Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footpri...Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footprint,there has been increasing interest in CO_(2)/CO conversion on MBenes,but mostly focused on C_(1)products.C^(2+)chemicals generally possess higher energy densities and wider applications than C_(1)counterparts.However,C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process.Here,we explore electrochemical CO reduction reaction to C_(2)chemicals on Mo_(2)B_(2)O_(2)MBene via density-functional theory calculations.Remarkably,the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process,making Mo_(2)B_(2)O_(2)an efficient catalyst for C–C coupling.Among C_(1)and C_(2)chemicals,ethanol is predicted to be the primary product.Furthermore,by charge and bond analysis,it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate*COH than other C_(1)intermediates,which is responsible for the facile C–C coupling.From an atomic scale,this work provides microscopic insight into C–C coupling process and suggests Mo_(2)B_(2)O_(2)a promising catalyst for electrochemical CO reduction to C_(2)chemicals.展开更多
Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electr...Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.展开更多
Oxidative stress has been considered as a major cause of cellular injuries in a variety of clinical abnormalities, especially prominent in neural diseases. One of the usable ways to prevent the reactive oxygen species...Oxidative stress has been considered as a major cause of cellular injuries in a variety of clinical abnormalities, especially prominent in neural diseases. One of the usable ways to prevent the reactive oxygen species (ROS)-mediated cellular injury is dietary or pharmaceutical augmentation of some free radical scavenger. Water-soluble amino-fullerene is a novel compound that behaves as a free radical scavenger with excellent biology consistent. In the present study, we have synthesized and characterized a novel cystine C60 derivative for the first time, and investigated the effects on hydrogen peroxide-induced oxidative stress and apoptotic death in cultured rat pheochromocytoma (PC12) cells. PC12 cells treated with hydrogen peroxide underwent apoptotic death as determined by MTT, PI/Hoechst 33342 staining and flow cytometry analysis. These results suggested that cystine C60 derivative has the potential to prevent oxidative stress-induced cell death and has no evident toxicity.展开更多
基金the A*STAR LCER-FI project(LCERFI01-0033 U2102d2006)the Ministry of Education of Singapore and the National University of Singapore(C-261-000-207-532/C-261-000-777-532 and R-279-000-574-114)for financial support.
文摘Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footprint,there has been increasing interest in CO_(2)/CO conversion on MBenes,but mostly focused on C_(1)products.C^(2+)chemicals generally possess higher energy densities and wider applications than C_(1)counterparts.However,C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process.Here,we explore electrochemical CO reduction reaction to C_(2)chemicals on Mo_(2)B_(2)O_(2)MBene via density-functional theory calculations.Remarkably,the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process,making Mo_(2)B_(2)O_(2)an efficient catalyst for C–C coupling.Among C_(1)and C_(2)chemicals,ethanol is predicted to be the primary product.Furthermore,by charge and bond analysis,it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate*COH than other C_(1)intermediates,which is responsible for the facile C–C coupling.From an atomic scale,this work provides microscopic insight into C–C coupling process and suggests Mo_(2)B_(2)O_(2)a promising catalyst for electrochemical CO reduction to C_(2)chemicals.
基金This work was supported by the University of Science and Technology Beijing.DG acknowledges the financial support from 111 Project(no.B170003)Foshan Science and Technology Innovation Project(no.2018IT100363).
文摘Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.
文摘Oxidative stress has been considered as a major cause of cellular injuries in a variety of clinical abnormalities, especially prominent in neural diseases. One of the usable ways to prevent the reactive oxygen species (ROS)-mediated cellular injury is dietary or pharmaceutical augmentation of some free radical scavenger. Water-soluble amino-fullerene is a novel compound that behaves as a free radical scavenger with excellent biology consistent. In the present study, we have synthesized and characterized a novel cystine C60 derivative for the first time, and investigated the effects on hydrogen peroxide-induced oxidative stress and apoptotic death in cultured rat pheochromocytoma (PC12) cells. PC12 cells treated with hydrogen peroxide underwent apoptotic death as determined by MTT, PI/Hoechst 33342 staining and flow cytometry analysis. These results suggested that cystine C60 derivative has the potential to prevent oxidative stress-induced cell death and has no evident toxicity.
