Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability...Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability.In response to the defects,herein,the Mg-incorporated perovskite cobaltite SrCo_(0.6)Fe_(0.3M)g_(0.1)O_(3-δ)(SCFM-0.1)is proposed as a novel earth-abundant and durable OER electrocatalyst.A well-consolidated cubic-symmetry structure and more active oxygen intermediates are enabled upon Mg substitution.Hence,the optimized SCFM-0.1 perovskite oxide achieves prominent OER electrocatalytic performance,that is,a low overpotential of only 320 mV at 10 mA cm^(-2),a small Tafel slope of 65 mV dec^(-1),as well as an outstanding durability within 20 h,substantially outperforming that of the pristine SrCo_(0.7)Fe_(0.3)O_(3-δ)and benchmark Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)and IrO_(2) catalysts.The strong pHdependent behavior associated with lattice oxygen activation mechanism for SCFM-0.1 catalyst is also confirmed.This work paves a unique avenue to develop cost-effective and robust perovskite cobaltites for efficient OER electrocatalysis.展开更多
Oxygen transfer presents a serious challenge in the application of liquid lead as a nuclear coolant in advanced reactors. To mitigate corrosion by liquid lead in contact with steel, carefully controlling the oxygen co...Oxygen transfer presents a serious challenge in the application of liquid lead as a nuclear coolant in advanced reactors. To mitigate corrosion by liquid lead in contact with steel, carefully controlling the oxygen concentration has been used as an effective way. Oxygen needs to mix in liquid lead uniformly and quickly. To enhance oxygen transport in liquid lead, nanoparticles are added to the liquid metal. In the current study, a lattice Boltzmann method is applied to investigate natural convection of copper/lead and aluminum oxide/lead in two-dimensional simplified container. Two thermal boundary cases are evaluated in order to check the effect of different natural convection flow patterns on oxygen transport. Some useful information are obtained such as improvement in natural convection and reduction in oxygen equilibrium time.展开更多
Supported noble metal catalysts have the promising application in volatile organic compounds(VOCs)catalytic combustion but suffer from the deactivation due to noble metal sintering at high temperatures.Herein,we repor...Supported noble metal catalysts have the promising application in volatile organic compounds(VOCs)catalytic combustion but suffer from the deactivation due to noble metal sintering at high temperatures.Herein,we report the construction of shellsandwiched MnO_(2)-Ag-CeO_(2)hollow spheres with remarkable sintering resistance and high activity in toluene combustion.Ag clusters were sandwiched between outer MnO_(2)and inner CeO_(2)shell to enlarge and stabilize metal–support active interface.The unique hollow structure could alter the electronic states of catalysts sites and increase the adsorbed site of reactant molecules.Meanwhile,Mn–Ag–Ce multi-interfaces in MnO_(2)-Ag-CeO_(2)could facilitate the sustainable activation and the stable release of oxygen species via a tandem transfer.The oxygen species at Ag–Mn interface perimeter were instantly replenished by Ag–Ce interface to accelerate a deep oxidation of intermediates,guaranteeing the opening of benzene ring to generate maleic anhydride.This investigation provides a promising method for constructing efficient and sintering-resistant cluster catalysts for VOCs oxidation.展开更多
基金supported by the National Natural Science Foundation of China(No.22108043)Natural Science Foundation of Guangdong Province,China(No.2023A1515012711).
文摘Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability.In response to the defects,herein,the Mg-incorporated perovskite cobaltite SrCo_(0.6)Fe_(0.3M)g_(0.1)O_(3-δ)(SCFM-0.1)is proposed as a novel earth-abundant and durable OER electrocatalyst.A well-consolidated cubic-symmetry structure and more active oxygen intermediates are enabled upon Mg substitution.Hence,the optimized SCFM-0.1 perovskite oxide achieves prominent OER electrocatalytic performance,that is,a low overpotential of only 320 mV at 10 mA cm^(-2),a small Tafel slope of 65 mV dec^(-1),as well as an outstanding durability within 20 h,substantially outperforming that of the pristine SrCo_(0.7)Fe_(0.3)O_(3-δ)and benchmark Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)and IrO_(2) catalysts.The strong pHdependent behavior associated with lattice oxygen activation mechanism for SCFM-0.1 catalyst is also confirmed.This work paves a unique avenue to develop cost-effective and robust perovskite cobaltites for efficient OER electrocatalysis.
基金the financial support from the office of Vice-President for Research at University of Nevada-Las Vegas
文摘Oxygen transfer presents a serious challenge in the application of liquid lead as a nuclear coolant in advanced reactors. To mitigate corrosion by liquid lead in contact with steel, carefully controlling the oxygen concentration has been used as an effective way. Oxygen needs to mix in liquid lead uniformly and quickly. To enhance oxygen transport in liquid lead, nanoparticles are added to the liquid metal. In the current study, a lattice Boltzmann method is applied to investigate natural convection of copper/lead and aluminum oxide/lead in two-dimensional simplified container. Two thermal boundary cases are evaluated in order to check the effect of different natural convection flow patterns on oxygen transport. Some useful information are obtained such as improvement in natural convection and reduction in oxygen equilibrium time.
基金the National Natural Science Foundation of China(Nos.22076192,22006032,21777166,42175133,and 21806169)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011)the National Key Research and Development Program of China(No.2016YFC0202202)。
文摘Supported noble metal catalysts have the promising application in volatile organic compounds(VOCs)catalytic combustion but suffer from the deactivation due to noble metal sintering at high temperatures.Herein,we report the construction of shellsandwiched MnO_(2)-Ag-CeO_(2)hollow spheres with remarkable sintering resistance and high activity in toluene combustion.Ag clusters were sandwiched between outer MnO_(2)and inner CeO_(2)shell to enlarge and stabilize metal–support active interface.The unique hollow structure could alter the electronic states of catalysts sites and increase the adsorbed site of reactant molecules.Meanwhile,Mn–Ag–Ce multi-interfaces in MnO_(2)-Ag-CeO_(2)could facilitate the sustainable activation and the stable release of oxygen species via a tandem transfer.The oxygen species at Ag–Mn interface perimeter were instantly replenished by Ag–Ce interface to accelerate a deep oxidation of intermediates,guaranteeing the opening of benzene ring to generate maleic anhydride.This investigation provides a promising method for constructing efficient and sintering-resistant cluster catalysts for VOCs oxidation.
