The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy goals.This study proposed an atom capture strategy for anchoring dual si...The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy goals.This study proposed an atom capture strategy for anchoring dual single atoms(DSAs)in a zinc-zeolitic imidazolate framework(Zn-ZIF),followed by calcination under an N_(2) atmosphere to synthesize ruthenium-platinum DSAs supported on a nitrogendoped carbon substrate(RuPt DSAs-NC).Theoretical calculations showed that the degree of Ru 5dxz-~*O 2p_x orbital hybridization was high when^(*)O was adsorbed at the Ru site,indicating enhanced covalent hybridization of metal sites and oxygen ligands,which benefited the adsorption of intermediate species.The presence of the RuPtN_6 active center optimized the absorption-desorption behavior of intermediates,improving the electrocatalytic performance of the oxygen reduction reaction(ORR)and the oxygen evolution reaction(DER),RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm^(-2)in an alkaline environment.Furthermore,rechargeable zinc-air batteries(ZABs)achieved a peak power density of 171 MW cm^(-2).The RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip efficiency.This study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocata lytic performance.展开更多
Accelerating beams have been the subject of extensive research in the last few decades because of their selfacceleration and diffraction-free propagation over several Rayleigh lengths.Here,we investigate the propagati...Accelerating beams have been the subject of extensive research in the last few decades because of their selfacceleration and diffraction-free propagation over several Rayleigh lengths.Here,we investigate the propagation dynamics of a Fresnel diffraction beam using the nonlocal nonlinear Schrodinger equation(NNLSE).When a nonlocal nonlinearity is introduced into the linear Schrodinger equation without invoking an external potential,the evolution behaviors of incident Fresnel diffraction beams are modulated regularly,and certain novel phenomena are observed.We show through numerical calculations,under varying degrees of nonlocality,that nonlocality significantly affects the evolution of Fresnel diffraction beams.Further,we briefly discuss the two-dimensional case as the equivalent of the product of two one-dimensional cases.At a critical point,the Airy-like intensity profile oscillates between the first and third quadrants,and the process repeats during propagation to yield an unusual oscillation.Our results are expected to contribute to the understanding of NNLSE and nonlinear optics.展开更多
Lipid nanoparticles(LNPs)have emerged as a powerful platform for RNA delivery;the chemical engineering of LNP for efficient delivery of RNA into cytosol remains critical but challenging.One promising strategy is the u...Lipid nanoparticles(LNPs)have emerged as a powerful platform for RNA delivery;the chemical engineering of LNP for efficient delivery of RNA into cytosol remains critical but challenging.One promising strategy is the use of permanently positively charged lipids,which have been shown to enhance the stability and delivery efficiency of LNPs.However,the resulting strong electrostatic interactions reduced the RNA release capacity from the lipoplexes.Herein,we engineered a hydrogen peroxide(H_(2)O_(2))-triggered charge-altering LNP(CALNP)for efficient small interfering RNA(siRNA)delivery and tumor therapy in mice.The incorporation of phenylboronic acid(PBA)into ionizable lipids generated permanently positively charged lipids.A CALNP with optimal lipid formulations was identified,exhibiting enhanced transfection efficiency with effective lysosomal escape through dual effects of electrostatic interaction and ligand-receptor binding.H_(2)O_(2)-triggered removal of PBA groups regenerated ionizable LNP with reduced positive charges at physiological pH,allowing cell-selective siRNA release in the cytoplasm.Our results demonstrated that CALNPs exhibited improved siRNA transfection and gene silencing efficiency.We also showed potent CALNP activity against the polo-like kinase 1(Plk1)gene by effectively silencing Plk1 mRNA and subsequent suppression of tumor growth.Collectively,these findings highlighted the potential of CALNP as an efficient platform for RNA delivery and tumor therapeutics.展开更多
基金supported by the National Natural Science Foundation of China (No.22309023,22179014)the project of Natural Science Foundation of Chongqing (Grant No.CSTB2022NSCQMSX0270)+3 种基金the China Postdoctoral Science Foundation (No.2022M720593)the youth project of science and technology research program of Chongqing Municipal Education Commission of China (Grant No.KJQN202201127)the Scientific Research Foundation of Chongqing University of Technology (2022ZDZ011,2022PYZ026)the special funding for research projects of Chongqing Human Resources and Social Security Bureau (Grant No.2022CQBSHTB1023)。
文摘The development of redox bifunctional electrocatalysts with high performance,low cost,and long lifetimes is essential for achieving clean energy goals.This study proposed an atom capture strategy for anchoring dual single atoms(DSAs)in a zinc-zeolitic imidazolate framework(Zn-ZIF),followed by calcination under an N_(2) atmosphere to synthesize ruthenium-platinum DSAs supported on a nitrogendoped carbon substrate(RuPt DSAs-NC).Theoretical calculations showed that the degree of Ru 5dxz-~*O 2p_x orbital hybridization was high when^(*)O was adsorbed at the Ru site,indicating enhanced covalent hybridization of metal sites and oxygen ligands,which benefited the adsorption of intermediate species.The presence of the RuPtN_6 active center optimized the absorption-desorption behavior of intermediates,improving the electrocatalytic performance of the oxygen reduction reaction(ORR)and the oxygen evolution reaction(DER),RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm^(-2)in an alkaline environment.Furthermore,rechargeable zinc-air batteries(ZABs)achieved a peak power density of 171 MW cm^(-2).The RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip efficiency.This study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocata lytic performance.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61805068,61875053,and 62074127)China Postdoctoral Science Foundation(Grant No.2017M620300)the Fund from the Science and Technology Department of Henan Province,China(Grant No.202102210111).
文摘Accelerating beams have been the subject of extensive research in the last few decades because of their selfacceleration and diffraction-free propagation over several Rayleigh lengths.Here,we investigate the propagation dynamics of a Fresnel diffraction beam using the nonlocal nonlinear Schrodinger equation(NNLSE).When a nonlocal nonlinearity is introduced into the linear Schrodinger equation without invoking an external potential,the evolution behaviors of incident Fresnel diffraction beams are modulated regularly,and certain novel phenomena are observed.We show through numerical calculations,under varying degrees of nonlocality,that nonlocality significantly affects the evolution of Fresnel diffraction beams.Further,we briefly discuss the two-dimensional case as the equivalent of the product of two one-dimensional cases.At a critical point,the Airy-like intensity profile oscillates between the first and third quadrants,and the process repeats during propagation to yield an unusual oscillation.Our results are expected to contribute to the understanding of NNLSE and nonlinear optics.
基金supported by the National Natural Science Foundation of China(grant nos.22174043,21904036,and 22090050)the National Key Research Program(grant nos.2019YFA0905800 and 2018YFA0902300)the Science and Technology Major Project of Hunan Province(grant no.2021SK1020).
文摘Lipid nanoparticles(LNPs)have emerged as a powerful platform for RNA delivery;the chemical engineering of LNP for efficient delivery of RNA into cytosol remains critical but challenging.One promising strategy is the use of permanently positively charged lipids,which have been shown to enhance the stability and delivery efficiency of LNPs.However,the resulting strong electrostatic interactions reduced the RNA release capacity from the lipoplexes.Herein,we engineered a hydrogen peroxide(H_(2)O_(2))-triggered charge-altering LNP(CALNP)for efficient small interfering RNA(siRNA)delivery and tumor therapy in mice.The incorporation of phenylboronic acid(PBA)into ionizable lipids generated permanently positively charged lipids.A CALNP with optimal lipid formulations was identified,exhibiting enhanced transfection efficiency with effective lysosomal escape through dual effects of electrostatic interaction and ligand-receptor binding.H_(2)O_(2)-triggered removal of PBA groups regenerated ionizable LNP with reduced positive charges at physiological pH,allowing cell-selective siRNA release in the cytoplasm.Our results demonstrated that CALNPs exhibited improved siRNA transfection and gene silencing efficiency.We also showed potent CALNP activity against the polo-like kinase 1(Plk1)gene by effectively silencing Plk1 mRNA and subsequent suppression of tumor growth.Collectively,these findings highlighted the potential of CALNP as an efficient platform for RNA delivery and tumor therapeutics.
