With high surface area,open porosity and high efficiency,a catalyst was prepared and firstly employed in electrocatalytic reduction of CO2 and electrosynthesis of dimethyl carbonate（DMC）.The electrochemical property...With high surface area,open porosity and high efficiency,a catalyst was prepared and firstly employed in electrocatalytic reduction of CO2 and electrosynthesis of dimethyl carbonate（DMC）.The electrochemical property for electrocatalytic reduction of CO2 in ionic liquid was studied by cyclic voltammogram（CV）.The effects of various reaction variables like temperature,working potential and cathode materials on the electrocatalytic performance were also investigated.80%yield of DMC was obtained under the optimal reaction conditions.展开更多
Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synth...Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synthesis and low yield of nanoporous silicon limit its practical application.Here,we develop a scalable,low-cost top-down process of controlled oxidation of Mg2Si in the air,followed by HCl removal of MgO to generate nanoporous silicon without the use of HF.By controlling the synthesis conditions,the oxygen content,grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints.In situ environmental transmission electron microscopy reveals the reaction mechanism;the Mg2Si microparticle reacts with O2 to form MgO and Si,while preventing SiO2 formation.Owing to the low oxygen content and microscale secondary structure,the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles(3,033 mAh/g vs.2,418 mAh/g,84.3%vs.73.1%).Synthesis is highly scalable,and a yield of 90.4%is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch.Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.展开更多
Nanoporous carbons（NPCs） derived from metal–organic frameworks（MOFs） are attracting increasing attention in many areas by virtue of their high specific surface area, large pore volume and unique porosity. The pre...Nanoporous carbons（NPCs） derived from metal–organic frameworks（MOFs） are attracting increasing attention in many areas by virtue of their high specific surface area, large pore volume and unique porosity. The present work reports the preparation of an NPC with high surface area（1731 m^2/g） and pore volume（1.68 cm^3/g） by direct carbonization of MOF-5. We examined the adsorption of three typical contaminants from aqueous solutions, i.e., sulfamethoxazole（SMX）,bisphenol A（BPA） and methyl orange（MO）, by using the as-prepared NPC. The results demonstrated that NPC could adsorb the contaminants effectively, with adsorption capacity（qm） of 625 mg/g（SMX）, 757 mg/g（BPA） and 872 mg/g（MO）, respectively. These values were approximately 1.0-3.2 times higher than those obtained for single-walled carbon nanotubes（SWCNTs） and commercial powder active carbon（PAC） under the same conditions. With its high surface area and unique meso/macropore structure, the enhanced adsorption of NPC most likely originates from the cooperative interaction of a pore-filling mechanism, electrostatic interaction,and hydrogen bonding. In particular, the p H value has a crucial impact on adsorption, suggesting the significant contribution of electrostatic interaction between NPC and the contaminants. This study provides a proof-of-concept demonstration of MOF-derived nanoporous carbons as effective adsorbents of contaminants for water treatment.展开更多
Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uni...Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uniform dispersion on the surface/inner channels of PCNO,as well as intimate contact with PCNO through hydrogen bonding,π-π,and chemical bonding interactions.In contrast with PCNO,the ox-GQDs/PCNO composite photocatalysts possessed improved light-harvesting ability,higher charge-transfer efficiency,enhanced photooxidation capacity,and increased amounts of reactive species due to the upconversion properties,strong electron capturing ability,and peroxidase-like activity of the ox-GQDs.Therefore,the visible-light photocatalytic degradation and disinfection performances of the ox-GQDs/PCNO composite were significantly enhanced.Remarkably,the composite with a 0.2 wt.% deposited amount of ox-GQDs(ox-GQDs-0.2%/PCNO)exhibited optimum amaranth photodegradation activity,with a corresponding rate about 3.1 times as high as that of PCNO.In addition,ox-GQDs-0.2%/PCNO could inactivate about 99.6%of Escherichia coli(E.coli)cells after 4 h of visible light irradiation,whereas only^31.9% of E.coli cells were killed by PCNO.Furthermore,h+,·O2-,and·OH were determined to be the reactive species generated in the photocatalytic process of the ox-GQDs/PCNO system;these species can thoroughly mineralize azo dyes and effectively inactivate pathogenic bacteria.展开更多
Fe3O4/CMK-3 was prepared by impregnation and used as a catalyst for the direct hydroxylation of benzene to phenol with hydro-gen peroxide. The iron species in the prepared catalyst was Fe3O4 because of the partial red...Fe3O4/CMK-3 was prepared by impregnation and used as a catalyst for the direct hydroxylation of benzene to phenol with hydro-gen peroxide. The iron species in the prepared catalyst was Fe3O4 because of the partial reduction of iron(III) to iron(II) on the surface of CMK-3. The high catalytic activity of the catalyst arises from the formation of Fe3O4 on the surface of CMK-3 and the high selectivity for phenol is attributed to the consumption of excess hydroxyl radicals by CMK-3. The effect of temperature,reaction time,volume of H2O2,and amount of catalyst on the catalytic performance of the prepared catalyst were investigated. Under optimized conditions,the catalyst showed excellent catalytic performance for the hydroxylation of benzene to phenol and 18% benzene conversion was achieved with 92% selectivity for phenol and with a TOF value of 8.7 h-1. The stability of catalyst was investigated by determining its activity after the fourth run and it was found to have decreased to 80% of the fresh catalyst's activity.展开更多
High entropy alloys(HEAs)containing five or more equimolar components have shown promising catalytic performance due to their unique chemical and mechanical properties.However,it is still challenging to prepare scalab...High entropy alloys(HEAs)containing five or more equimolar components have shown promising catalytic performance due to their unique chemical and mechanical properties.However,it is still challenging to prepare scalable and efficient nanoporous HEAs as catalysts.Here,we present a facile strategy to synthesize largescale nanoporous HEAs particles by combing vacuum induction melting,gas atomization,and acidic etching procedure.The application of HEAs to energy conversion is evaluated with electrocatalytic oxygen evolution reaction(OER)on AlCrCuFeNi HEAs.The HEAs exhibit a low OER overpotential of 270 mV to achieve a current density of 10 mA·cm^(-2),a small Tafel slope of 77.5 mV·dec^(-1),and long-term stability for over 35 h in 1 mol·L^(-1) KOH,which is comparable to the state-of-the-art OER electrocatalyst RuO2.The findings in this paper not only provide an industrial approach to produce nanoporous HEAs powder but also inspire the applications of HEAs as catalysts.展开更多
A simple and rapid approach for the electrochemical synthesis of Ag nanoparticles-coated gold nanoporous film (AgGNF) on a gold substrate was reported. The solid gold electrode (SGE) was directly anodized under a high...A simple and rapid approach for the electrochemical synthesis of Ag nanoparticles-coated gold nanoporous film (AgGNF) on a gold substrate was reported. The solid gold electrode (SGE) was directly anodized under a high potential of 5 V, and then reduced to obtain gold nanoporous film (AuNF) by freshly prepared ascorbic acid. The Ag nanoparticles (AgNPs) were grown on the AuNF electrode by potential-step electrodeposition. The resulting AgGNF composites electrodes were characterized by scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy and cyclic voltammetry (CV). As-prepared AgGNF electrode was used as a kind of superior sensor for Cr(VI) detection, which exhibited better electrocatalytic behavior than those of AuNF and SGE under identical conditions. Such a designed AgGNF nanocomposites electrode showed outstanding sensitivity (about 0.15 nA/ppb) and favorable reproducibility for Cr(VI) detection. The dependence of reduction current on Cr(VI) concentration is linear from 2 to 370 ppb with a low detection limit of 0.65 ppb. Interferences from other heavy metals ions (Cr3+, Cu2+, Pb2+, As3+ and Hg2+) associated with Cr(VI) analysis could be effectively diminished. The present method proves to be rapid, reliable, sensitive and low-cost.展开更多
基金the National Natural Science Foundation of China(No.20976197) for its financial support of this project
文摘With high surface area,open porosity and high efficiency,a catalyst was prepared and firstly employed in electrocatalytic reduction of CO2 and electrosynthesis of dimethyl carbonate（DMC）.The electrochemical property for electrocatalytic reduction of CO2 in ionic liquid was studied by cyclic voltammogram（CV）.The effects of various reaction variables like temperature,working potential and cathode materials on the electrocatalytic performance were also investigated.80%yield of DMC was obtained under the optimal reaction conditions.
基金This work was supported by Samsung SDI.Part of this work was performed at the Stanford Nano Shared Facilities(SNSF)Stanford Nanofabrication Facility(SNF).
文摘Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synthesis and low yield of nanoporous silicon limit its practical application.Here,we develop a scalable,low-cost top-down process of controlled oxidation of Mg2Si in the air,followed by HCl removal of MgO to generate nanoporous silicon without the use of HF.By controlling the synthesis conditions,the oxygen content,grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints.In situ environmental transmission electron microscopy reveals the reaction mechanism;the Mg2Si microparticle reacts with O2 to form MgO and Si,while preventing SiO2 formation.Owing to the low oxygen content and microscale secondary structure,the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles(3,033 mAh/g vs.2,418 mAh/g,84.3%vs.73.1%).Synthesis is highly scalable,and a yield of 90.4%is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch.Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.
基金supported by the National Natural Science Foundation of China (Nos. 21437001 and 21407019)Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (No. QA201617)
文摘Nanoporous carbons（NPCs） derived from metal–organic frameworks（MOFs） are attracting increasing attention in many areas by virtue of their high specific surface area, large pore volume and unique porosity. The present work reports the preparation of an NPC with high surface area（1731 m^2/g） and pore volume（1.68 cm^3/g） by direct carbonization of MOF-5. We examined the adsorption of three typical contaminants from aqueous solutions, i.e., sulfamethoxazole（SMX）,bisphenol A（BPA） and methyl orange（MO）, by using the as-prepared NPC. The results demonstrated that NPC could adsorb the contaminants effectively, with adsorption capacity（qm） of 625 mg/g（SMX）, 757 mg/g（BPA） and 872 mg/g（MO）, respectively. These values were approximately 1.0-3.2 times higher than those obtained for single-walled carbon nanotubes（SWCNTs） and commercial powder active carbon（PAC） under the same conditions. With its high surface area and unique meso/macropore structure, the enhanced adsorption of NPC most likely originates from the cooperative interaction of a pore-filling mechanism, electrostatic interaction,and hydrogen bonding. In particular, the p H value has a crucial impact on adsorption, suggesting the significant contribution of electrostatic interaction between NPC and the contaminants. This study provides a proof-of-concept demonstration of MOF-derived nanoporous carbons as effective adsorbents of contaminants for water treatment.
基金supported by the National Natural Science Foundation of China(21707052)Jiangsu Agriculture Science and Technology Innovation Fund(CX(18)2025)+1 种基金Fundamental Research Funds for the Central Universities(JUSRP11905 and JUSRP51714B)Key Research and Development Program of Jiangsu Province(BE2017623)~~
文摘Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uniform dispersion on the surface/inner channels of PCNO,as well as intimate contact with PCNO through hydrogen bonding,π-π,and chemical bonding interactions.In contrast with PCNO,the ox-GQDs/PCNO composite photocatalysts possessed improved light-harvesting ability,higher charge-transfer efficiency,enhanced photooxidation capacity,and increased amounts of reactive species due to the upconversion properties,strong electron capturing ability,and peroxidase-like activity of the ox-GQDs.Therefore,the visible-light photocatalytic degradation and disinfection performances of the ox-GQDs/PCNO composite were significantly enhanced.Remarkably,the composite with a 0.2 wt.% deposited amount of ox-GQDs(ox-GQDs-0.2%/PCNO)exhibited optimum amaranth photodegradation activity,with a corresponding rate about 3.1 times as high as that of PCNO.In addition,ox-GQDs-0.2%/PCNO could inactivate about 99.6%of Escherichia coli(E.coli)cells after 4 h of visible light irradiation,whereas only^31.9% of E.coli cells were killed by PCNO.Furthermore,h+,·O2-,and·OH were determined to be the reactive species generated in the photocatalytic process of the ox-GQDs/PCNO system;these species can thoroughly mineralize azo dyes and effectively inactivate pathogenic bacteria.
文摘Fe3O4/CMK-3 was prepared by impregnation and used as a catalyst for the direct hydroxylation of benzene to phenol with hydro-gen peroxide. The iron species in the prepared catalyst was Fe3O4 because of the partial reduction of iron(III) to iron(II) on the surface of CMK-3. The high catalytic activity of the catalyst arises from the formation of Fe3O4 on the surface of CMK-3 and the high selectivity for phenol is attributed to the consumption of excess hydroxyl radicals by CMK-3. The effect of temperature,reaction time,volume of H2O2,and amount of catalyst on the catalytic performance of the prepared catalyst were investigated. Under optimized conditions,the catalyst showed excellent catalytic performance for the hydroxylation of benzene to phenol and 18% benzene conversion was achieved with 92% selectivity for phenol and with a TOF value of 8.7 h-1. The stability of catalyst was investigated by determining its activity after the fourth run and it was found to have decreased to 80% of the fresh catalyst's activity.
基金This study was financially supported by the National Natural Science Foundation of China(No.51771132).
文摘High entropy alloys(HEAs)containing five or more equimolar components have shown promising catalytic performance due to their unique chemical and mechanical properties.However,it is still challenging to prepare scalable and efficient nanoporous HEAs as catalysts.Here,we present a facile strategy to synthesize largescale nanoporous HEAs particles by combing vacuum induction melting,gas atomization,and acidic etching procedure.The application of HEAs to energy conversion is evaluated with electrocatalytic oxygen evolution reaction(OER)on AlCrCuFeNi HEAs.The HEAs exhibit a low OER overpotential of 270 mV to achieve a current density of 10 mA·cm^(-2),a small Tafel slope of 77.5 mV·dec^(-1),and long-term stability for over 35 h in 1 mol·L^(-1) KOH,which is comparable to the state-of-the-art OER electrocatalyst RuO2.The findings in this paper not only provide an industrial approach to produce nanoporous HEAs powder but also inspire the applications of HEAs as catalysts.
基金supported by the National Natural Science Foundation of China (21005014)the Foundation of Donghua University (113-10-0044029)
文摘A simple and rapid approach for the electrochemical synthesis of Ag nanoparticles-coated gold nanoporous film (AgGNF) on a gold substrate was reported. The solid gold electrode (SGE) was directly anodized under a high potential of 5 V, and then reduced to obtain gold nanoporous film (AuNF) by freshly prepared ascorbic acid. The Ag nanoparticles (AgNPs) were grown on the AuNF electrode by potential-step electrodeposition. The resulting AgGNF composites electrodes were characterized by scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy and cyclic voltammetry (CV). As-prepared AgGNF electrode was used as a kind of superior sensor for Cr(VI) detection, which exhibited better electrocatalytic behavior than those of AuNF and SGE under identical conditions. Such a designed AgGNF nanocomposites electrode showed outstanding sensitivity (about 0.15 nA/ppb) and favorable reproducibility for Cr(VI) detection. The dependence of reduction current on Cr(VI) concentration is linear from 2 to 370 ppb with a low detection limit of 0.65 ppb. Interferences from other heavy metals ions (Cr3+, Cu2+, Pb2+, As3+ and Hg2+) associated with Cr(VI) analysis could be effectively diminished. The present method proves to be rapid, reliable, sensitive and low-cost.
