The in situ growth of nano-array on material structure is a novel and high-efficient strategy to design catalysts,however,it still remains a challenge to fabricate unique nano-architecture electrocatalyst with promine...The in situ growth of nano-array on material structure is a novel and high-efficient strategy to design catalysts,however,it still remains a challenge to fabricate unique nano-architecture electrocatalyst with prominent activity and superior durability for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Herein,a unique nano-architecture catalyst is successfully synthesized by using NiFe LDH nanosheets as framework to the in situ growth Mo-doped Ni2 P ultrafine nanosheets(marked as Mo-Ni2 P@NiFe LDH/NF).The unique 3 D core-shell nano-architecture is favorable for enhancing electron transfer/mass diffusion,providing abundant active sites,prompting O2/H2 gas release,and creating the synergistic effect between Mo-Ni2 P and NiFe LDH.Therefore,comparing with pure NiFe LDH/NF and MoNi2 P/NF electrodes,walnut-like Mo-Ni2 P@Ni Fe LDH/NF catalyst exhibits significantly improved electrocatalytic activities and durability towards OER(269 m V@40 m A cm^-2),HER(82 mV@10 mA cm^-2),and overall water splitting(1.46 V@10 m A cm^-2),respectively.Such electrocatalytic activity of Mo-Ni2 P@NiFe LDH/NF is comparable with that of majority reported non-precious metal catalysts and even precious catalysts(IrO2 and Pt/C).This work presents a new perspective strategy to fabricate ingeniously bifunctional electrocatalysts with well-designed structure and superior performance for clean energy conversion technologies or storage devices.展开更多
A flame retardant containing multiple antiflaming elements usually exhibits high-efficient flame retardancy. Here, a novel P/N/Si-containing ammonium polyphosphate derivative(APTES-APP) is synthesized from ammonium po...A flame retardant containing multiple antiflaming elements usually exhibits high-efficient flame retardancy. Here, a novel P/N/Si-containing ammonium polyphosphate derivative(APTES-APP) is synthesized from ammonium polyphosphate(APP) and silane coupling agent(3-aminopropyl)triethoxysilane(APTES)via cation exchange, which is quite different in the chemical structure from APTES-modified APP for retaining silicon hydroxyls. APTES-APP is highly efficient for the epoxy resin. 8%(mass) APTES-APP imparts excellent flame retardancy to the epoxy resin, with a V-0 rating at the UL-94 test(1.6 mm)and an LOI value of 26%(vol). The peak heat release rate and total smoke production of the flameretardant epoxy resin are decreased by 68.1% and 31.3%, respectively. The synergy of P/N/Si contributes to the well-expanded char residue with a strong and dense surface layer, which is a very good barrier against heat and mass transfer. Besides, there is no significant deterioration in the mechanical properties of flame-retardant epoxy resin thanks to silicon hydroxyls forming hydrogen bonds with epoxy molecules. Meanwhile, other molecules can be grafted onto APTES-APP via these silicon hydroxyls, if needed.Briefly, this work has developed a new strategy for amino silane as flame retardants. In conjunction with a low-cost and simple preparation method, APTES-APP has a promising prospect in the high-performance flame-retardant epoxy.展开更多
The precise control of multiple chiral elements through a single step catalytic process remains a significant challenge in asymmetric catalysis.Reported herein is rhodium-catalyzed three-component asymmetric carboamid...The precise control of multiple chiral elements through a single step catalytic process remains a significant challenge in asymmetric catalysis.Reported herein is rhodium-catalyzed three-component asymmetric carboamidation between aryl boronic acid,achiral strain-activated symmetric bicyclic olefins bearing a prochiral C-N or N-N axis,and dioxazolones.The reaction proceeded effectively in excellent enantio-and diastereoselectivity under mild conditions to produce the bicyclic framework with six contiguous chiral centers as well as a N-N or C-N chiral axis.The reaction featured excellent functional group tolerance,chemoselectivity,and stereoselectivity.Mechanistic studies indicated that the coupling system proceeded via initial transmetalation,followed by stereo-determining migratory insertion into the olefin and electrophilic amidation.展开更多
The exploration of cost-effective,high-performance,and stable electrocatalysts for the hydrogen evolution reaction(HER)over wide pH range(0–14)is of paramount importance for future renewable energy conversion technol...The exploration of cost-effective,high-performance,and stable electrocatalysts for the hydrogen evolution reaction(HER)over wide pH range(0–14)is of paramount importance for future renewable energy conversion technologies.Regulation of electronic structure through doping vanadium atoms is a feasible construction strategy to enhance catalytic activities,electron transfer capability,and stability of the HER electrode.Herein,V-doped NiCoP nanosheets on carbon fiber paper(CFP)(denoted as Vx-NiCoP/CFP)were constructed by doping V modulation on NiCoP nanosheets on CFP and used for pH-universal HER.Benefiting from the abundant catalytic sites and optimized hydrogen binding thermodynamics,the resultant V15-NiCoP/CFP demonstrates a significantly improved HER catalytic activity,requiring overpotentials of 46.5,52.4,and 85.3 mV to reach a current density of 10 mA·cm^(−2)in 1 mol·L^(−1) KOH,0.5 mol·L^(−1) H_(2)SO_(4),and 1 mol·L^(−1) phosphate buffer solution(PBS)electrolytes,respectively.This proposed cation-doping strategy provides a new inspiration to rationally enhance or design new-type nonprecious metal-based,highly efficient,and pH-universal electrocatalysts for various energy conversion systems.展开更多
基金supported financially by the Key Research and Development Program of Shanxi(201803D421085)Shanxi Scholarship Council of China,Shanxi Graduate Education Innovation ProjectState key laboratory of physical chemistry of solid surface,Xiamen University(201912)。
文摘The in situ growth of nano-array on material structure is a novel and high-efficient strategy to design catalysts,however,it still remains a challenge to fabricate unique nano-architecture electrocatalyst with prominent activity and superior durability for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Herein,a unique nano-architecture catalyst is successfully synthesized by using NiFe LDH nanosheets as framework to the in situ growth Mo-doped Ni2 P ultrafine nanosheets(marked as Mo-Ni2 P@NiFe LDH/NF).The unique 3 D core-shell nano-architecture is favorable for enhancing electron transfer/mass diffusion,providing abundant active sites,prompting O2/H2 gas release,and creating the synergistic effect between Mo-Ni2 P and NiFe LDH.Therefore,comparing with pure NiFe LDH/NF and MoNi2 P/NF electrodes,walnut-like Mo-Ni2 P@Ni Fe LDH/NF catalyst exhibits significantly improved electrocatalytic activities and durability towards OER(269 m V@40 m A cm^-2),HER(82 mV@10 mA cm^-2),and overall water splitting(1.46 V@10 m A cm^-2),respectively.Such electrocatalytic activity of Mo-Ni2 P@NiFe LDH/NF is comparable with that of majority reported non-precious metal catalysts and even precious catalysts(IrO2 and Pt/C).This work presents a new perspective strategy to fabricate ingeniously bifunctional electrocatalysts with well-designed structure and superior performance for clean energy conversion technologies or storage devices.
基金financially supported by the National Natural Science Foundation of China (22178242)。
文摘A flame retardant containing multiple antiflaming elements usually exhibits high-efficient flame retardancy. Here, a novel P/N/Si-containing ammonium polyphosphate derivative(APTES-APP) is synthesized from ammonium polyphosphate(APP) and silane coupling agent(3-aminopropyl)triethoxysilane(APTES)via cation exchange, which is quite different in the chemical structure from APTES-modified APP for retaining silicon hydroxyls. APTES-APP is highly efficient for the epoxy resin. 8%(mass) APTES-APP imparts excellent flame retardancy to the epoxy resin, with a V-0 rating at the UL-94 test(1.6 mm)and an LOI value of 26%(vol). The peak heat release rate and total smoke production of the flameretardant epoxy resin are decreased by 68.1% and 31.3%, respectively. The synergy of P/N/Si contributes to the well-expanded char residue with a strong and dense surface layer, which is a very good barrier against heat and mass transfer. Besides, there is no significant deterioration in the mechanical properties of flame-retardant epoxy resin thanks to silicon hydroxyls forming hydrogen bonds with epoxy molecules. Meanwhile, other molecules can be grafted onto APTES-APP via these silicon hydroxyls, if needed.Briefly, this work has developed a new strategy for amino silane as flame retardants. In conjunction with a low-cost and simple preparation method, APTES-APP has a promising prospect in the high-performance flame-retardant epoxy.
基金supported by the National Natural Science Foundation of China(21525208)the Fundamental Research Funds for the Central Universities(2020CSLZ005,GK202103031)
文摘The precise control of multiple chiral elements through a single step catalytic process remains a significant challenge in asymmetric catalysis.Reported herein is rhodium-catalyzed three-component asymmetric carboamidation between aryl boronic acid,achiral strain-activated symmetric bicyclic olefins bearing a prochiral C-N or N-N axis,and dioxazolones.The reaction proceeded effectively in excellent enantio-and diastereoselectivity under mild conditions to produce the bicyclic framework with six contiguous chiral centers as well as a N-N or C-N chiral axis.The reaction featured excellent functional group tolerance,chemoselectivity,and stereoselectivity.Mechanistic studies indicated that the coupling system proceeded via initial transmetalation,followed by stereo-determining migratory insertion into the olefin and electrophilic amidation.
基金Key Research and Development Program of Shanxi(Grant No.201803D421085)Shanxi Scholarship Council of China(Grant No.2019070)+1 种基金Shanxi Graduate Education Innovation Project(Grant No.2020BY095)State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(Grant No.201912)。
文摘The exploration of cost-effective,high-performance,and stable electrocatalysts for the hydrogen evolution reaction(HER)over wide pH range(0–14)is of paramount importance for future renewable energy conversion technologies.Regulation of electronic structure through doping vanadium atoms is a feasible construction strategy to enhance catalytic activities,electron transfer capability,and stability of the HER electrode.Herein,V-doped NiCoP nanosheets on carbon fiber paper(CFP)(denoted as Vx-NiCoP/CFP)were constructed by doping V modulation on NiCoP nanosheets on CFP and used for pH-universal HER.Benefiting from the abundant catalytic sites and optimized hydrogen binding thermodynamics,the resultant V15-NiCoP/CFP demonstrates a significantly improved HER catalytic activity,requiring overpotentials of 46.5,52.4,and 85.3 mV to reach a current density of 10 mA·cm^(−2)in 1 mol·L^(−1) KOH,0.5 mol·L^(−1) H_(2)SO_(4),and 1 mol·L^(−1) phosphate buffer solution(PBS)electrolytes,respectively.This proposed cation-doping strategy provides a new inspiration to rationally enhance or design new-type nonprecious metal-based,highly efficient,and pH-universal electrocatalysts for various energy conversion systems.