Electrochemical CO2 reduction reaction(CO2RR)powered by renewable electricity has emerged as the most promising technique for CO2 conversion,making it possible to realize a carbon‐neutral cycle.Highly efficient,robus...Electrochemical CO2 reduction reaction(CO2RR)powered by renewable electricity has emerged as the most promising technique for CO2 conversion,making it possible to realize a carbon‐neutral cycle.Highly efficient,robust,and cost‐effective catalysts are highly demanded for the near‐future practical applications of CO2RR.Previous studies on atomically dispersed metal‐nitrogen(M‐Nx)sites constituted of earth abundant elements with maximum atom‐utilization efficiency have demonstrated their performance towards CO2RR.This review summarizes recent advances on a variety of M‐Nx sites‐containing transition metal‐centered macrocyclic complexes,metal organic frameworks,and M‐Nx‐doped carbon materials for efficient CO2RR,including both experimental and theoretical studies.The roles of metal centers,coordinated ligands,and conductive supports on the intrinsic activity and selectivity,together with the importance of reaction conditions for improved performance are discussed.The mechanisms of CO2RR over these M‐Nx‐containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO2RR.展开更多
In this work, a double signal amplified immunosen- sor based on the enhanced CdSe@ZnS quantum dots （QDs） electrochemiluminescence （ECL） via TiO2 nanoparticles （TiO2 NPs） and the outstanding quencher of polydopam...In this work, a double signal amplified immunosen- sor based on the enhanced CdSe@ZnS quantum dots （QDs） electrochemiluminescence （ECL） via TiO2 nanoparticles （TiO2 NPs） and the outstanding quencher of polydopamine （PDA） decorated Au nanoparticles （Au@PDA NPs） for ultrasensitive detection of carcinoembryonic antigen （CEA） has been successfully achieved. The ECL of CdSe@ZnS QDs with different sizes has been investigated carefully, especially cooperation with TiO2 NPs. Au@PDA NPs have been synthesized and characterized by transmission electron microscopy （TEM） and UV-Vis spectrum, which acted as ECL quenchers to label the secondary antibody （Ab2） of CEA to form Ab2/Au@PDA NPs conjugates. The sandwich-structured immunosensor was formed between capture antibody （Abl） on CdSe@ZnS QDs/TiO2 NPs/glassy carbon electrode, CEA and Ab2/Au@PDA NPs conjugates, resulting in a proportional ECL quenching signal relevant to the CEA concentration. Thus, CEA as a model biomarker has been detected in the linear range from 0.001 to 100 ng mL^-1 with a limit of detection of 0.35 pg mL^-1 （S/N = 3）.展开更多
基金supported by the National Key R&D Program of China(2017YFA0700102)the National Natural Science Foundation of China(21573222 and 91545202)+1 种基金the Outstanding Youth Talent Project of Dalian(2017RJ03)the DMTO Project of Dalian Institute of Chemical Physics,CAS(DICP DMTO201702),the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020200),the Youth Innovation Promotion Association,CAS(2015145)~~
文摘Electrochemical CO2 reduction reaction(CO2RR)powered by renewable electricity has emerged as the most promising technique for CO2 conversion,making it possible to realize a carbon‐neutral cycle.Highly efficient,robust,and cost‐effective catalysts are highly demanded for the near‐future practical applications of CO2RR.Previous studies on atomically dispersed metal‐nitrogen(M‐Nx)sites constituted of earth abundant elements with maximum atom‐utilization efficiency have demonstrated their performance towards CO2RR.This review summarizes recent advances on a variety of M‐Nx sites‐containing transition metal‐centered macrocyclic complexes,metal organic frameworks,and M‐Nx‐doped carbon materials for efficient CO2RR,including both experimental and theoretical studies.The roles of metal centers,coordinated ligands,and conductive supports on the intrinsic activity and selectivity,together with the importance of reaction conditions for improved performance are discussed.The mechanisms of CO2RR over these M‐Nx‐containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO2RR.
基金supported by the National Natural Science Foundation of China (21575022, 21535003)the National High Technology Research and Development Program of China (2015AA020502)+1 种基金the Open Research Fund of Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, Southeast Universitythe Fundamental Research Funds for the Central Universities (KYLX15-0127)
文摘In this work, a double signal amplified immunosen- sor based on the enhanced CdSe@ZnS quantum dots （QDs） electrochemiluminescence （ECL） via TiO2 nanoparticles （TiO2 NPs） and the outstanding quencher of polydopamine （PDA） decorated Au nanoparticles （Au@PDA NPs） for ultrasensitive detection of carcinoembryonic antigen （CEA） has been successfully achieved. The ECL of CdSe@ZnS QDs with different sizes has been investigated carefully, especially cooperation with TiO2 NPs. Au@PDA NPs have been synthesized and characterized by transmission electron microscopy （TEM） and UV-Vis spectrum, which acted as ECL quenchers to label the secondary antibody （Ab2） of CEA to form Ab2/Au@PDA NPs conjugates. The sandwich-structured immunosensor was formed between capture antibody （Abl） on CdSe@ZnS QDs/TiO2 NPs/glassy carbon electrode, CEA and Ab2/Au@PDA NPs conjugates, resulting in a proportional ECL quenching signal relevant to the CEA concentration. Thus, CEA as a model biomarker has been detected in the linear range from 0.001 to 100 ng mL^-1 with a limit of detection of 0.35 pg mL^-1 （S/N = 3）.
