Developing efficient and stable catalysts for the electrocatalytic N_(2)reduction reaction(NRR)shows promise in nitrogen fixation.Here,we proposed active and stable single-atom catalysts(SACs)toward NRR,where transiti...Developing efficient and stable catalysts for the electrocatalytic N_(2)reduction reaction(NRR)shows promise in nitrogen fixation.Here,we proposed active and stable single-atom catalysts(SACs)toward NRR,where transition metals are anchored on nitrogenated carbon nanotubes(NCNTs).Among the screened nine common transition metals(Ti,V,Cr,Mn,Fe,Mo,Ru,Rh,and Ag)on(4,4)NCNTs,we found Mo-NCNT possesses the most excellent NRR catalytic activity and selectivity with a low overpotential of 0.29 V.Then,the NRR performance of Mo-NCNT was further engineered by controlling the nanotube diameter,where the lowest overpotential is 0.18 V at a diameter of 9.6Å.In addition,we found a linear scaling relation between*NNH and*NH_(2)on the studied catalysts with the exception of(2,2)and(3,3)Mo-NCNTs,owing to their extremely unstable structures.We attribute the outstanding NRR performance of Mo-NCNT to the moderate adsorption of N_(2)due to the slightly low d-band center of Mo,and the charge donating and accepting capacity of NCNTs.This work has provided a deeper insight into designing highefficiency and stable NRR SACs supported by NCNTs.展开更多
Development of biocompatible hydrogel adhesives with robust tissue adhesion to realize instant hemorrhage control and injury sealing,especially for emergency rescue and tissue repair,is still challenging.Herein,we rep...Development of biocompatible hydrogel adhesives with robust tissue adhesion to realize instant hemorrhage control and injury sealing,especially for emergency rescue and tissue repair,is still challenging.Herein,we report a potent hydrogel adhesive by free radical polymerization of N-acryloyl aspartic acid(AASP)in a facile and straightforward way.Through delicate adjustment of steric hindrance,the synergistic effect between interface interactions and cohesion energy can be achieved in PAASP hydrogel verified by X-ray photoelectron spectroscopy(XPS)analysis and simulation calculation compared to poly(N-acryloyl glutamic acid)(PAGLU)and poly(N-acryloyl amidomalonic acid)(PAAMI)hydrogels.The adhesion strength of the PAASP hydrogel could reach 120 kPa to firmly seal the broken organs to withstand the external force with persistent stability under physiological conditions,and rapid hemostasis in different hemorrhage models on mice is achieved using PAASP hydrogel as physical barrier.Furthermore,the paper-based Fe^(3+)transfer printing method is applied to construct PAASP-based Janus hydrogel patch with both adhesive and non-adhesive surfaces,by which simultaneous wound healing and postoperative anti-adhesion can be realized in gastric perforation model on mice.This advanced hydrogel may show vast potential as bio-adhesives for emergency rescue and tissue/organ repair.展开更多
基金supported by the National Natural Science Foundation of China (52273081, 52202295, and 51973171)Fundamental Research Funds for the Central Universities (xhj032021008-02)+1 种基金Chang Huang at the Instrument Analysis Center of Xi’an Jiaotong University for assistance with SEM and XRDthe “Young Talent Support Plan” of Xi’an Jiaotong University。
基金This work is financially supported by the National Natural Science Foundation of China(No.22103059)Y.S.acknowledges the“Young Talent Support Plan”of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University No.202018)Supercomputing facilities were provided by Hefei Advanced Computing Center.
文摘Developing efficient and stable catalysts for the electrocatalytic N_(2)reduction reaction(NRR)shows promise in nitrogen fixation.Here,we proposed active and stable single-atom catalysts(SACs)toward NRR,where transition metals are anchored on nitrogenated carbon nanotubes(NCNTs).Among the screened nine common transition metals(Ti,V,Cr,Mn,Fe,Mo,Ru,Rh,and Ag)on(4,4)NCNTs,we found Mo-NCNT possesses the most excellent NRR catalytic activity and selectivity with a low overpotential of 0.29 V.Then,the NRR performance of Mo-NCNT was further engineered by controlling the nanotube diameter,where the lowest overpotential is 0.18 V at a diameter of 9.6Å.In addition,we found a linear scaling relation between*NNH and*NH_(2)on the studied catalysts with the exception of(2,2)and(3,3)Mo-NCNTs,owing to their extremely unstable structures.We attribute the outstanding NRR performance of Mo-NCNT to the moderate adsorption of N_(2)due to the slightly low d-band center of Mo,and the charge donating and accepting capacity of NCNTs.This work has provided a deeper insight into designing highefficiency and stable NRR SACs supported by NCNTs.
基金the National Natural Science Foundation of China(NSFC 52173139)the Shaanxi International Science and Technology Cooperation Program Project(2020KW-062)+1 种基金the“Young Talent Support Plan”of Xi’an Jiaotong University,and Fundamental Research Funds for the Central Universities(xzy022021040)supported by the Opening Research Fund from Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research,College of Stomatology,Xi’an Jiaotong University(2021LHM-KFKT003).
文摘Development of biocompatible hydrogel adhesives with robust tissue adhesion to realize instant hemorrhage control and injury sealing,especially for emergency rescue and tissue repair,is still challenging.Herein,we report a potent hydrogel adhesive by free radical polymerization of N-acryloyl aspartic acid(AASP)in a facile and straightforward way.Through delicate adjustment of steric hindrance,the synergistic effect between interface interactions and cohesion energy can be achieved in PAASP hydrogel verified by X-ray photoelectron spectroscopy(XPS)analysis and simulation calculation compared to poly(N-acryloyl glutamic acid)(PAGLU)and poly(N-acryloyl amidomalonic acid)(PAAMI)hydrogels.The adhesion strength of the PAASP hydrogel could reach 120 kPa to firmly seal the broken organs to withstand the external force with persistent stability under physiological conditions,and rapid hemostasis in different hemorrhage models on mice is achieved using PAASP hydrogel as physical barrier.Furthermore,the paper-based Fe^(3+)transfer printing method is applied to construct PAASP-based Janus hydrogel patch with both adhesive and non-adhesive surfaces,by which simultaneous wound healing and postoperative anti-adhesion can be realized in gastric perforation model on mice.This advanced hydrogel may show vast potential as bio-adhesives for emergency rescue and tissue/organ repair.
