Downsizing to sub-nm is a general strategy to reduce the cost of catalysts. However, theoretical Wulff-constructed model suggests that sub-nm clusters show little activity for various reactions such as ammonia decompo...Downsizing to sub-nm is a general strategy to reduce the cost of catalysts. However, theoretical Wulff-constructed model suggests that sub-nm clusters show little activity for various reactions such as ammonia decomposition and ammonia synthesis because of the lack of active sites. As clusters may deviate from the ideal model construction under reaction conditions, a host-guest strategy to synthesize thermally stable 1.0 run monodispersed Ru dusters by the pyrolysis of MIL-101 hosts is reported here to verify the hypothesis. For ammonia decomposition, the activity of the Ru clusters is 25 times higher than that of commercial Ru/active carbon （AC） at full-conversion temperature, while for ammonia synthesis, the activity of the Ru dusters is 500 times as high as that of promoted Ru NPs counterpart. The catalyst also maintains its activities for 40 h without any increase in the size. This model can be used to develop a host-guest strategy for designing thermally stable sub-nm clusters to atomic-efficiently catalyze reactions.展开更多
We propose to generate a sub-nanometer-confined optical field in a nanoslit waveguiding mode in a coupled nanowire pair(CNP).We show that,when a conventional waveguide mode with a proper polarization is evanescently c...We propose to generate a sub-nanometer-confined optical field in a nanoslit waveguiding mode in a coupled nanowire pair(CNP).We show that,when a conventional waveguide mode with a proper polarization is evanescently coupled into a properly designed CNP with a central nanoslit,it can be efficiently channeled into a high-purity nanoslit mode within a waveguiding length<10μm.The CNP can be either freestanding or on-chip by using a tapered fiber or planar waveguide for input-coupling,with a coupling efficiency up to 95%.Within the slit region,the output diffraction-limited nanoslit mode offers an extremely confined optical field(∼0.3 nm×3.3 nm)with a peak-to-background ratio higher than 25 dB and can be operated within a 200-nm bandwidth.The group velocity dispersion of the nanoslit mode for ultrafast pulsed operation is also briefly investigated.Compared with the previous lasing configuration,the waveguiding scheme demonstrated here is not only simple and straightforward in structural design but is also much flexible and versatile in operation.Therefore,the waveguiding scheme we show here may offer an efficient and flexible platform for exploring light–matter interactions beyond the nanometer scale,and developing optical technologies ranging from superresolution nanoscopy and atom/molecule manipulation to ultra-sensitivity detection.展开更多
文摘Downsizing to sub-nm is a general strategy to reduce the cost of catalysts. However, theoretical Wulff-constructed model suggests that sub-nm clusters show little activity for various reactions such as ammonia decomposition and ammonia synthesis because of the lack of active sites. As clusters may deviate from the ideal model construction under reaction conditions, a host-guest strategy to synthesize thermally stable 1.0 run monodispersed Ru dusters by the pyrolysis of MIL-101 hosts is reported here to verify the hypothesis. For ammonia decomposition, the activity of the Ru clusters is 25 times higher than that of commercial Ru/active carbon （AC） at full-conversion temperature, while for ammonia synthesis, the activity of the Ru dusters is 500 times as high as that of promoted Ru NPs counterpart. The catalyst also maintains its activities for 40 h without any increase in the size. This model can be used to develop a host-guest strategy for designing thermally stable sub-nm clusters to atomic-efficiently catalyze reactions.
基金This work was sup-ported by the National Key Research and Development Program of China(2018YFB2200404)the New Cornerstone Science Foundation,the National Natural Science Foundation of China(92150302 and 62175213)+1 种基金the Natural Science Foundation of Zhejiang Province(LR21F050002)the Fundamental Research Funds for the Central Universities.
文摘We propose to generate a sub-nanometer-confined optical field in a nanoslit waveguiding mode in a coupled nanowire pair(CNP).We show that,when a conventional waveguide mode with a proper polarization is evanescently coupled into a properly designed CNP with a central nanoslit,it can be efficiently channeled into a high-purity nanoslit mode within a waveguiding length<10μm.The CNP can be either freestanding or on-chip by using a tapered fiber or planar waveguide for input-coupling,with a coupling efficiency up to 95%.Within the slit region,the output diffraction-limited nanoslit mode offers an extremely confined optical field(∼0.3 nm×3.3 nm)with a peak-to-background ratio higher than 25 dB and can be operated within a 200-nm bandwidth.The group velocity dispersion of the nanoslit mode for ultrafast pulsed operation is also briefly investigated.Compared with the previous lasing configuration,the waveguiding scheme demonstrated here is not only simple and straightforward in structural design but is also much flexible and versatile in operation.Therefore,the waveguiding scheme we show here may offer an efficient and flexible platform for exploring light–matter interactions beyond the nanometer scale,and developing optical technologies ranging from superresolution nanoscopy and atom/molecule manipulation to ultra-sensitivity detection.
基金supported by the Ministry of Science and Technology of China (2017YFA0700101, 2016YFA0202801 and 2016YBF0100100)China Postdoctoral Science Foundation funded project (2020TQ0164)+7 种基金the Shuimu Tsinghua Scholar Programthe National Natural Science Foundation of China (22035004, 51872283 and 21805273)Liaoning Bai Qian Wan Talents ProgramLiaoning Revitalization Talents Program (XLYC1807153)Dalian Institute of Chemical Physics (DICP ZZBS201708, DICP ZZBS201802 and DICP I202032)DICP&QIBEBT (DICP&QIBEBT UN201702)Dalian National Laboratory For Clean Energy (DNL) Cooperation FundCAS (DNL180310, DNL180308, DNL201912 and DNL201915)。
