The granule shape and crystal structure of the the ceria-based rare earth oxide which were roasted at 600～1050 ℃ for 2～6 h and then cooled in furnace, cooled out of furnace or cooled in water were studied by means ...The granule shape and crystal structure of the the ceria-based rare earth oxide which were roasted at 600～1050 ℃ for 2～6 h and then cooled in furnace, cooled out of furnace or cooled in water were studied by means of XRD and SEM. The results revealed that the rich cerium rare earth carbonate could be changed into the rare earth oxide which was a kind of sandwich made of globose granule whose diameter was between 0.5～3.0 μm after being roasted in 900 ℃ for 2 h. This kind of crystal lattice in rare earth oxide belonged to face-centered cubic lattice and its space between crystal surface {111} and {200} (viz. L111 and L200) would enlarge as the roasting temperature increasing. With increasing roasting temperature, L111 would rise straightly upward, and L200 would rise straightly upward when roasting time was 2～4 h but changed little when roasting time was 4～6 h. The glass-polishing experiments found that the polishing ability of the ceria-based rare earth oxide was the best as L111 was 43～53 nm and the L200 was 43～56 nm.展开更多
While the electrochemical nitrogen reduction reaction(NRR) represents a prospective blueprint for environmentally renewable ammonia generation,it has yet to overcome the limitations of weak activity and inferior selec...While the electrochemical nitrogen reduction reaction(NRR) represents a prospective blueprint for environmentally renewable ammonia generation,it has yet to overcome the limitations of weak activity and inferior selectivity.In this regard,surface modification tactic was constructed to markedly enhance the activity and selectivity via introducing Sn atoms into the surface of defective cerium oxide(denoted as Sn-CeO_(2-x)) as the active and robust electrocatalyst for NRR under benign environment.The introduction of Sn atoms in CeO_(2-x)can not only inhibit the HER activity of the catalyst but also modulate the electronic structure of ceria and optimize N-Ce interaction,thus enhancing NRR activity and selectivity.Outperforming all previous CeO_(2)-based NRR catalysts,this catalyst has demonstrated an ammonia yield rate of 41.1 μg mg_(cat)^(-1) h^(-1) and an exceptional Faradic efficiency of 35.3%.This work presents a viable approach for the development of advanced NRR electrocatalysts.展开更多
Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-a...Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.展开更多
As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au species.Previous reports were extensively focused...As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au species.Previous reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was limited.Herein,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),respectively.Based on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) matrix.The CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) sites.This work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.展开更多
文摘The granule shape and crystal structure of the the ceria-based rare earth oxide which were roasted at 600～1050 ℃ for 2～6 h and then cooled in furnace, cooled out of furnace or cooled in water were studied by means of XRD and SEM. The results revealed that the rich cerium rare earth carbonate could be changed into the rare earth oxide which was a kind of sandwich made of globose granule whose diameter was between 0.5～3.0 μm after being roasted in 900 ℃ for 2 h. This kind of crystal lattice in rare earth oxide belonged to face-centered cubic lattice and its space between crystal surface {111} and {200} (viz. L111 and L200) would enlarge as the roasting temperature increasing. With increasing roasting temperature, L111 would rise straightly upward, and L200 would rise straightly upward when roasting time was 2～4 h but changed little when roasting time was 4～6 h. The glass-polishing experiments found that the polishing ability of the ceria-based rare earth oxide was the best as L111 was 43～53 nm and the L200 was 43～56 nm.
基金financially supported by the National Natural Science Foundation of China (51972349 and 91963210)the Natural Science Foundation of Guangdong Province (2022A1515011596)the Key Research and Development Program of Guangdong Province (2020B0101690001)。
文摘While the electrochemical nitrogen reduction reaction(NRR) represents a prospective blueprint for environmentally renewable ammonia generation,it has yet to overcome the limitations of weak activity and inferior selectivity.In this regard,surface modification tactic was constructed to markedly enhance the activity and selectivity via introducing Sn atoms into the surface of defective cerium oxide(denoted as Sn-CeO_(2-x)) as the active and robust electrocatalyst for NRR under benign environment.The introduction of Sn atoms in CeO_(2-x)can not only inhibit the HER activity of the catalyst but also modulate the electronic structure of ceria and optimize N-Ce interaction,thus enhancing NRR activity and selectivity.Outperforming all previous CeO_(2)-based NRR catalysts,this catalyst has demonstrated an ammonia yield rate of 41.1 μg mg_(cat)^(-1) h^(-1) and an exceptional Faradic efficiency of 35.3%.This work presents a viable approach for the development of advanced NRR electrocatalysts.
文摘Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.
基金funded by the National Key Research and Development Program of China(2021YFA1501103)the National Science Fund for Distinguished Young Scholars of China(22225110)+1 种基金the National Science Foundation of China(22075166,22271177)the Young Scholars Program of Shandong University.
文摘As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au species.Previous reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was limited.Herein,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),respectively.Based on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) matrix.The CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) sites.This work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.
