(3-12).After being designated as vB_BpP_HN01,it was fully sequenced,and the 71,398 bp linear genome,containing 93 open reading frames and a tRNA-Asn,displayed a low sequence similarity with known viruses.Additionally,protective effects of applications of vB_BpP_HNo1(MOl=0.1 and MOl=1)alone or in combination with antibiotics were found to improve viability of infected cells(70.6±6.8%,85.8±5.7%,91.9±1.8%,and 96.8±1.8%,respectively).A significantly reduced mortality(10%)and a decreased pathogen load were demonstrated in infected C.elegans following the addition of this phage.Conclusions:As the frst B.pseudomallei phage was isolated in Hainan,China,phage vB_BpP_HNO1 was characterized by promising lytic property,stability,and effciency of bacterial elimination during the in vitro/vivo experiments.Therefore,we can conclude that it is a potential alternative agent for combating melioidosis.展开更多
基金supported by National Science Foundation of China(No.22273072)the Shaanxi Provincial Enterprise Joint Fund(No.2021JLM-31)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2021JM-311)。
文摘The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry.By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)_(2)I andβ-diketiminato Fe^Ⅱchloride,the ferrogermylene complexes 3a,3b and 4a were synthesized and structurally characterized.The structural and IR characterizations show the presence of the Ge←Feπbackbonding in molecules 3a,3b and 4a.The computational works on frontier molecular orbitals and their comparison of energy states confirmed thatσdonation andπbackbonding are both weak in these molecules,despite three complexes have longer Ge-Fe bonds,whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a,3b to 4a.
基金the financial support provided by the NSFC(No.21531007)the Shaanxi Provincial Natural Science Basic Research Program(No.2019JM-590)the Shaanxi Science and Technology Department(Nos.2022GY-384,2022JBGS2–07,2021LLRH05–21,2022QFY06–06)。
文摘Nitroaromatic hydrogenation catalysis without precious metals remains a longstanding challenge.The rate of electron transfer is the crucial factor affecting hydrogenation catalysis.Herein,an ionic Cd-based metal-organic framework(I-Cd-MOF)exhibiting a unique structure with one-dimensional(1D)opening nanochannels and good electron transfer ability was synthesized for catalyzing hydrogenation of 4-nitrophenol(4-NP).The catalytic activity of the unique I-Cd-MOF without noble metals is detected,which is higher than most reported noble metal catalysts.Remarkably,the reaction rate of I-Cd-MOF(4.28 min^(-1))is about 47.6 times higher than that of the Cd-based neutral MOF(N-Cd-MOF)with the similar crystalline structure.Liquid chromatograph mass spectrometer(LC-MS)and theoretical results demonstrate that 4-NP and five intermediates are stabilized in the channels of I-Cd-MOF,which increases the possibility of contact with H^*and H_(2)g enerated at the Cd sites.The I-Cd-MOF was extended to other nitroaromatic hydrogenation catalysis,which still displays excellent activity.More importantly,the I-MOF@Filter membrane was successfully constructed for continuous hydrogenation catalytic reactions,which maintains a high catalytic performance after 7 cycles of recycling without washing.This work fills in the application of the I-MOFs in hydrogenation catalytic reactions and provides an effective way for the rapid and green degradation of nitroaromatic compounds.
基金supported by the National Natural Science Foundation of China(nos.22122108,21971208,and 21771145)the Natural Science Basic Research Plan for Distinguished Young Scholars in Shaanxi Province of China(no.2021JC-37)+1 种基金the Fok Ying Tong Education Foundation(no.171010)the Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates(no.2019B030301003)from South China University of Technology.
文摘The hydrogen-bonded(H-bonded)base pairs,double H-bonded A•T and triple H-bonded G•C in DNA,are important units for storing,encoding,and expressing genetic information.Owing to the interference from water,however,the formation of H-bonded base pairs from short deoxynucleotide fragments such as mono-or di-deoxynucleotide are not easily achieved in aqueous solutions.
基金supported by grants from the National Natural Science Foundation of China(No.82374081)the Natural Science Foundation of Fujian Province(No.2023J011257).
文摘Ovarian cancer(OC)is a lethal threat to females.According to the 2022 Global Cancer Observatory(GLOBOCAN),new cases of OC were estimated to reach 324,398,with mortality figures at 206,839.China,with one-fifth of the world population,is bearing a heavy OC health burden,accounting for 18.82%of all OC new cases and 15.8%of OC-related deaths worldwide.The OC incidence and mortality in China increased by 6.3%and 20%in the time intervals from 2016 to 2022,with a significant disparity between urban and rural areas in China[Supplementary Figure 1A,http://links.lww.com/CM9/C570].The new cases and deaths will reach 70,822 and 46,845 by 2050,respectively[Supplementary Figure 1B,http://links.lww.com/CM9/C570].Moreover,females are more susceptible to OC at ages above 50 years[Supplementary Figures 1C and D,http://links.lww.com/CM9/C570].Notably,nearly 50–70%of OC patients suffer from disease recurrence and will ultimately develop platinum resistance,causing over 90%of deaths with a median survival of less than 12 months.
文摘Background:Burkholderia pseudomallei is a tropical pathogen that causes melioidosis.Its intrinsic drug-resistance is a leading cause of treatment failure,and the few available antibiotics require prolonged use to be effective.This study aimed to assess the clinical potential of B.pseudomallei phages isolated from Hainan,China.Methods:Burkholderia pseudomallei strain(HNBPoo1)was used as the isolation host,and phages were recovered from domestic environmental sources,which were submitted to the host range determination,lytic property assays,and stability tests.The best candidate was examined via the transmission electron microscope for classification.With its genome sequenced and analyzed,its protective efficacy against B.pseudomallei infection in A549 cells and Caenorhabditis elegans was evaluated,in which cell viability and survival rates were compared using the one-way ANOVA method and the log-rank test.Results:A phage able to lyse 24/25 clinical isolates was recovered.It was classified in the Podoviridae family and was found to be amenable to propagation.Under the optimal multiplicity of infection(MOl)of o.1,an eclipse period of around 20 min and a high titer(io12 PFU/ml)produced within 1 h were demonstrated.This phage was found stabile at a wide range of temperatures(24,37,40,50,and 60 C)and pH values(3-12).After being designated as vB_BpP_HN01,it was fully sequenced,and the 71,398 bp linear genome,containing 93 open reading frames and a tRNA-Asn,displayed a low sequence similarity with known viruses.Additionally,protective effects of applications of vB_BpP_HNo1(MOl=0.1 and MOl=1)alone or in combination with antibiotics were found to improve viability of infected cells(70.6±6.8%,85.8±5.7%,91.9±1.8%,and 96.8±1.8%,respectively).A significantly reduced mortality(10%)and a decreased pathogen load were demonstrated in infected C.elegans following the addition of this phage.Conclusions:As the frst B.pseudomallei phage was isolated in Hainan,China,phage vB_BpP_HNO1 was characterized by promising lytic property,stability,and effciency of bacterial elimination during the in vitro/vivo experiments.Therefore,we can conclude that it is a potential alternative agent for combating melioidosis.
