The rational synthesis of a two-dimensional(2D)porous aromatic framework(PAF)with a controllable growth direction remains a challenge to overcome the limitation of traditional stacked 2D materials.Herein,a step-growth...The rational synthesis of a two-dimensional(2D)porous aromatic framework(PAF)with a controllable growth direction remains a challenge to overcome the limitation of traditional stacked 2D materials.Herein,a step-growth strategy is developed to fabricate a vertically oriented nitrogen-rich porous aromatic framework on graphene oxide(V-PAF-GO)using monolayer benzidine-functionalized GO(BZ-GO)as a molecular pillar.Then,the confined Co nanoparticle(NP)catalysts are synthesized by encapsulating ultra-small Co into the slit pores of V-PAF-GO.Due to the high nitrogen content,large specific surface area,and adequate slit pores,the optimized vertical nanocomposites V-PAF-GO provide abundant anchoring sites for metal NPs,leading to ultrafine Co NPs(1.4 nm).The resultant Co/V-PAF-GO catalyst shows an extraordinary catalytic activity for ammonia borane(AB)methanolysis,yielding a turnover frequency value of 47.6 min−1 at 25°C,comparable to the most effective non-noble-metal catalysts ever reported for AB methanolysis.Experimental and density functional theory studies demonstrate that the electron-donating effect of N species of PAF positively corresponds to the low barrier in methanol molecule activation,and the cleavage of the O–H bond in CH3OH has been proven to be the rate-determining step for AB methanolysis.This work presents a versatile step-growth strategy to prepare a vertically oriented PAF on GO to solve the stacking problem of 2D materials,which will be used to fabricate other novel 2D or 2D–2D materials with controllable orientation for various applications.展开更多
Expression of transient receptor potential （TRP） channels is widespread with transcripts distributed throughout the brain. All TRP channel subunits are activated following phospholipase C activation and form cation-...Expression of transient receptor potential （TRP） channels is widespread with transcripts distributed throughout the brain. All TRP channel subunits are activated following phospholipase C activation and form cation-selective ion channels. Previous studies examining the existence of TRP channels in hippocampal CA1 pyramidal neurons were based on cultured neurons. Therefore, their relevance for living tissue remains unclear. In the present study, patch-clamp recordings were conducted from CA1 pyramidal neurons in hippocampal slices from 7-day-old rats. Whole-cell currents were obtained from CA1 hippocampal neurons with potentiation effects of 2-aminoethoxydiphenyl borate and lanthanum, revealing that recorded experimental currents were characteristic TRP-like channel currents. Identification of rat hippocampal mRNA transcripts of TRPC4, TRPC5, TRPV1, TRPV2, and TRPV3 channels further verified the expression of characteristic TRP-like channels on rat CA1 hippocampal neurons.展开更多
Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hy...Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hydrogen economy.In this work,ultrafine and well-dispersed bimetallic NiPt nanoparticles(3.4 nm) were successfully immobilized on Y_(2)O_(3)-functionalized graphene(Y_(2)O_(3)/rGO) without any surfactant by a simple liquid impregnation approach.It is firstly found that integration of graphene and Y_(2)O_(3) not only can facilitate the formation of ultrafine NiPt nanoparticles(NPs),but also can effectively modulate the electronic structure of NiPt NPs,thereby boosting the catalytic performance.Compared with NiPt/Y_(2)O_(3) and NiPt/rGO,the NiPt/Y_(2)O_(3)/rGO nanocomposites(NCs) show remarkable enhanced catalytic efficiency for hydrogen production from N_(2)H_(4)-H_(2)O.In particular,the optimized Ni_(0.6)Pt_(0.4/)Y_(2)O_(3)/rGO NCs display the best catalytic efficiency and 100% H_(2) selectivity for N_(2)H_(4)-H_(2)O dehydrogenation,providing a turnover frequency(TOF) of2182 h^(-1) at 323 K,which is among the highest values ever reported.Moreover,the Ni_(0.6)Pt_(0.4)/Y_(2)O_(3)/rGO NCs also exhibit an excellent catalytic performance(TOF=3191 h^(-1)) and 100% H_(2) selectively for N_(2)H_(4)BH_(3)dehydrogenation at 323 K.The outstanding catalytic results obtained provide more possibilities for the potential applications of N_(2)H_(4)·H_(2)O and N_(2)H_(4)BH_(3) as promising chemical hydrogen storage materials.展开更多
Well-defined polycarbonate diol was successfully synthesized through a strategy using a combination of organocatalyst and water.Such strategy was less developed in organocatalyzed polymerization and frequently regarde...Well-defined polycarbonate diol was successfully synthesized through a strategy using a combination of organocatalyst and water.Such strategy was less developed in organocatalyzed polymerization and frequently regarded as side reactions.Herein,one-component phosphonium borane Lewis pairs PB1-PB8 were successfully applied in the copolymerization of CO_(2) and cyclohexene oxide(CHO)to generate poly(CHO-alt-CO_(2))carbonate(PCHC).Parameters of linker length and counter anion effects on the catalyst activity were investigated.It was found that Lewis pair PB3 served as a dual initiator and catalyst in the copolymerization of CHO and CO_(2) with or without the presence of water.In contrast,Lewis pair PB8 can serve as a true catalyst for the preparation of well-definedα,ω-hydroxyl PCHC diols.This was achieved by introducing a labile CF3COO group as counter anion through anion exchange reaction while water molecules acted as chain transfer agents.The function of trifluoroacetate group in the polymerization process was investigated in detail and possible mechanism was proposed.Upon changing the amount of water and catalyst loading,PCHC diols with varied molecular weight(1.5 kg/mol to 7.5 kg/mol),low dispersities(D<1.2)and carbonate content(>99%)could be easily obtained.The low molecular weight PCHC diol was used as a bifunctional macroinitiator for the ring-opening polymerization of L-lactide(LLA)to afford ABA triblock copolymer in one-pot synthesis.展开更多
Ammonia borane(NH3BH3,AB)holds promise for chemical storage of hydrogen.However,designing superb and low-cost photocatalyst to drive hydrogen evolution from AB under visible light irradiation is highly desirable but r...Ammonia borane(NH3BH3,AB)holds promise for chemical storage of hydrogen.However,designing superb and low-cost photocatalyst to drive hydrogen evolution from AB under visible light irradiation is highly desirable but remains a major challenge for promoting the practical utilization of AB.Herein,we demonstrated a heterostructure photocatalyst consisting of zerodimensional(0D)CoP nanoparticles immobilized on two-dimensional(2D)Co_(2)P nanosheets(CoP/Co_(2)Ps)as a high-performance and low-cost catalyst for hydrogen evolution from AB hydrolysis,in which 0D/2D heterostructure was synthesized using the saltinduced phase transformation strategy.Interestingly,the optimized CoP/Co_(2)Ps exhibit a robust H_(2) evolution rate of 32.1 L∙min^(−1)∙g_(Co)^(−1),corresponding to a turnover frequency(TOF)value of 64.1 min^(−1),being among the highest TOF for non-noblemetal catalysts ever reported,even outperforming some precious metal catalysts.This work not only opens a new avenue to accelerate hydrogen evolution from AB by regulating the electronic structures of heterointerfaces,but also provides a novel strategy for the construction of precious-metal-free materials for hydrogen-related energy catalysis in the future.展开更多
Herein,we first describe the physical mixture of Cu(OH)_2/Fe(OH)_3 as a composite catalyst precursor for the dehydrogenation of ammonia borane(AB)in methanol.During the initial period of catalytic reaction,Cu nanopart...Herein,we first describe the physical mixture of Cu(OH)_2/Fe(OH)_3 as a composite catalyst precursor for the dehydrogenation of ammonia borane(AB)in methanol.During the initial period of catalytic reaction,Cu nanoparticles were formed in-situ.The catalytic activity of Cu nanoparticles can be significantly enhanced with the assistance of Fe species and OH~à.A maximum turnover frequency(TOF)of 50.3 mol_(H2)mol^(à1)_(total metal)min^(à1)(135.6 mol_(H2)mol_(Cu)^(à1)min^(à1))was achieved at ambient temperature,which is superior to those of previously reported Fe or Cu based systems.展开更多
Ge-based selenides have attracted extensive attention as promising candidates for future optoelectronic applications.Despite great progress has been achieved,the controlled synthesis of GeSe2and GeSe nanostructures an...Ge-based selenides have attracted extensive attention as promising candidates for future optoelectronic applications.Despite great progress has been achieved,the controlled synthesis of GeSe2and GeSe nanostructures and understanding the relative growth mechanisms of them are still lacking.Herein,monodispersed GeSe_(2) nanoflowers with a diameter of~4μm and highly uniform GeSe nanoparticles with a lateral size of~100 nm are presented by using a colloidal synthetic method.It is found that borane tert-butylamine complex(TBAB)plays an important role in determining the Ge-Se crystal phases due to its moderately reducibility.Furthermore,the coexistence of GeSe_(2) and GeSe phases can also be acquired by precisely controlling the amount of TBAB.In brief,this work provides both new insights of the phase control of Gebased selenides by liquid-phase method and a practical means of producing well-controlled germanium selenide nanostructures.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:22162014 and 22162013Natural Science Foundation of Jiangxi Province of China,Grant/Award Number:20212ACB204009+1 种基金Sponsored Program for Academic and Technical Leaders of Major Disciplines of Jiangxi Province of China,Grant/Award Number:20212BCJL23059Doctoral Research Foundation Project of Tongren University,Grant/Award Number:trxyDH2204。
文摘The rational synthesis of a two-dimensional(2D)porous aromatic framework(PAF)with a controllable growth direction remains a challenge to overcome the limitation of traditional stacked 2D materials.Herein,a step-growth strategy is developed to fabricate a vertically oriented nitrogen-rich porous aromatic framework on graphene oxide(V-PAF-GO)using monolayer benzidine-functionalized GO(BZ-GO)as a molecular pillar.Then,the confined Co nanoparticle(NP)catalysts are synthesized by encapsulating ultra-small Co into the slit pores of V-PAF-GO.Due to the high nitrogen content,large specific surface area,and adequate slit pores,the optimized vertical nanocomposites V-PAF-GO provide abundant anchoring sites for metal NPs,leading to ultrafine Co NPs(1.4 nm).The resultant Co/V-PAF-GO catalyst shows an extraordinary catalytic activity for ammonia borane(AB)methanolysis,yielding a turnover frequency value of 47.6 min−1 at 25°C,comparable to the most effective non-noble-metal catalysts ever reported for AB methanolysis.Experimental and density functional theory studies demonstrate that the electron-donating effect of N species of PAF positively corresponds to the low barrier in methanol molecule activation,and the cleavage of the O–H bond in CH3OH has been proven to be the rate-determining step for AB methanolysis.This work presents a versatile step-growth strategy to prepare a vertically oriented PAF on GO to solve the stacking problem of 2D materials,which will be used to fabricate other novel 2D or 2D–2D materials with controllable orientation for various applications.
基金the Medical Scientific Research Foundation of Guangdong Province,No.A2006372the National Natural Science Foundation of China,No.U0632007+3 种基金the Natural Science Foundation of Guangdong Province,No.9351051501000003the Major Program of Natural Science Research of Higher Learning School of Guangdong Province,No.06Z007the Key Project of Science and Technology of Guangzhou City,No.2007zl-E0081the Program for Changjiang Scholars and Innovative Research Team,No.IRT0731
文摘Expression of transient receptor potential （TRP） channels is widespread with transcripts distributed throughout the brain. All TRP channel subunits are activated following phospholipase C activation and form cation-selective ion channels. Previous studies examining the existence of TRP channels in hippocampal CA1 pyramidal neurons were based on cultured neurons. Therefore, their relevance for living tissue remains unclear. In the present study, patch-clamp recordings were conducted from CA1 pyramidal neurons in hippocampal slices from 7-day-old rats. Whole-cell currents were obtained from CA1 hippocampal neurons with potentiation effects of 2-aminoethoxydiphenyl borate and lanthanum, revealing that recorded experimental currents were characteristic TRP-like channel currents. Identification of rat hippocampal mRNA transcripts of TRPC4, TRPC5, TRPV1, TRPV2, and TRPV3 channels further verified the expression of characteristic TRP-like channels on rat CA1 hippocampal neurons.
基金financially supported by the National Natural Science Foundation of China (Nos. 22162013 and 22162014)Natural Science Foundation of Jiangxi Province (No. 20212ACB204009)+2 种基金the Program of the Academic and Technical Leaders of Major Disciplines of Jiangxi Province (No. 20212BCJL23059)the Thousand Talents Plan of Jiangxi Provincethe Open Project Program of State-Province Joint Engineering Laboratory of Zeolite Membrane Materials of China (No. SPJELZMM-202210)。
文摘Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hydrogen economy.In this work,ultrafine and well-dispersed bimetallic NiPt nanoparticles(3.4 nm) were successfully immobilized on Y_(2)O_(3)-functionalized graphene(Y_(2)O_(3)/rGO) without any surfactant by a simple liquid impregnation approach.It is firstly found that integration of graphene and Y_(2)O_(3) not only can facilitate the formation of ultrafine NiPt nanoparticles(NPs),but also can effectively modulate the electronic structure of NiPt NPs,thereby boosting the catalytic performance.Compared with NiPt/Y_(2)O_(3) and NiPt/rGO,the NiPt/Y_(2)O_(3)/rGO nanocomposites(NCs) show remarkable enhanced catalytic efficiency for hydrogen production from N_(2)H_(4)-H_(2)O.In particular,the optimized Ni_(0.6)Pt_(0.4/)Y_(2)O_(3)/rGO NCs display the best catalytic efficiency and 100% H_(2) selectivity for N_(2)H_(4)-H_(2)O dehydrogenation,providing a turnover frequency(TOF) of2182 h^(-1) at 323 K,which is among the highest values ever reported.Moreover,the Ni_(0.6)Pt_(0.4)/Y_(2)O_(3)/rGO NCs also exhibit an excellent catalytic performance(TOF=3191 h^(-1)) and 100% H_(2) selectively for N_(2)H_(4)BH_(3)dehydrogenation at 323 K.The outstanding catalytic results obtained provide more possibilities for the potential applications of N_(2)H_(4)·H_(2)O and N_(2)H_(4)BH_(3) as promising chemical hydrogen storage materials.
基金financially supported by the National Key R&D Program of China(No.2021YFA1501600)the National Natural Science Foundation of China(Nos.22175105 and 22031005)。
文摘Well-defined polycarbonate diol was successfully synthesized through a strategy using a combination of organocatalyst and water.Such strategy was less developed in organocatalyzed polymerization and frequently regarded as side reactions.Herein,one-component phosphonium borane Lewis pairs PB1-PB8 were successfully applied in the copolymerization of CO_(2) and cyclohexene oxide(CHO)to generate poly(CHO-alt-CO_(2))carbonate(PCHC).Parameters of linker length and counter anion effects on the catalyst activity were investigated.It was found that Lewis pair PB3 served as a dual initiator and catalyst in the copolymerization of CHO and CO_(2) with or without the presence of water.In contrast,Lewis pair PB8 can serve as a true catalyst for the preparation of well-definedα,ω-hydroxyl PCHC diols.This was achieved by introducing a labile CF3COO group as counter anion through anion exchange reaction while water molecules acted as chain transfer agents.The function of trifluoroacetate group in the polymerization process was investigated in detail and possible mechanism was proposed.Upon changing the amount of water and catalyst loading,PCHC diols with varied molecular weight(1.5 kg/mol to 7.5 kg/mol),low dispersities(D<1.2)and carbonate content(>99%)could be easily obtained.The low molecular weight PCHC diol was used as a bifunctional macroinitiator for the ring-opening polymerization of L-lactide(LLA)to afford ABA triblock copolymer in one-pot synthesis.
基金the National Natural Science Foundation of China(Nos.22108238,21878259,22278353,and U22A20408)the Zhejiang Provincial Natural Science Foundation of China(Nos.LR18B060001 and Z23B060009)China Postdoctoral Science Foundation(Nos.2020T130580,PC2022046,and 2019M662060).
文摘Ammonia borane(NH3BH3,AB)holds promise for chemical storage of hydrogen.However,designing superb and low-cost photocatalyst to drive hydrogen evolution from AB under visible light irradiation is highly desirable but remains a major challenge for promoting the practical utilization of AB.Herein,we demonstrated a heterostructure photocatalyst consisting of zerodimensional(0D)CoP nanoparticles immobilized on two-dimensional(2D)Co_(2)P nanosheets(CoP/Co_(2)Ps)as a high-performance and low-cost catalyst for hydrogen evolution from AB hydrolysis,in which 0D/2D heterostructure was synthesized using the saltinduced phase transformation strategy.Interestingly,the optimized CoP/Co_(2)Ps exhibit a robust H_(2) evolution rate of 32.1 L∙min^(−1)∙g_(Co)^(−1),corresponding to a turnover frequency(TOF)value of 64.1 min^(−1),being among the highest TOF for non-noblemetal catalysts ever reported,even outperforming some precious metal catalysts.This work not only opens a new avenue to accelerate hydrogen evolution from AB by regulating the electronic structures of heterointerfaces,but also provides a novel strategy for the construction of precious-metal-free materials for hydrogen-related energy catalysis in the future.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17000000)the National Natural Science Foundation of China (21773275)
文摘Herein,we first describe the physical mixture of Cu(OH)_2/Fe(OH)_3 as a composite catalyst precursor for the dehydrogenation of ammonia borane(AB)in methanol.During the initial period of catalytic reaction,Cu nanoparticles were formed in-situ.The catalytic activity of Cu nanoparticles can be significantly enhanced with the assistance of Fe species and OH~à.A maximum turnover frequency(TOF)of 50.3 mol_(H2)mol^(à1)_(total metal)min^(à1)(135.6 mol_(H2)mol_(Cu)^(à1)min^(à1))was achieved at ambient temperature,which is superior to those of previously reported Fe or Cu based systems.
基金supported by the National Natural Science Foundation of China(Nos.51971122 and 12174237)Technological Innovation Programs of Higher Education Institutions in Shanxi(No.2021Y440)。
文摘Ge-based selenides have attracted extensive attention as promising candidates for future optoelectronic applications.Despite great progress has been achieved,the controlled synthesis of GeSe2and GeSe nanostructures and understanding the relative growth mechanisms of them are still lacking.Herein,monodispersed GeSe_(2) nanoflowers with a diameter of~4μm and highly uniform GeSe nanoparticles with a lateral size of~100 nm are presented by using a colloidal synthetic method.It is found that borane tert-butylamine complex(TBAB)plays an important role in determining the Ge-Se crystal phases due to its moderately reducibility.Furthermore,the coexistence of GeSe_(2) and GeSe phases can also be acquired by precisely controlling the amount of TBAB.In brief,this work provides both new insights of the phase control of Gebased selenides by liquid-phase method and a practical means of producing well-controlled germanium selenide nanostructures.
