Developing fluorescence porous probe for detecting and eliminating Cu^(2+) contamination in water or biosystem is an essential research project that has attracted considerable attention.However,improving the fluoresce...Developing fluorescence porous probe for detecting and eliminating Cu^(2+) contamination in water or biosystem is an essential research project that has attracted considerable attention.However,improving the fluorescence detecting efficiency while enhancing the adsorption capacity of the porous probe is of great challenge.Herein,a bifunctional two-dimensional imine-based porous covalent organic framework(TTP-COF)probe was designed and synthesized from 1,3,5-tris(4-aminophenyl)benzene(TAPB)and 2,4,6-Triformylphloroglucinol(TP)ligand.TTP-COF displayed rapid detection of Cu^(2+)(limit of detection(LOD)=10 nmol·L^(−1) while achieving a high adsorption capacity of 214 mg·g^(−1)(pH=6)at room temperature with high reusability(>5 cycles).The key roles and contributions of highπ-conjugate and delocalized electrons in TABP and functional–OH groups in TP were proved.More importantly,the fluorescence quenching mechanism of TTP-COF was studied by density functional theory theoretical calculations,revealing the crucial role of intramolecular hydrogen bonds among C=N and–OH groups and the blocking of the excited state intramolecular proton transfer process in detecting process of Cu^(2+).展开更多
Although chemotherapy has been intensively applied in cancer treatments,its inadequate therapeutic efficacy and severe side effects are still under constant concerns.Nanoplatforms used as anti-tumor drug delivery syst...Although chemotherapy has been intensively applied in cancer treatments,its inadequate therapeutic efficacy and severe side effects are still under constant concerns.Nanoplatforms used as anti-tumor drug delivery system(DDS)have attracted tremendous attentions owing to their various intriguing properties.Herein,Mn-doped MoO_(2)nanoparticles coated with ZrO_(2)and capped with Bi_(2)O_(3)have been designed as a DDS,namely MMZB.MMZB possesses good magnetic properties,great photothermal conversion ability,sensitive tumor microenvironment(TME)responsiveness,and good biocompatibility in hemocompatibility in vitro.Thus,MMZB has been utilized to load the chemotherapeutic agent daunomycin(DNM)(MMZB@DNM)for chemo-photothermal combined therapy.MMZB@DNM demonstrates a more impressive anti-cancer effect than the individual photothermal or chemotherapy both in vitro and in vivo.Furthermore,the analysis of tumor specimen sections and serum levels after the treatment indicates negligible side effects for MMZB@DNM in vivo.This contribution provides a valuable concept in designing therapeutic agents for achieving significantly enhanced tumor treatments,which benefits from the synergistic combination of chemotherapy and photothermal therapy in one single nanoagent.展开更多
To develop efficient visible-light photocatalysis on α-Fe2O3, it is highly desirable to promote visible-light-excited high-energy-level electron transfer to a proper energy platform thermodynamically. Herein, based o...To develop efficient visible-light photocatalysis on α-Fe2O3, it is highly desirable to promote visible-light-excited high-energy-level electron transfer to a proper energy platform thermodynamically. Herein, based on the transient-state surface photovoltage responses and the atmosphere-controlled steady-state surface photovoltage spectra, it is demonstrated that the lifetime and separation of photogenerated charges of nanosized α-Fe2O3 are increased after coupling a proper amount of nanocrystalline SnO2. This naturally leads to greatly improved photocatalytic activities for CO2 reduction and acetaldehyde degradation. It is suggested that the enhanced charge separation results from the electron transfer from α-Fe2O3 to SnO2, which acts as a proper energy platform. Based on the photocurrent action spectra, it is confirmed that the coupled SnO2 exhibits longer visible-light threshold wavelength （-590 nm） compared with the coupled TiO2 （-550 nm）, indicating that the energy platform introduced by SnO2 would accept more photogenerated electrons from α-Fe2O3. Moreover, electrochemical reduction experiments proved that the coupled SnO2 possesses better catalytic ability for reducing CO2 and O2. These are well responsible for the much efficient photocatalysis on SnO2-coupled α-Fe2O3.展开更多
The electrocatalytic nitrogen reduction reaction(NRR)has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia(NH_(3))synthesis.However,finding an efficient an...The electrocatalytic nitrogen reduction reaction(NRR)has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia(NH_(3))synthesis.However,finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen(N_(2))for electrocatalytic NRR is still a challenge.Herein,a FeNi@CNS nanocomposite as an efficient catalyst for N_(2) fixation under ambient conditions is designed.This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination.The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst,which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83%and an NH_(3) yield of 16.52μg h^(−1) cm^(−2) in 0.1 M Na_(2)SO_(4) aqueous solution.Besides,high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h.Meanwhile,the FeNi@CNS catalyst encourages N_(2) adsorption and activation as well as effectively suppressing competitive HER.Therefore,this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.展开更多
基金supported by the National Natural Science Foundation of China(U1401245,91622119)the Program for Innovative Research Team in Chinese Universities(IRT1237)+1 种基金the Research Project of Chinese Ministry of Education(213011A)the Science Foundation for Excellent Youth of Harbin City of China(2014RFYXJ002)~~
基金This study was financially supported by the National Natural Science Foundation of China(Nos.22001156 and 22271178)the Innovation Capability Support Program of Shaanxi(No.2022KJXX-88)the Technology Innovation Leading Program of Shaanxi(No.2020QFY07-05).
文摘Developing fluorescence porous probe for detecting and eliminating Cu^(2+) contamination in water or biosystem is an essential research project that has attracted considerable attention.However,improving the fluorescence detecting efficiency while enhancing the adsorption capacity of the porous probe is of great challenge.Herein,a bifunctional two-dimensional imine-based porous covalent organic framework(TTP-COF)probe was designed and synthesized from 1,3,5-tris(4-aminophenyl)benzene(TAPB)and 2,4,6-Triformylphloroglucinol(TP)ligand.TTP-COF displayed rapid detection of Cu^(2+)(limit of detection(LOD)=10 nmol·L^(−1) while achieving a high adsorption capacity of 214 mg·g^(−1)(pH=6)at room temperature with high reusability(>5 cycles).The key roles and contributions of highπ-conjugate and delocalized electrons in TABP and functional–OH groups in TP were proved.More importantly,the fluorescence quenching mechanism of TTP-COF was studied by density functional theory theoretical calculations,revealing the crucial role of intramolecular hydrogen bonds among C=N and–OH groups and the blocking of the excited state intramolecular proton transfer process in detecting process of Cu^(2+).
基金supported by the National Natural Science Foundation of China(Nos.22271178 and 22001156)Project of Special Key Fields in Guangdong Province(No.2021ZDZX4019)+1 种基金the Science and technology innovation strategy of Guangdong province(No.51361212)Guangdong Provincial Science and Technology Innovation Strategy Special Fund Approval Project(No.pdjh2021b0266)。
文摘Although chemotherapy has been intensively applied in cancer treatments,its inadequate therapeutic efficacy and severe side effects are still under constant concerns.Nanoplatforms used as anti-tumor drug delivery system(DDS)have attracted tremendous attentions owing to their various intriguing properties.Herein,Mn-doped MoO_(2)nanoparticles coated with ZrO_(2)and capped with Bi_(2)O_(3)have been designed as a DDS,namely MMZB.MMZB possesses good magnetic properties,great photothermal conversion ability,sensitive tumor microenvironment(TME)responsiveness,and good biocompatibility in hemocompatibility in vitro.Thus,MMZB has been utilized to load the chemotherapeutic agent daunomycin(DNM)(MMZB@DNM)for chemo-photothermal combined therapy.MMZB@DNM demonstrates a more impressive anti-cancer effect than the individual photothermal or chemotherapy both in vitro and in vivo.Furthermore,the analysis of tumor specimen sections and serum levels after the treatment indicates negligible side effects for MMZB@DNM in vivo.This contribution provides a valuable concept in designing therapeutic agents for achieving significantly enhanced tumor treatments,which benefits from the synergistic combination of chemotherapy and photothermal therapy in one single nanoagent.
基金We are grateful for financial support from the National Natural Science Foundation of China （Nos. U1401245 and 21501052）, the National Basic Research Program of China （No. 2014CB660814）, the Project of Chinese Ministry of Education （No. 213011A）, Special Funding for Postdoctoral of Heilongjiang Province （No. LBH- TZ06019） and the Science Foundation for Excellent Youth of Harbin City of China （No. 2014RFYXJ002）.
文摘To develop efficient visible-light photocatalysis on α-Fe2O3, it is highly desirable to promote visible-light-excited high-energy-level electron transfer to a proper energy platform thermodynamically. Herein, based on the transient-state surface photovoltage responses and the atmosphere-controlled steady-state surface photovoltage spectra, it is demonstrated that the lifetime and separation of photogenerated charges of nanosized α-Fe2O3 are increased after coupling a proper amount of nanocrystalline SnO2. This naturally leads to greatly improved photocatalytic activities for CO2 reduction and acetaldehyde degradation. It is suggested that the enhanced charge separation results from the electron transfer from α-Fe2O3 to SnO2, which acts as a proper energy platform. Based on the photocurrent action spectra, it is confirmed that the coupled SnO2 exhibits longer visible-light threshold wavelength （-590 nm） compared with the coupled TiO2 （-550 nm）, indicating that the energy platform introduced by SnO2 would accept more photogenerated electrons from α-Fe2O3. Moreover, electrochemical reduction experiments proved that the coupled SnO2 possesses better catalytic ability for reducing CO2 and O2. These are well responsible for the much efficient photocatalysis on SnO2-coupled α-Fe2O3.
基金support by the National Natural Science Foundation of China(No.11774044)。
文摘The electrocatalytic nitrogen reduction reaction(NRR)has emerged as a promising renewable energy source and a feasible strategy as an alternative to Haber-Bosch ammonia(NH_(3))synthesis.However,finding an efficient and cost-effective robust catalyst to activate and cleave the extremely strong triple bond in nitrogen(N_(2))for electrocatalytic NRR is still a challenge.Herein,a FeNi@CNS nanocomposite as an efficient catalyst for N_(2) fixation under ambient conditions is designed.This FeNi@CNS nanocomposite was prepared by a simple water bath process and post-calcination.The FeNi@CNS is demonstrated to be a highly efficient NRR catalyst,which exhibits better NRR performance with exceptional Faradaic efficiency of 9.83%and an NH_(3) yield of 16.52μg h^(−1) cm^(−2) in 0.1 M Na_(2)SO_(4) aqueous solution.Besides,high stability and reproducibility with consecutive 6 cycles for two hours are also demonstrated throughout the NRR electrocatalytic process for 12 h.Meanwhile,the FeNi@CNS catalyst encourages N_(2) adsorption and activation as well as effectively suppressing competitive HER.Therefore,this earth-abundant FeNi@CNS catalyst with a subtle balance of activity and stability has excellent potential in NRR industrial applications.
