The composite of zeolitic imidazolate frameworks(ZIF-67)and ordered macroporous carbon(OMC)was successfully synthesized via in situ growth from the OMC matrix.The ZIF67–OMC composite was verified by scanning electron...The composite of zeolitic imidazolate frameworks(ZIF-67)and ordered macroporous carbon(OMC)was successfully synthesized via in situ growth from the OMC matrix.The ZIF67–OMC composite was verified by scanning electron microscopy(SEM)and transmission electron microscopy(TEM),powder X-ray diffraction(XRD)and electrochemical impedance spectroscopy(EIS)and then evaluated as a modified material for electrochemical sensor.Benefitting from the large surface area and enhanced conductivity of the ZIF67–OMC composite,ZIF67–OMC nanocomposite showed superior electrocatalytic performance toward acetaminophen(AP)oxidation.The redox reaction of AP underwent a quasi-reversible redox reaction with higher anodic current at ZIF67–OMC modified electrode compared with the bare glassy carbon electrode(GCE).In optimal condition,the ZIF67–OMC/GCE was stable,reproducible and had a linear range of 0.05–100 μmol·L^(-1) AP concentration,with the detection limit of 20 nmol·L^(-1)(signal-to-noise of S/N=3).In addition,the prepared sensing platform for the detection of AP was evaluated for the compound paracetamol tablets and urine samples.展开更多
Ammonia is a key feedstock of fertilizers for farming and convenient hydrogen carrier as an emerging clean fuel,but industrial ammonium production process,Haber-Bosch reaction,is an energy-intensive process,consuming...Ammonia is a key feedstock of fertilizers for farming and convenient hydrogen carrier as an emerging clean fuel,but industrial ammonium production process,Haber-Bosch reaction,is an energy-intensive process,consuming 1%–2%of global energy and producing 3%global CO2.Electrochemical nitrogen reduction reaction(NRR)is one of the most promising routes to realize highly efficient NH3 production under ambient conditions.However,up to now,few precious-metal-free electrocatalysts with desirable catalytic performance have been explored.In this work,Mo2C nanodots anchored on three-dimensional ultrathin macroporous carbon(Mo2C@3DUM-C)framework is developed toward significantly enhanced nitrogen reduction reaction.Thanks to the special structural design of 3D ultrathin macroporous carbon and highly active and stable Mo2C toward N2 electrochemical reduction,the Mo2C@3DUM-C framework exhibits a high Faradaic efficiency of 9.5%for NH3 production at−0.20 V and the yield rate reaches 30.4µg h−1 mgMo2C−1.Further electrochemical characterizations reveal the enhanced electron transfer and increased electrochemical surface area in the 3D macroporous carbon framework.Moreover,the Mo2C@3DUM-C electrocatalysts hold high catalytic stability after long-term NRR test.The temperature-dependent yield rate of NH3 demonstrates that the activation energy of nitrogen reduction on the employed catalyst was calculated to be 28.1 kJ mol−1.Our proposed earth-abundant Mo2C@3DUM-C demonstrates an alternative insight into developing efficient and stable nitrogen fixation catalysts in acids as alternatives to noble metal catalysts.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.21904004 and 11804003)the Domestic Visiting Scholar Program for Outstanding Young Talents of Anhui Province(No.gxgnfx2019019)+2 种基金the Nature Foundation of Anhui Province(No.1808085MB31)the University Synergy Innovation Program of Anhui Province(Nos.GXXT-2019-043 and GXXT-2019-019)the Stable Talent Program and the Outstanding Talent Program of Anhui Science and Technology University。
文摘The composite of zeolitic imidazolate frameworks(ZIF-67)and ordered macroporous carbon(OMC)was successfully synthesized via in situ growth from the OMC matrix.The ZIF67–OMC composite was verified by scanning electron microscopy(SEM)and transmission electron microscopy(TEM),powder X-ray diffraction(XRD)and electrochemical impedance spectroscopy(EIS)and then evaluated as a modified material for electrochemical sensor.Benefitting from the large surface area and enhanced conductivity of the ZIF67–OMC composite,ZIF67–OMC nanocomposite showed superior electrocatalytic performance toward acetaminophen(AP)oxidation.The redox reaction of AP underwent a quasi-reversible redox reaction with higher anodic current at ZIF67–OMC modified electrode compared with the bare glassy carbon electrode(GCE).In optimal condition,the ZIF67–OMC/GCE was stable,reproducible and had a linear range of 0.05–100 μmol·L^(-1) AP concentration,with the detection limit of 20 nmol·L^(-1)(signal-to-noise of S/N=3).In addition,the prepared sensing platform for the detection of AP was evaluated for the compound paracetamol tablets and urine samples.
基金G.Yu acknowledges the funding support from US Department of Energy,Office of Science,Basic Energy Sciences,under Award DE-SC0019019,and Camille Dreyfus Teacher-Scholar Award.
文摘Ammonia is a key feedstock of fertilizers for farming and convenient hydrogen carrier as an emerging clean fuel,but industrial ammonium production process,Haber-Bosch reaction,is an energy-intensive process,consuming 1%–2%of global energy and producing 3%global CO2.Electrochemical nitrogen reduction reaction(NRR)is one of the most promising routes to realize highly efficient NH3 production under ambient conditions.However,up to now,few precious-metal-free electrocatalysts with desirable catalytic performance have been explored.In this work,Mo2C nanodots anchored on three-dimensional ultrathin macroporous carbon(Mo2C@3DUM-C)framework is developed toward significantly enhanced nitrogen reduction reaction.Thanks to the special structural design of 3D ultrathin macroporous carbon and highly active and stable Mo2C toward N2 electrochemical reduction,the Mo2C@3DUM-C framework exhibits a high Faradaic efficiency of 9.5%for NH3 production at−0.20 V and the yield rate reaches 30.4µg h−1 mgMo2C−1.Further electrochemical characterizations reveal the enhanced electron transfer and increased electrochemical surface area in the 3D macroporous carbon framework.Moreover,the Mo2C@3DUM-C electrocatalysts hold high catalytic stability after long-term NRR test.The temperature-dependent yield rate of NH3 demonstrates that the activation energy of nitrogen reduction on the employed catalyst was calculated to be 28.1 kJ mol−1.Our proposed earth-abundant Mo2C@3DUM-C demonstrates an alternative insight into developing efficient and stable nitrogen fixation catalysts in acids as alternatives to noble metal catalysts.