Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-gr...Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.展开更多
Developing efficient and durable electrocatalysts for water splitting, which has long been regarded as one of the most promising patterns to produce green hydrogen, is of great significance but still challenging. Here...Developing efficient and durable electrocatalysts for water splitting, which has long been regarded as one of the most promising patterns to produce green hydrogen, is of great significance but still challenging. Herein,ample Co/MoN heterogeneous domains/nitrogen-doped carbon(Co/MoN/NC) nanosheet arrays as high-performance hydrogen evolution reaction(HER) electrocatalyst via a typical nitriding-carbonization strategy are successfully prepared on nickel foam(NF), which exhibits a low overpotential of 29 m V at 10 m A cm, together with excellent durability at 20 m A cmfor 90 h in alkaline solution. Such excellent catalytic property for HER can be attributed to the generation of abundant Co/Mo N heterogeneous structures. Additionally, the high conductivity of Co/Mo N and NC also increases the charge transfer rate, further helping accelerate the reaction rate of HER. This work presents an efficient method for improving the catalytic hydrogen evolution activity in basic solution.展开更多
Understanding the negative thermal expansion(NTE)mechanism remains an important and challenging thing.In this work,we selected the case of YFe(CN)_(6)to investigate the structure-mechanism relation on the base of crys...Understanding the negative thermal expansion(NTE)mechanism remains an important and challenging thing.In this work,we selected the case of YFe(CN)_(6)to investigate the structure-mechanism relation on the base of crystal structure,electro nic structure and lattice dynamics.We expanded the NTE of YFe(CN)_(6)to 150 K,and the temperature dependence of volume and lattice constants was determined by temperature-variable synchrotro n X-ray diffraction measure ments.A large NTE was found in the system.Our theoretical calculations indicate that the Y-N bond exhibits a strong ionic feature through the calculated electron localization function(ELF),which has a strong influence on the anisotropic vibration of the N atom.The detailed lattice dynamics simulations suggest that the NTE of YFe(CN)_(6)may be related to the presence of the unusual low-frequency modes of the YN_(6)triangular prism(tri-prism)units.The optical branches with low frequencies are mainly related to the distortion and twisting modes of the YN_(6)tri-prism units,which contribute most to the NTE effect in the crystal.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22075159,22002066)Shandong Taishan Scholars Project(Grant Nos.ts20190932,tsqn202103058)+1 种基金Open Fund of Hubei Key Laboratory of Processing and Application of Catalytic Materials(Grant No.202203404)Postdoctoral Applied Research Project in Qingdao,and the Youth Innovation Team Project of Shandong Provincial Education Department(Grant No.2019KJC023).
文摘Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.
基金financially supported by the National Natural Science Foundation of China (No. 22075159)Taishan Scholar Program (No. tsqn202103058)the Youth Innovation Team Project of Shandong Provincial Education Department (No. 2019KJC023)。
文摘Developing efficient and durable electrocatalysts for water splitting, which has long been regarded as one of the most promising patterns to produce green hydrogen, is of great significance but still challenging. Herein,ample Co/MoN heterogeneous domains/nitrogen-doped carbon(Co/MoN/NC) nanosheet arrays as high-performance hydrogen evolution reaction(HER) electrocatalyst via a typical nitriding-carbonization strategy are successfully prepared on nickel foam(NF), which exhibits a low overpotential of 29 m V at 10 m A cm, together with excellent durability at 20 m A cmfor 90 h in alkaline solution. Such excellent catalytic property for HER can be attributed to the generation of abundant Co/Mo N heterogeneous structures. Additionally, the high conductivity of Co/Mo N and NC also increases the charge transfer rate, further helping accelerate the reaction rate of HER. This work presents an efficient method for improving the catalytic hydrogen evolution activity in basic solution.
基金supported by the National Natural Science Foundation of China(22071221,21905252)Natural Science Foundation of Henan Province(212300410086)。
文摘Understanding the negative thermal expansion(NTE)mechanism remains an important and challenging thing.In this work,we selected the case of YFe(CN)_(6)to investigate the structure-mechanism relation on the base of crystal structure,electro nic structure and lattice dynamics.We expanded the NTE of YFe(CN)_(6)to 150 K,and the temperature dependence of volume and lattice constants was determined by temperature-variable synchrotro n X-ray diffraction measure ments.A large NTE was found in the system.Our theoretical calculations indicate that the Y-N bond exhibits a strong ionic feature through the calculated electron localization function(ELF),which has a strong influence on the anisotropic vibration of the N atom.The detailed lattice dynamics simulations suggest that the NTE of YFe(CN)_(6)may be related to the presence of the unusual low-frequency modes of the YN_(6)triangular prism(tri-prism)units.The optical branches with low frequencies are mainly related to the distortion and twisting modes of the YN_(6)tri-prism units,which contribute most to the NTE effect in the crystal.