Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined su...Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined superfluid" (QSF). This ordered ultrafast flow in the confined channel can be considered as "quantum tunneling fluid effect" with a "tunneling distance", which is corresponding to the period of QSF. Recent research demonstrated that artificial biomimetic nanochannels also showed the phenomenon of QSF, such as ion and water channels. The introduction of QSF concept in the fields of chemistry and biology may create significant impact. As for chemistry, the QSF effect provides new ideas for accurate synthesis in organic, inorganic, polymer, etc. We believe the implementation of the idea of QSF will promote the development of QSF biochemistry, biophysics, bioinformatics and biomedical science.展开更多
Metal-organic radicals are reactive and transient because of the existence of unpaired valence electrons,and thus the characterization of these open-shell systems is challenging.In our work,the radicals are synthesize...Metal-organic radicals are reactive and transient because of the existence of unpaired valence electrons,and thus the characterization of these open-shell systems is challenging.In our work,the radicals are synthesized by the reaction of bare metal atoms and organic ligands in a laser-vaporization supersonic molecular beam source and characterized with pulsed-field ionization zero electron kinetic energy(ZEKE) spectroscopy.The molecular beam ZEKE technique routinely yields sub-meV spectral resolution and is a powerful means to study the molecular bonding and structures.This account presents several examples of single-photon ZEKE spectroscopic applications in determining metal binding modes and molecular conformations.展开更多
In this review a series of organic-based open porous networks are discussed, in which hydrogen bonds play an important role in network formation. Using these open networks as molecular templates: 1) a wealth of functi...In this review a series of organic-based open porous networks are discussed, in which hydrogen bonds play an important role in network formation. Using these open networks as molecular templates: 1) a wealth of functional guest species can be immo- bilized; 2) fullerene molecules can be separated and recognized; 3) photoisomerization reactions can be observed by STM; 4) 1D molecular arrays can be constructed; and 5) heterogeneous bilayer structures can be formed. It is envisioned that these su- pramolecular networks might be developed into a new family of useful soft frameworks for studies toward shape-selective ca- talysis, molecular recognition and host-guest supramolecular chemistry.展开更多
The self-assembled phospholipid-or cytosolassociated multienzyme complexes constitute necessary components of the foundation of life.As a proof of concept,metalcoordinated supramolecular nanogels (MCSGs) have been des...The self-assembled phospholipid-or cytosolassociated multienzyme complexes constitute necessary components of the foundation of life.As a proof of concept,metalcoordinated supramolecular nanogels (MCSGs) have been designed,with the self-assembly of di-lysine coordinated iron(Fe(Lys)_(2))-functionalized peptide gelators on the interface by an in situ amidation-induced protonation process.The monoatomic and highly dispersed active centers of Fe(Lys)_(2) offered the nanogel mimics with excellent reaction rates due to the high density and nano compartmental structure similar to the natural matrix-associated multienzyme complex.SiO_(2)@MCSGs show both superoxide dismutase (SOD) activity and peroxidase (POD) activity,and the higher activities compared with the activity of free Fe(Lys);molecules can be detected.After loading the substrate 2,2'-azinobis-(3-ethylbenzthiazoline-6-sulphonate)(ABTS),SiO_(2)@MCSGs;can responsively convert O^(-)_(2) in the tumor microenvironment into H_(2)O_(2) intermediates and then tandem catalyze the oxidization of ABTS for contrast photoacoustic (PA) imaging of tumor by the SOD-POD mimic activity,showing their great potential as the efficient enzymatic agents for pathological theranostics.展开更多
基金supported by the National Key R&D Program of China(2017YFA0206900)the National Natural Science Foundation of China(21625303)
文摘Biological ion channels show that ultrafast ions and molecules transmission are in a quantum way of single molecular or ionic chain with a certain number of molecules or ions, and we define it as "quantum-confined superfluid" (QSF). This ordered ultrafast flow in the confined channel can be considered as "quantum tunneling fluid effect" with a "tunneling distance", which is corresponding to the period of QSF. Recent research demonstrated that artificial biomimetic nanochannels also showed the phenomenon of QSF, such as ion and water channels. The introduction of QSF concept in the fields of chemistry and biology may create significant impact. As for chemistry, the QSF effect provides new ideas for accurate synthesis in organic, inorganic, polymer, etc. We believe the implementation of the idea of QSF will promote the development of QSF biochemistry, biophysics, bioinformatics and biomedical science.
基金the financial support from the Chemistry Division of the National Science Foundationdonors of the Petroleum Research Fund of the American Chemical SocietyKentucky Science and Engineering Foundation
文摘Metal-organic radicals are reactive and transient because of the existence of unpaired valence electrons,and thus the characterization of these open-shell systems is challenging.In our work,the radicals are synthesized by the reaction of bare metal atoms and organic ligands in a laser-vaporization supersonic molecular beam source and characterized with pulsed-field ionization zero electron kinetic energy(ZEKE) spectroscopy.The molecular beam ZEKE technique routinely yields sub-meV spectral resolution and is a powerful means to study the molecular bonding and structures.This account presents several examples of single-photon ZEKE spectroscopic applications in determining metal binding modes and molecular conformations.
文摘In this review a series of organic-based open porous networks are discussed, in which hydrogen bonds play an important role in network formation. Using these open networks as molecular templates: 1) a wealth of functional guest species can be immo- bilized; 2) fullerene molecules can be separated and recognized; 3) photoisomerization reactions can be observed by STM; 4) 1D molecular arrays can be constructed; and 5) heterogeneous bilayer structures can be formed. It is envisioned that these su- pramolecular networks might be developed into a new family of useful soft frameworks for studies toward shape-selective ca- talysis, molecular recognition and host-guest supramolecular chemistry.
基金supported by the National Natural Science Foundation of China (51773155 and 51873156)the National Key Research and Development Program (2016YFA0100800 and 2018YFC1803100)。
文摘The self-assembled phospholipid-or cytosolassociated multienzyme complexes constitute necessary components of the foundation of life.As a proof of concept,metalcoordinated supramolecular nanogels (MCSGs) have been designed,with the self-assembly of di-lysine coordinated iron(Fe(Lys)_(2))-functionalized peptide gelators on the interface by an in situ amidation-induced protonation process.The monoatomic and highly dispersed active centers of Fe(Lys)_(2) offered the nanogel mimics with excellent reaction rates due to the high density and nano compartmental structure similar to the natural matrix-associated multienzyme complex.SiO_(2)@MCSGs show both superoxide dismutase (SOD) activity and peroxidase (POD) activity,and the higher activities compared with the activity of free Fe(Lys);molecules can be detected.After loading the substrate 2,2'-azinobis-(3-ethylbenzthiazoline-6-sulphonate)(ABTS),SiO_(2)@MCSGs;can responsively convert O^(-)_(2) in the tumor microenvironment into H_(2)O_(2) intermediates and then tandem catalyze the oxidization of ABTS for contrast photoacoustic (PA) imaging of tumor by the SOD-POD mimic activity,showing their great potential as the efficient enzymatic agents for pathological theranostics.