The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of ...The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.展开更多
Efficiently reducing carbon dioxide(CO_(2))into carbon chemicals and fuels is highly desirable due to the rapid growth of atmospheric CO_(2)ncentration.In prior work,we described a unique H/CO_(2)fuel cell driven by l...Efficiently reducing carbon dioxide(CO_(2))into carbon chemicals and fuels is highly desirable due to the rapid growth of atmospheric CO_(2)ncentration.In prior work,we described a unique H/CO_(2)fuel cell driven by low-valued waste heat,which not only CO_(2)nverts CO_(2)to methane(CH_(4))but also outputs electrical energy,yet the CO_(2)reduction rate needs to be urgently improved.Here,a novel Ru-RuOcatalyst with heterostructure was grafted on mesoporous carbon spheres by in situ partially reducing RuOinto ultrasmall Ru clusters(~1 nm),in which heteroatom-doped carbon spheres as a matrix with excellent CO_(2)nductivity and abundant pores can not only easily CO_(2)nfine the formation of Ru nanocluster but also are beneficial to the exposed active sites of Ru CO_(2)mplex and the mass transport.CO_(2)mpared to pure RuOnanoparticles supported on carbon spheres,our CO_(2)mposite catalyst boosts the CO_(2) nversion rate by more than 5-fold,reaching a value of 382.7μmol gcat.h-1at 170℃.Moreover,a decent output power density of 2.92 W mwas obtained from this H2/CO_(2)fuel cell using Ru-RuOembedded carbon spheres as a cathode catalyst.The Ru-RuOheterostructure can modify the adsorption energy of CO_(2)and induce the redistribution of charge density,thus boosting CO_(2)reduction significantly.This work not only offers an efficient catalyst for this novel H_(2)/CO_(2)fuel cell but also presents a facile method to prepare Ru nanoclusters.展开更多
Mesoporous SiO_2 microspheres were synthesized using the sol-gel method and were characterized by TEM, FT-IR and BET techniques. The diameter of the microspheres is about 100—150 nm, and the average mesopore diameter...Mesoporous SiO_2 microspheres were synthesized using the sol-gel method and were characterized by TEM, FT-IR and BET techniques. The diameter of the microspheres is about 100—150 nm, and the average mesopore diameter is 2.55 nm, while the specific surface area is 1 088.9 m2/g. Mesoporous SiO_2 microspheres adsorb glutaraldehyde and immobilize laccase by means of the aldehyde group in glutaral which can react with the amidogen of laccase. The immobilization conditions were optimized at a glutaraldehyde concentration of 0.75%, a crosslinking time of 8 h, a laccase concentration of 0.04 L/L and an immobilization time of 10 h. When diesel leakage concentration was 80 mg/L, the highest corrosion inhibition efficiency of immobilized laccase reached 49.23%, which was slightly lower than the corrosion inhibition efficiency of free laccase(59%). The diesel degradation ratio could reach up to 45%. It has been proved that the immobilized laccase could degrade diesel to inhibit corrosion.展开更多
基金supported by the National Natural Science Foundation of China (21972124, 22272148)the Priority Academic Program Development of Jiangsu Higher Education Institution。
文摘The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.
基金financially supported by the Natural Science Foundation of Shaanxi Provincial(2021JQ-034)Chongqing University Key Laboratory of Micro/Nano Materials Engineering and Technology(KFJJ2012)by University Joint Project of Shaanxi Province(2021GXLH-Z-067)。
文摘Efficiently reducing carbon dioxide(CO_(2))into carbon chemicals and fuels is highly desirable due to the rapid growth of atmospheric CO_(2)ncentration.In prior work,we described a unique H/CO_(2)fuel cell driven by low-valued waste heat,which not only CO_(2)nverts CO_(2)to methane(CH_(4))but also outputs electrical energy,yet the CO_(2)reduction rate needs to be urgently improved.Here,a novel Ru-RuOcatalyst with heterostructure was grafted on mesoporous carbon spheres by in situ partially reducing RuOinto ultrasmall Ru clusters(~1 nm),in which heteroatom-doped carbon spheres as a matrix with excellent CO_(2)nductivity and abundant pores can not only easily CO_(2)nfine the formation of Ru nanocluster but also are beneficial to the exposed active sites of Ru CO_(2)mplex and the mass transport.CO_(2)mpared to pure RuOnanoparticles supported on carbon spheres,our CO_(2)mposite catalyst boosts the CO_(2) nversion rate by more than 5-fold,reaching a value of 382.7μmol gcat.h-1at 170℃.Moreover,a decent output power density of 2.92 W mwas obtained from this H2/CO_(2)fuel cell using Ru-RuOembedded carbon spheres as a cathode catalyst.The Ru-RuOheterostructure can modify the adsorption energy of CO_(2)and induce the redistribution of charge density,thus boosting CO_(2)reduction significantly.This work not only offers an efficient catalyst for this novel H_(2)/CO_(2)fuel cell but also presents a facile method to prepare Ru nanoclusters.
基金supported by the Foundation for Top Talents Program of China University of Petroleum
文摘Mesoporous SiO_2 microspheres were synthesized using the sol-gel method and were characterized by TEM, FT-IR and BET techniques. The diameter of the microspheres is about 100—150 nm, and the average mesopore diameter is 2.55 nm, while the specific surface area is 1 088.9 m2/g. Mesoporous SiO_2 microspheres adsorb glutaraldehyde and immobilize laccase by means of the aldehyde group in glutaral which can react with the amidogen of laccase. The immobilization conditions were optimized at a glutaraldehyde concentration of 0.75%, a crosslinking time of 8 h, a laccase concentration of 0.04 L/L and an immobilization time of 10 h. When diesel leakage concentration was 80 mg/L, the highest corrosion inhibition efficiency of immobilized laccase reached 49.23%, which was slightly lower than the corrosion inhibition efficiency of free laccase(59%). The diesel degradation ratio could reach up to 45%. It has been proved that the immobilized laccase could degrade diesel to inhibit corrosion.
