Single-atom site(SA)catalysts on N-doped carbon(CN)materials exhibit prominent performance for their active sites being M-Nx.Due to the commonly random doping behaviors of N species in these CN,it is a tough issue to ...Single-atom site(SA)catalysts on N-doped carbon(CN)materials exhibit prominent performance for their active sites being M-Nx.Due to the commonly random doping behaviors of N species in these CN,it is a tough issue to finely regulate their doping types and clarify their effect on the catalytic property of such catalysts.Herein,we report that the N-doping type in CN can be dominated as pyrrolic-N and pyridinic-N respectively through compounding with different metal oxides.It is found that the proportion of distinct doped N species in CN depends on the acidity and basicity of compounded metal oxide host.Owing to the coordination by pyrrolic-N,the SA Cu catalyst displays an enhanced activity(two-fold)for transfer hydrogenation of quinoline to access the valuable molecule tetrahydroquinoline with a good selectivity(99%)under mild conditions.The higher electron density of SA Cu species induced by the predominate pyrrolic-N coordination benefits the hydrogen transfer process and reduces the energy barrier of the hydrogenation pathway,which accounts for the improved catalytic effeciency.展开更多
Tailored synthesis of well-defined anatase TiO2-based crystals with exposed {001} facets has stimulated incessant research interest worldwide due to their scientific and technological importance. Herein, anatase nitro...Tailored synthesis of well-defined anatase TiO2-based crystals with exposed {001} facets has stimulated incessant research interest worldwide due to their scientific and technological importance. Herein, anatase nitrogen-doped TiO2 （N-TiO2） nanoparticles with exposed {001} facets deposited on the graphene （GR） sheets （N-TiO2-001/GR） were synthesized for the first time via a one-step solvothermal synthetic route using NH4F as the morphology-controlling agent. The experimental results exemplified that GR was uniformly covered with anatase N-TiO2 nanoparticles （10-17 nm）, exposing the {001} facets. The percentage of exposed {001} facets in the N-TiO2-001/GR nanocomposites was calculated to be ca. 35%. Also, a red shift in the absorption edge and a strong absorption in the visible light range were observed due to the formation of Ti-O-C bonds, resulting in the successful narrowing of the band gap from 3.23 to 2.9 eV. The photocatalytic activities of the as-prepared photocatalysts were evaluated for CO2 reduction to produce CH, in the presence of water vapor under ambient temperature and atmospheric pressure using a low-power 15 W energy-saving daylight lamp as the visible light source--in contrast to the most commonly employed high-power xenon lamps--which rendered the process economically and practically feasible. Among all the studied photocatalysts, the N-TiO2-001/GR nanocomposites exhibited the greatest CH4 yield of 3.70 p-mol＇gcatalyst 1, approxi- mately 11-fold higher activity than the TiO2-001. The enhancement of photocatalyfic performance was ascribed to the effective charge anti-recombination of graphene, high absorption of visible light region relative to the {101} facets. and high catalytic activity of {001} facets展开更多
The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous ...The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous N-doped carb on frameworks with tun able configurati ons and contents of N dopants,by using a secondary doping process via the treatment of N,N-dimethylformamide(DMF)solvent.The obtained mesoporous N-doped carbon(denoted as MNC-D)served as an efficient electrocatalyst for electroreduction of CO2 to CO.A high Faradaic efficiency of^92%and a partial current density for CO of-6.8 mA·cm^-2 were achieved at a potential of-0.58 V vs.RHE.Electrochemical analyses further revealed that the active sites within the N-doped carb on catalysts were the pyridinic N and defects gen erated by the DMF treatme nt,which enhan ced the activati on and adsorpti on CO2 molecules.Our study suggests a new approach to develop efficie nt carb on-based catalysts for potential scalable CO2 reduction reaction(CO2RR)to fuels and chemicals.展开更多
Iodine ion is one of the most indispensable anions in living organisms,particularly being an important substance for the synthesis of thyroid hormones.Curcumin is a yellow-orange polyphenol compound derived from the r...Iodine ion is one of the most indispensable anions in living organisms,particularly being an important substance for the synthesis of thyroid hormones.Curcumin is a yellow-orange polyphenol compound derived from the rhizome of Curcuma longa L.,which has been commonly used as a spice and natural coloring agent,food additives,cosmetics as well as Chinese medicine.However,excess curcumin may cause DNA inactivation,lead to a decrease in intracellular ATP levels,and trigger the tissue necrosis.Therefore,quantitative detection of iodine and curcumin is of great significance in the fields of food and life sciences.Herein,we develop nitrogen-doped fluorescent carbon dots(NCDs)as a multi-mechanism detection for iodide and curcumin in actual complex biological and food samples,which was prepared by a one-step solid-phase synthesis using tartaric acid and urea as precursors without adding any other reagents.An assembled NCDs-Hg^(2+) fluorescence-enhanced sensor for the quantitative detection of I^(-) was established based on a fluorescence“turn-off-on”mechanism in a linear range of 0.3-15μM with a detection limit of 69.4 nM and successfully quantified trace amounts of I^(-) in water samples and urine sample.Meanwhile,the as-synthesized NCDs also can be used as a fluorescent quenched sensor for curcumin detection based on the synergistic internal filtration effect(IFE)and static quenching,achieving a good linear range of 0.1-20μM with a satisfactory detection limit of 29.8 nM.These results indicate that carbon dots are potential sensing materials for iodine and curcumin detection for the good of our health.展开更多
The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively increasing.Herein,single-atomic copper sites supported on...The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively increasing.Herein,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu_(1)/NC)was prepared by coordination pyrolysis strategy.Remarkably,the Cu_(1)/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(vs.RHE)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol tolerance.Moreover,the Cu_(1)/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/C.Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu_(1)/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process.This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.展开更多
Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we ...Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon （HPNC） via acombination of salt template （ZnC12） and hard template （SiO2） as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC （IC= 1675 mAh g^-1 ）, a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.展开更多
Well-dispersed bimetallic NiRh nanoparticles （NPs） with different compositions supported on nitrogen-doped porous carbon （NPC） derived from metal-organic frameworks （ZIF-8） were synthesized through a co-reductio...Well-dispersed bimetallic NiRh nanoparticles （NPs） with different compositions supported on nitrogen-doped porous carbon （NPC） derived from metal-organic frameworks （ZIF-8） were synthesized through a co-reduction method. The NPC-900 supported NiRh catalyst exhibits the highest catalytic activity and 100% hydrogen selectivity toward hydrogen generation from hydrazine. These properties might be attributed to the high surface area and high graphitization of the NPC. This strategy may open up a new avenue for designing high-performance catalysts by utilizing NPC as a support to anchor active metal NPs for additional applications.展开更多
Electrocatalytic conversion of oxygen holds great potential for clean energy technologies, including water electrolysis, regenerative fuel cells, and rechargeable metal-air batteries. The development of highly efficie...Electrocatalytic conversion of oxygen holds great potential for clean energy technologies, including water electrolysis, regenerative fuel cells, and rechargeable metal-air batteries. The development of highly efficient and inexpensive oxygen electrocatalysts as replacements for precious metal-based catalysts is vitally important for large-scale practical application in the future. A bifunctional oxygen electrocatalyst based on FeCo nanoparticles/N-doped carbon core-shell spheres supported on N-doped graphene sheets was prepared via one-step pyrolysis of graphitic carbon nitride and acetylacetonates. The optimized product exhibited an oxygen electrode activity of 0.87 V and excellent durability. The remarkable performance is mainly attributed to the synergetic effect arising from the FeCo nanoparticles and N-doped carbon shell. This study introduces an inexpensive and simple way to develop highly active bifunctional oxygen electrocatalysts.展开更多
Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorpt...Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorption-desorption,thermogravimetry,high-resolution transmission electron microscopy,and Raman and X-ray photoelectron spectroscopy.The selective oxidation of ethylbenzene with molecular oxygen under a solvent-free condition was carried out to explore the catalytic performance of the M-N-Cs,which exhibited different catalytic performance.That was ascribed to the difference in M（Co,Fe,Mn） and different graphitization degree forming during the heating process,in which M（Co,Fe,Mn） might have different catalytic activity on the formation of the M-N-C catalyst.All the M-N-C composites had remarkable recyclability in the selective oxidation of ethylbenzene.展开更多
Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology l...Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology lies in seeking eco-efficient synthetic processes to the design of suitable anode materials.Herein,a spherical sponge-like carbon superstructure(NCS)assembled by 2D nanosheets is rationally and efficiently designed for K+storage.The optimized NCS electrode exhibits an outstanding rate capability,high reversible specific capacity(250 mAh g^(−1) at 200 mA g^(−1) after 300 cycles),and promising cycling performance(205 mAh g^(−1) at 1000 mA g^(−1) after 2000 cycles).The superior performance can be attributed to the unique robust spherical structure and 3D electrical transfer network together with nitrogen-rich nanosheets.Moreover,the regulation of the nitrogen doping types and morphology of NCS-5 is also discussed in detail based on the experiments results and density functional theory calculations.This strategy for manipulating the structure and properties of 3D materials is expected to meet the grand challenges for advanced carbon materials as high-performance PIB anodes in practical applications.展开更多
Here,we successfully developed nano structured PtNi particles supported on n itroge rrdoped carbon(NC),which were obtai ned by carbon izati on of metal-organic frameworks under different temperatures,forming the nano-...Here,we successfully developed nano structured PtNi particles supported on n itroge rrdoped carbon(NC),which were obtai ned by carbon izati on of metal-organic frameworks under different temperatures,forming the nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 and nano-PtNi/NC-1000 catalysts.For hydrosilylation of 1-octene,we found that the nano-PtNi/NC-1000 catalyst exhibits higher activity for anti-Markovnikov hydrosilylation of 1-octene than those of nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 catalysts.Experiments have verified that benefiting from obvious charge transfer from nano-PtNi particles to NC support carbonized at 1,000℃,the nano-PtNi/NC-1000 catalyst achieved almost complete conversion and produce exclusive adduct for anti-Markovnikov hydrosilylation of 1-octene.Importantly,the nano-PtNi/NC-1000 catalyst exhibited good reusability for the hydrosilylation reaction.This work provides a new path to optimize electronic structure of catalysts by support modification to enhance electron transfer between metal active species and supports for highly catalytic performance.展开更多
A Co-based metal-organic framework （Co-MOF） with a unique three-dimensional starfish-like nanostructure was successfully synthesized using a simple ultrasonic method. After subsequent carbonization and oxidation, a ...A Co-based metal-organic framework （Co-MOF） with a unique three-dimensional starfish-like nanostructure was successfully synthesized using a simple ultrasonic method. After subsequent carbonization and oxidation, a nanocomposite of nitrogen-doped carbon with a Co3O4 coating （Co3O4@N-C） with a porous starfish-like nanostructure was obtained. The final hybrid exhibited excellent lithium storage performance when evaluated as an anode material in a lithiumion battery. A remarkable and stable discharge capacity of 795 mAh·g^-1 was maintained at 0.5 A·g^-1 after 300 cycles. Excellent rate capability was also obtained. In addition, a full Co3O4@N-C/LiFePO4 battery displayed stable capacity retention of 95% after 100 cycles. This excellent lithium storage performance is attributed to the unique porous starfish-like structure, which effectively buffers the volume expansion that occurs during Li^＋ insertion/deinsertion. Meanwhile, the nitrogendoped carbon coating enhances the electrical conductivity and provides a buffer layer to accommodate the volume change and accelerate the formation of a stable solid electrolyte interface layer.展开更多
基金supported by the National Key R&D Program of China(Nos.2018YFA0702003 and 2016YFA0202801)the National Natural Science Foundation of China(Nos.21890383,21671117,21871159,and 21901135)+2 种基金the National Postdoctoral Program for Innovative Talents,the Shuimu Tsinghua Scholar,Science and Technology Key Project of Guangdong Province of China(No.2020B010188002)Beijing Municipal Science&Technology Commission(No.Z191100007219003)We thank the BL14W1 station in Shanghai Synchrotron Radiation Facility(SSRF)and 1W1B station for XAFS measurement in Beijing Synchrotron Radiation Facility(BSRF).
文摘Single-atom site(SA)catalysts on N-doped carbon(CN)materials exhibit prominent performance for their active sites being M-Nx.Due to the commonly random doping behaviors of N species in these CN,it is a tough issue to finely regulate their doping types and clarify their effect on the catalytic property of such catalysts.Herein,we report that the N-doping type in CN can be dominated as pyrrolic-N and pyridinic-N respectively through compounding with different metal oxides.It is found that the proportion of distinct doped N species in CN depends on the acidity and basicity of compounded metal oxide host.Owing to the coordination by pyrrolic-N,the SA Cu catalyst displays an enhanced activity(two-fold)for transfer hydrogenation of quinoline to access the valuable molecule tetrahydroquinoline with a good selectivity(99%)under mild conditions.The higher electron density of SA Cu species induced by the predominate pyrrolic-N coordination benefits the hydrogen transfer process and reduces the energy barrier of the hydrogenation pathway,which accounts for the improved catalytic effeciency.
文摘Tailored synthesis of well-defined anatase TiO2-based crystals with exposed {001} facets has stimulated incessant research interest worldwide due to their scientific and technological importance. Herein, anatase nitrogen-doped TiO2 （N-TiO2） nanoparticles with exposed {001} facets deposited on the graphene （GR） sheets （N-TiO2-001/GR） were synthesized for the first time via a one-step solvothermal synthetic route using NH4F as the morphology-controlling agent. The experimental results exemplified that GR was uniformly covered with anatase N-TiO2 nanoparticles （10-17 nm）, exposing the {001} facets. The percentage of exposed {001} facets in the N-TiO2-001/GR nanocomposites was calculated to be ca. 35%. Also, a red shift in the absorption edge and a strong absorption in the visible light range were observed due to the formation of Ti-O-C bonds, resulting in the successful narrowing of the band gap from 3.23 to 2.9 eV. The photocatalytic activities of the as-prepared photocatalysts were evaluated for CO2 reduction to produce CH, in the presence of water vapor under ambient temperature and atmospheric pressure using a low-power 15 W energy-saving daylight lamp as the visible light source--in contrast to the most commonly employed high-power xenon lamps--which rendered the process economically and practically feasible. Among all the studied photocatalysts, the N-TiO2-001/GR nanocomposites exhibited the greatest CH4 yield of 3.70 p-mol＇gcatalyst 1, approxi- mately 11-fold higher activity than the TiO2-001. The enhancement of photocatalyfic performance was ascribed to the effective charge anti-recombination of graphene, high absorption of visible light region relative to the {101} facets. and high catalytic activity of {001} facets
基金We thank the following funding agencies for supporting this work:the National Key Research and Development Program of China(Nos.2017YFA0206901 and 2018YFA0209401)the National Natural Science Foundation of China(No.21773036)+1 种基金the Science and Technology Commission of Shanghai Municipality(Nos.17JC1402000 and 19XD1420400)the Innovation Program of Shanghai Municipal Education Commission(No.2019-01-07-00-07-E00045).
文摘The capability of electrocatalytic reducti on of carbon dioxide(CO2)using nitrogen(N)-doped carb on strongly depe nds on the N-dopi ng level and their types.In this work,we developed a strategy to generate mesoporous N-doped carb on frameworks with tun able configurati ons and contents of N dopants,by using a secondary doping process via the treatment of N,N-dimethylformamide(DMF)solvent.The obtained mesoporous N-doped carbon(denoted as MNC-D)served as an efficient electrocatalyst for electroreduction of CO2 to CO.A high Faradaic efficiency of^92%and a partial current density for CO of-6.8 mA·cm^-2 were achieved at a potential of-0.58 V vs.RHE.Electrochemical analyses further revealed that the active sites within the N-doped carb on catalysts were the pyridinic N and defects gen erated by the DMF treatme nt,which enhan ced the activati on and adsorpti on CO2 molecules.Our study suggests a new approach to develop efficie nt carb on-based catalysts for potential scalable CO2 reduction reaction(CO2RR)to fuels and chemicals.
基金Financial supports from the XingLiao Talent Project Grants(No.XLYC1902076)the University of Science and Technology Liaoning Talent Project Grants(No.601010302)are highly appreciated.
文摘Iodine ion is one of the most indispensable anions in living organisms,particularly being an important substance for the synthesis of thyroid hormones.Curcumin is a yellow-orange polyphenol compound derived from the rhizome of Curcuma longa L.,which has been commonly used as a spice and natural coloring agent,food additives,cosmetics as well as Chinese medicine.However,excess curcumin may cause DNA inactivation,lead to a decrease in intracellular ATP levels,and trigger the tissue necrosis.Therefore,quantitative detection of iodine and curcumin is of great significance in the fields of food and life sciences.Herein,we develop nitrogen-doped fluorescent carbon dots(NCDs)as a multi-mechanism detection for iodide and curcumin in actual complex biological and food samples,which was prepared by a one-step solid-phase synthesis using tartaric acid and urea as precursors without adding any other reagents.An assembled NCDs-Hg^(2+) fluorescence-enhanced sensor for the quantitative detection of I^(-) was established based on a fluorescence“turn-off-on”mechanism in a linear range of 0.3-15μM with a detection limit of 69.4 nM and successfully quantified trace amounts of I^(-) in water samples and urine sample.Meanwhile,the as-synthesized NCDs also can be used as a fluorescent quenched sensor for curcumin detection based on the synergistic internal filtration effect(IFE)and static quenching,achieving a good linear range of 0.1-20μM with a satisfactory detection limit of 29.8 nM.These results indicate that carbon dots are potential sensing materials for iodine and curcumin detection for the good of our health.
基金the National Natural Science Foundation of China(Nos.21804319,21971002)the Natural Science Foundation of Anhui province(Nos.1908085QB45 and 2008085QB81)the Education Departm ent of Anhui Province Foundation(No.KJ2019A0503).We thank the BL14W1 station in Shanghai Synchrotron Radiation Facility(SSRF)and 1W1B station for XAFS measurement in Beijing Synchrotron Radiation Facility(BSRF).The calculations in this paper have been done on the supercomputing system of the National Supercomputing Center in Changsha.
文摘The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively increasing.Herein,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu_(1)/NC)was prepared by coordination pyrolysis strategy.Remarkably,the Cu_(1)/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(vs.RHE)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol tolerance.Moreover,the Cu_(1)/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/C.Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu_(1)/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process.This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.
基金financially supported by the National Key Research and Development Program of China (2016YFB0101202)the NSFC of China (Grants 91534205,21436003 and 21576031)Graduate Research and Innovation Foundation of Chongqing China (Grant No.CYB17021)
文摘Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon （HPNC） via acombination of salt template （ZnC12） and hard template （SiO2） as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC （IC= 1675 mAh g^-1 ）, a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.
基金Acknowledgements This work was financially supported by the National Natural Science Foundation of China （Nos. 21201134 and 21571145）, the Natural Science Foundation of Jiangsu Province （No. BK20130370）, the Natural Science Foundation of Hubei Province （No. 2013CFB288）, the Creative Research Groups of Hubei Province （No. 2014CFA007）, and Large-scale Instrument and Equipment Sharing Foundation of Wuhan University.
文摘Well-dispersed bimetallic NiRh nanoparticles （NPs） with different compositions supported on nitrogen-doped porous carbon （NPC） derived from metal-organic frameworks （ZIF-8） were synthesized through a co-reduction method. The NPC-900 supported NiRh catalyst exhibits the highest catalytic activity and 100% hydrogen selectivity toward hydrogen generation from hydrazine. These properties might be attributed to the high surface area and high graphitization of the NPC. This strategy may open up a new avenue for designing high-performance catalysts by utilizing NPC as a support to anchor active metal NPs for additional applications.
基金The work was financially supported by the National Natural Science Foundation of China （No. 51173202）, Innovation Foundation for Superior Postgraduate of National University of Defense Technology, Hunan Provincial Innovation Foundation for Postgraduate, Research Project of NUDT （No. ZK16-03-32）, Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province and Aid Program for Innovative Group of National University of Defense Technology.
文摘Electrocatalytic conversion of oxygen holds great potential for clean energy technologies, including water electrolysis, regenerative fuel cells, and rechargeable metal-air batteries. The development of highly efficient and inexpensive oxygen electrocatalysts as replacements for precious metal-based catalysts is vitally important for large-scale practical application in the future. A bifunctional oxygen electrocatalyst based on FeCo nanoparticles/N-doped carbon core-shell spheres supported on N-doped graphene sheets was prepared via one-step pyrolysis of graphitic carbon nitride and acetylacetonates. The optimized product exhibited an oxygen electrode activity of 0.87 V and excellent durability. The remarkable performance is mainly attributed to the synergetic effect arising from the FeCo nanoparticles and N-doped carbon shell. This study introduces an inexpensive and simple way to develop highly active bifunctional oxygen electrocatalysts.
基金supported by the National Natural Science Foundation of China (21103045, 1210040, 1103312)State Key Laboratory of Heavy Oil at China University of Petroleum (SKCHOP201504)Key Laboratory of Mineralogy and Metallogeny of the Chinese Academy of Sciences at Guangzhou Institute of Geochemistry(KLMM20150103)~~
文摘Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorption-desorption,thermogravimetry,high-resolution transmission electron microscopy,and Raman and X-ray photoelectron spectroscopy.The selective oxidation of ethylbenzene with molecular oxygen under a solvent-free condition was carried out to explore the catalytic performance of the M-N-Cs,which exhibited different catalytic performance.That was ascribed to the difference in M（Co,Fe,Mn） and different graphitization degree forming during the heating process,in which M（Co,Fe,Mn） might have different catalytic activity on the formation of the M-N-C catalyst.All the M-N-C composites had remarkable recyclability in the selective oxidation of ethylbenzene.
基金the National Natural Science Foundation of China(Grant Nos.51772086,51572078,51872087,and 11605053)the Natural Science Foundation of Hunan Province(Grant No.2018JJ2038)the Hunan Provincial Natural Science Foundation of China(Grant No.2017JJ3052)。
文摘Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology lies in seeking eco-efficient synthetic processes to the design of suitable anode materials.Herein,a spherical sponge-like carbon superstructure(NCS)assembled by 2D nanosheets is rationally and efficiently designed for K+storage.The optimized NCS electrode exhibits an outstanding rate capability,high reversible specific capacity(250 mAh g^(−1) at 200 mA g^(−1) after 300 cycles),and promising cycling performance(205 mAh g^(−1) at 1000 mA g^(−1) after 2000 cycles).The superior performance can be attributed to the unique robust spherical structure and 3D electrical transfer network together with nitrogen-rich nanosheets.Moreover,the regulation of the nitrogen doping types and morphology of NCS-5 is also discussed in detail based on the experiments results and density functional theory calculations.This strategy for manipulating the structure and properties of 3D materials is expected to meet the grand challenges for advanced carbon materials as high-performance PIB anodes in practical applications.
基金This work was supported by the National Postdoctoral Program for Innovative Talents(No.BX20180160)the China Postdoctoral Science Foundation(No.2018M640113)+1 种基金the National Natural Science Foundation of China(No.21890383)the Industrial Science and Technology Tackling Program of Shaanxi Province(No.2016GY-245).
文摘Here,we successfully developed nano structured PtNi particles supported on n itroge rrdoped carbon(NC),which were obtai ned by carbon izati on of metal-organic frameworks under different temperatures,forming the nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 and nano-PtNi/NC-1000 catalysts.For hydrosilylation of 1-octene,we found that the nano-PtNi/NC-1000 catalyst exhibits higher activity for anti-Markovnikov hydrosilylation of 1-octene than those of nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 catalysts.Experiments have verified that benefiting from obvious charge transfer from nano-PtNi particles to NC support carbonized at 1,000℃,the nano-PtNi/NC-1000 catalyst achieved almost complete conversion and produce exclusive adduct for anti-Markovnikov hydrosilylation of 1-octene.Importantly,the nano-PtNi/NC-1000 catalyst exhibited good reusability for the hydrosilylation reaction.This work provides a new path to optimize electronic structure of catalysts by support modification to enhance electron transfer between metal active species and supports for highly catalytic performance.
基金Acknowledgements This work is supported by the National Natural Science Foundation of China （Nos. 21173001 and 21371003） and Anhui Province Key Laboratory of Environment-Friendly Polymer Materials.
文摘A Co-based metal-organic framework （Co-MOF） with a unique three-dimensional starfish-like nanostructure was successfully synthesized using a simple ultrasonic method. After subsequent carbonization and oxidation, a nanocomposite of nitrogen-doped carbon with a Co3O4 coating （Co3O4@N-C） with a porous starfish-like nanostructure was obtained. The final hybrid exhibited excellent lithium storage performance when evaluated as an anode material in a lithiumion battery. A remarkable and stable discharge capacity of 795 mAh·g^-1 was maintained at 0.5 A·g^-1 after 300 cycles. Excellent rate capability was also obtained. In addition, a full Co3O4@N-C/LiFePO4 battery displayed stable capacity retention of 95% after 100 cycles. This excellent lithium storage performance is attributed to the unique porous starfish-like structure, which effectively buffers the volume expansion that occurs during Li^＋ insertion/deinsertion. Meanwhile, the nitrogendoped carbon coating enhances the electrical conductivity and provides a buffer layer to accommodate the volume change and accelerate the formation of a stable solid electrolyte interface layer.
