To search the new effective nitrogen reduction reaction(NRR)electrocatalyst is very important for the ammonia-based industry.Herein,we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-va...To search the new effective nitrogen reduction reaction(NRR)electrocatalyst is very important for the ammonia-based industry.Herein,we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-vacancy TiO2(Ru/TiO2-Vo).Structural characterizations revealed that oxygen vacancy was loaded in the matrix of Ru/TiO2-Vo.Electrocatalytic results indicated that Ru/TiO2-Vo showed good NRR performance(2.11μg h^-1 cm^-2).Contrast tests showed that NRR property of Ru/TiO2-Vo was much better than those of Ru/TiO-12(B)(0.53μg hcm^-2)and Ru/P25(0.42μg h^-1 cm^-2).Furthermore,density functional theory calculation results indicated catalytic mechanism of NRR and rate-determining step(*N2+1/2 H2→*N+*NH)was the potential-determining step with the overpotential requirement of 0.21 V.A combination of electronic structure analysis and catalytic measurement shed light on the synergistic effect of Ru and oxygen vacancy on the NRR performance.展开更多
Research on water-splitting electrocatalysts is crucial to establishing a solution to the energy crisis.Herein,we report a facile bottom-up strategy for the preparation of high performance supported electrocatalysts f...Research on water-splitting electrocatalysts is crucial to establishing a solution to the energy crisis.Herein,we report a facile bottom-up strategy for the preparation of high performance supported electrocatalysts for overall water-splitting reaction via a rationally designed defect covalent triazine frameworks(CTFs)support.Specifically,defect CTFs are obtained via binary-precursor polymerization,followed by loading Ru nanoparticles(Ru/D-CTFs-900)with high HER performance at a current density of 10 mA cm-2.The overpotential is only 17 mV.Calcination of the resultant Ru–RuO2/D-CTFs-300 in air,produces excellent OER performance with 190 mV overpotential(at 10 mA cm-2).Furthermore,overall water splitting measurements reveal the potential of 1.47 V,which is better than the majority of the reported Ru-based catalysts.Moreover,density functional theory calculation results show that excellent electrocatalytic properties are attributed to the synergistic effect of Ru nanoparticles and carbon support.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21671172,21625604,21776251,21706229and Z86101001)Zhejiang Provincial Natural Science Foundation(No.LR19B010001)
文摘To search the new effective nitrogen reduction reaction(NRR)electrocatalyst is very important for the ammonia-based industry.Herein,we reported the design of a novel NRR electrocatalyst with Ru NPs loaded on oxygen-vacancy TiO2(Ru/TiO2-Vo).Structural characterizations revealed that oxygen vacancy was loaded in the matrix of Ru/TiO2-Vo.Electrocatalytic results indicated that Ru/TiO2-Vo showed good NRR performance(2.11μg h^-1 cm^-2).Contrast tests showed that NRR property of Ru/TiO2-Vo was much better than those of Ru/TiO-12(B)(0.53μg hcm^-2)and Ru/P25(0.42μg h^-1 cm^-2).Furthermore,density functional theory calculation results indicated catalytic mechanism of NRR and rate-determining step(*N2+1/2 H2→*N+*NH)was the potential-determining step with the overpotential requirement of 0.21 V.A combination of electronic structure analysis and catalytic measurement shed light on the synergistic effect of Ru and oxygen vacancy on the NRR performance.
基金National Natural Science Foundation of China(Grant nos.21671172,21625604,21706229,21776251)Zhejiang Provincial Natural Science Foundation of China(Grant no.LR19B010001)open fund of State Key Laboratory of Structural Chemistry(No.20170036)。
文摘Research on water-splitting electrocatalysts is crucial to establishing a solution to the energy crisis.Herein,we report a facile bottom-up strategy for the preparation of high performance supported electrocatalysts for overall water-splitting reaction via a rationally designed defect covalent triazine frameworks(CTFs)support.Specifically,defect CTFs are obtained via binary-precursor polymerization,followed by loading Ru nanoparticles(Ru/D-CTFs-900)with high HER performance at a current density of 10 mA cm-2.The overpotential is only 17 mV.Calcination of the resultant Ru–RuO2/D-CTFs-300 in air,produces excellent OER performance with 190 mV overpotential(at 10 mA cm-2).Furthermore,overall water splitting measurements reveal the potential of 1.47 V,which is better than the majority of the reported Ru-based catalysts.Moreover,density functional theory calculation results show that excellent electrocatalytic properties are attributed to the synergistic effect of Ru nanoparticles and carbon support.
