钯催化剂对碱性溶液的乙醇电催化氧化反应表现较好的催化活性.本文通过简单的化学沉积法,将钯原子成功修饰到金纳米颗粒表面,制备的催化剂对乙醇电催化氧化反应表现出比钯更好的催化性能.研究发现,钯原子不均匀地覆盖在金核表面,部分金...钯催化剂对碱性溶液的乙醇电催化氧化反应表现较好的催化活性.本文通过简单的化学沉积法,将钯原子成功修饰到金纳米颗粒表面,制备的催化剂对乙醇电催化氧化反应表现出比钯更好的催化性能.研究发现,钯原子不均匀地覆盖在金核表面,部分金原子暴露在外层.制备的催化剂的峰电流密度是钯催化剂的4.6倍,起始电势低100 m V.该催化剂较好的催化性能可能归因于金核的电子效应和表面双功能电催化反应机制.展开更多
A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Comp...A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.展开更多
By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts d...By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.展开更多
基金support from Research Grant Council(No.26206115) of the Hong Kong Special Administrative RegionScientific Research Fund of Zhejiang Provincial Education Department(No.Y201840545).
文摘钯催化剂对碱性溶液的乙醇电催化氧化反应表现较好的催化活性.本文通过简单的化学沉积法,将钯原子成功修饰到金纳米颗粒表面,制备的催化剂对乙醇电催化氧化反应表现出比钯更好的催化性能.研究发现,钯原子不均匀地覆盖在金核表面,部分金原子暴露在外层.制备的催化剂的峰电流密度是钯催化剂的4.6倍,起始电势低100 m V.该催化剂较好的催化性能可能归因于金核的电子效应和表面双功能电催化反应机制.
基金Project(cstc2020jcyj-msxm X0930) supported by the Natural Science Foundation of Chongqing,ChinaProject(KJQN201901522) supported by Technological Research Program of Chongqing Municipal Education Commission,ChinaProject(cx2020068) supported by the Venture&Innovation Support Program for Chongqing Overseas Returnees,China。
文摘A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.
基金supported by the Petrochemical Research Institute Foundation(21-CB-09-01)the National Natural Science Foundation of China(22302186,22025205)+1 种基金the China Postdoctoral Science Foundation(2022M713030,2023T160618)the Fundamental Research Funds for the Central Universities(WK2060000058,WK2060000038).
文摘By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.
