Hydrogenation modification is one of the most important ways to produce high-quality petroleum resin. The col- orless C9 petroleum resin （CgPR） was obtained by two-stage catalytic hydrogenation over NiWS/？-A1203 ca...Hydrogenation modification is one of the most important ways to produce high-quality petroleum resin. The col- orless C9 petroleum resin （CgPR） was obtained by two-stage catalytic hydrogenation over NiWS/？-A1203 catalyst and PdRu/ y-A1203 catalyst connected in series. Via the hydrogenation reaction, aromatic rings in C9PR were converted to alicyclic rings, and its color was reduced from Gardner color grade No. 11 to Gardner color grade No. 0. The optimum Ni/W atomic ratio was found to be close to 0.23, while the optimum Pd/Ru atomic ratio was close to 3.80. The TEM results showed that the morphology and size of sulfide or metal particles of the two kinds of catalysts remained almost unchanged after the reac- tion was carried our for 1 204 hours, attesting to their good catalytic stability.展开更多
The hydrogen evolution reaction(HER)in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production.Herein,we employ...The hydrogen evolution reaction(HER)in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production.Herein,we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H_(Inc)-PdRu electrocatalyst,thereby modulating its electronic structure and enhancing its alkaline HER performance.We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity,achieving a remarkably low overpotential of 25 mV at 10 mA cm^(-2)compared with the Pd,Ru and PdRu catalysts while maintaining robust catalyst stability.Operando spectroscopic analysis indicates that H insertion into the H_(Inc)-PdRu electrocatalyst enhances the availability of H_(2)O^(*)at the surface,promoting water dissociation at the active sites.Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices,effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics.This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.展开更多
Fluorinated organic compounds are of great importance to modern industries,while their release to the environment is inevitable,causing extreme environmental pollution and the subsequent hazardous effect on ecosystems...Fluorinated organic compounds are of great importance to modern industries,while their release to the environment is inevitable,causing extreme environmental pollution and the subsequent hazardous effect on ecosystems.This is because the degradation of fluorinated compounds under mild conditions remains a challenging task due to the strong C-F bond strength.In this study,we report preparation of PdRu@MIL-101 through immobilizing ultrafine PdRu alloy nanoparticles with a mean diameter of∼2 nminto the metal-organic framework(MOF),MIL-101(Cr),which was highly active and stable in the hydrodefluorination of 4-fluorophenol(4-FP)under mild aqueous conditions.The optimized catalyst Pd0.5Ru0.5@MIL-101 achieved impressive hydrogenation performance with a 98.5% conversion of 4-FP and a 97.7% selectivity of cyclohexanol,much better than the single metal-doped Pd@MIL-101 and Ru@MIL-101 catalysts.The excellent catalytic behavior contributed to the synergistic effect of combining the PdRu alloying effect and the MOF nanospace confinement effect,providing a promising strategy to develop highly efficient hydrodefluorination catalysts to assist environmental restoration and green ecology.展开更多
基金financially supported by the Scientific Research Fund of Zhejiang Provincial Education Department (Y201018517)
文摘Hydrogenation modification is one of the most important ways to produce high-quality petroleum resin. The col- orless C9 petroleum resin （CgPR） was obtained by two-stage catalytic hydrogenation over NiWS/？-A1203 catalyst and PdRu/ y-A1203 catalyst connected in series. Via the hydrogenation reaction, aromatic rings in C9PR were converted to alicyclic rings, and its color was reduced from Gardner color grade No. 11 to Gardner color grade No. 0. The optimum Ni/W atomic ratio was found to be close to 0.23, while the optimum Pd/Ru atomic ratio was close to 3.80. The TEM results showed that the morphology and size of sulfide or metal particles of the two kinds of catalysts remained almost unchanged after the reac- tion was carried our for 1 204 hours, attesting to their good catalytic stability.
文摘The hydrogen evolution reaction(HER)in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production.Herein,we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H_(Inc)-PdRu electrocatalyst,thereby modulating its electronic structure and enhancing its alkaline HER performance.We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity,achieving a remarkably low overpotential of 25 mV at 10 mA cm^(-2)compared with the Pd,Ru and PdRu catalysts while maintaining robust catalyst stability.Operando spectroscopic analysis indicates that H insertion into the H_(Inc)-PdRu electrocatalyst enhances the availability of H_(2)O^(*)at the surface,promoting water dissociation at the active sites.Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices,effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics.This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.
基金supported by the National Key R&D Program of China(no.2018YFA0108300)the Overseas High-level Talents Plan of China and Guangdong Province,the Fundamental Research Funds for the Central Universities+2 种基金the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(no.2017Z T07C069)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(no.2017BT01C161)the NSFC Projects(nos.22075321,21821003,21890380,and 21905315).
文摘Fluorinated organic compounds are of great importance to modern industries,while their release to the environment is inevitable,causing extreme environmental pollution and the subsequent hazardous effect on ecosystems.This is because the degradation of fluorinated compounds under mild conditions remains a challenging task due to the strong C-F bond strength.In this study,we report preparation of PdRu@MIL-101 through immobilizing ultrafine PdRu alloy nanoparticles with a mean diameter of∼2 nminto the metal-organic framework(MOF),MIL-101(Cr),which was highly active and stable in the hydrodefluorination of 4-fluorophenol(4-FP)under mild aqueous conditions.The optimized catalyst Pd0.5Ru0.5@MIL-101 achieved impressive hydrogenation performance with a 98.5% conversion of 4-FP and a 97.7% selectivity of cyclohexanol,much better than the single metal-doped Pd@MIL-101 and Ru@MIL-101 catalysts.The excellent catalytic behavior contributed to the synergistic effect of combining the PdRu alloying effect and the MOF nanospace confinement effect,providing a promising strategy to develop highly efficient hydrodefluorination catalysts to assist environmental restoration and green ecology.
