Hydrogenation of N-ethylcarbazole(NEC),the hydrogen lean form of a liquid organic hydrogen carrier,on TiO2 supported Ru-Ni bimetallic catalysts is investigated.Crystal structure of TiO2 plays a critical role on the hy...Hydrogenation of N-ethylcarbazole(NEC),the hydrogen lean form of a liquid organic hydrogen carrier,on TiO2 supported Ru-Ni bimetallic catalysts is investigated.Crystal structure of TiO2 plays a critical role on the hydrogenation activity and selectivity towards fully hydrogenated product.Ru/anatase catalyst exhibits higher selectivity but lower reactivity compared to Ru/rutile catalyst.Ni addition significantly promotes the performance of Ru/anatase catalyst while causes severe performance deterioration of Ru/rutile catalyst.Commercial P25,a mixture of anatase and rutile phases in approximate ratio A/R1/4,is found to be the best TiO2 support for NEC hydrogenation.Ru/P25 catalyst outperforms both Ru/rutile and Ru/anatase and its activity can be further slightly improved by Ni addition.The unexpected synergism between the two different TiO2 phases for Ru based NEC hydrogenation catalysts is related to metal-support interaction and Ru-Ni interaction.展开更多
Gadolinium oxide(Gd2O3) film has potential as a candidate gate dielectric to replace Hf O2. In this work,we provide a simple method by trace Ta(~1%) doping to significantly improve the dielectric properties of Gd2O3 f...Gadolinium oxide(Gd2O3) film has potential as a candidate gate dielectric to replace Hf O2. In this work,we provide a simple method by trace Ta(~1%) doping to significantly improve the dielectric properties of Gd2O3 film. And effects of annealing temperatures of Ta-doped Gd2O3(GTO) films are investigated in detail. Results show that GTO film annealed at 500℃ exhibits excellent performance as a novel gate dielectric material for integrated circuit, showing a small surface roughness of 0.199 nm, a large band gap of 5.45 e V, a high dielectric constant(k) of 21.2 and a low leakage current density(Jg) of 2.10 × 10^-3A/cm^2.All properties of GTO films are superior to pure Gd2O3 films and these GTO films meet the requirements for next-generation gate dielectrics. In addition, impedance spectrum is first used to analyze the equivalent circuit of GTO based metal-oxide-semiconductor(MOS) capacitors, which represents a new insight to understand observed electrical behaviors.展开更多
N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobal...N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobalt(Co)-based catalyst promoted by nonstoichiometric yttrium hydride(YH_(3−x))to achieve high-efficiency,reversible hydrogen storage in NEC,with>5.5 wt%reversible hydrogen storage capacity could be achieved below 473 K,and with good kinetics.The YH_(3−x)-promoted Co-based catalyst is the first non-noble metal catalyst with high activity for NEC hydrogenation and 12H-NEC dehydrogenation reactions.A mechanistic study suggests that YH_(3−x)facilitates the reversible hydrogen transfer both in the hydrogenation and the dehydrogenation reactions.The nonstoichiometric YH_(3−x)contained both lattice H and H vacancies with tunable H chemical potential serve as the H donor and H acceptor for reversible hydrogen transfer.Our results support the practical application of LOHCs and inspire new approaches for the utilization of conventional metal hydrides to promote versatile H transfer reactions.展开更多
基金NSFC (Nos. 21771006, U1607126 and 51771002)MOST of China (No. 2017YFB0405902)Beijing Municipal Commission of Science and Technology (Z17110000091702)
文摘Hydrogenation of N-ethylcarbazole(NEC),the hydrogen lean form of a liquid organic hydrogen carrier,on TiO2 supported Ru-Ni bimetallic catalysts is investigated.Crystal structure of TiO2 plays a critical role on the hydrogenation activity and selectivity towards fully hydrogenated product.Ru/anatase catalyst exhibits higher selectivity but lower reactivity compared to Ru/rutile catalyst.Ni addition significantly promotes the performance of Ru/anatase catalyst while causes severe performance deterioration of Ru/rutile catalyst.Commercial P25,a mixture of anatase and rutile phases in approximate ratio A/R1/4,is found to be the best TiO2 support for NEC hydrogenation.Ru/P25 catalyst outperforms both Ru/rutile and Ru/anatase and its activity can be further slightly improved by Ni addition.The unexpected synergism between the two different TiO2 phases for Ru based NEC hydrogenation catalysts is related to metal-support interaction and Ru-Ni interaction.
基金supported financially by the Project of Ministry of Science and Technology of the People’s Republic of China (No. 2017YFB0405902)the National Natural Science Foundation of China (Nos. 51431001, 51771002, 21771006, U1607126 and 21621061)Beijing Municipal Commission of Science and Technology (No. Z17110000091702)
文摘Gadolinium oxide(Gd2O3) film has potential as a candidate gate dielectric to replace Hf O2. In this work,we provide a simple method by trace Ta(~1%) doping to significantly improve the dielectric properties of Gd2O3 film. And effects of annealing temperatures of Ta-doped Gd2O3(GTO) films are investigated in detail. Results show that GTO film annealed at 500℃ exhibits excellent performance as a novel gate dielectric material for integrated circuit, showing a small surface roughness of 0.199 nm, a large band gap of 5.45 e V, a high dielectric constant(k) of 21.2 and a low leakage current density(Jg) of 2.10 × 10^-3A/cm^2.All properties of GTO films are superior to pure Gd2O3 films and these GTO films meet the requirements for next-generation gate dielectrics. In addition, impedance spectrum is first used to analyze the equivalent circuit of GTO based metal-oxide-semiconductor(MOS) capacitors, which represents a new insight to understand observed electrical behaviors.
基金This research was made possible as a result of a generous grant from MOST of China(no.2018YFB1502102)NSFC(nos.21771006,51771002,and 51971004).
文摘N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobalt(Co)-based catalyst promoted by nonstoichiometric yttrium hydride(YH_(3−x))to achieve high-efficiency,reversible hydrogen storage in NEC,with>5.5 wt%reversible hydrogen storage capacity could be achieved below 473 K,and with good kinetics.The YH_(3−x)-promoted Co-based catalyst is the first non-noble metal catalyst with high activity for NEC hydrogenation and 12H-NEC dehydrogenation reactions.A mechanistic study suggests that YH_(3−x)facilitates the reversible hydrogen transfer both in the hydrogenation and the dehydrogenation reactions.The nonstoichiometric YH_(3−x)contained both lattice H and H vacancies with tunable H chemical potential serve as the H donor and H acceptor for reversible hydrogen transfer.Our results support the practical application of LOHCs and inspire new approaches for the utilization of conventional metal hydrides to promote versatile H transfer reactions.
