Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applicat...Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.展开更多
Reduced graphene oxide(rGO)aerogels are emerging as very attractive scaffolds for high-performance electromagnetic wave absorption materials(EWAMs)due to their intrinsic conductive networks and intricate interior micr...Reduced graphene oxide(rGO)aerogels are emerging as very attractive scaffolds for high-performance electromagnetic wave absorption materials(EWAMs)due to their intrinsic conductive networks and intricate interior microstructure,as well as good compatibility with other electromagnetic(EM)components.Herein,we realized the decoration of rGO aerogel with Mo_(2)C nanoparticles by sequential hydrothermal assembly,freeze-drying,and high-temperature pyrolysis.Results show that Mo_(2)C nanoparticle loading can be easily controlled by the ammonium molybdate to glucose molar ratio.The hydrophobicity and thermal insulation of the rGO aerogel are effectively improved upon the introduction of Mo_(2)C nanoparticles,and more importantly,these nanoparticles regulate the EM properties of the rGO aerogel to a large extent.Although more Mo_(2)C nanoparticles may decrease the overall attenuation ability of the rGO aerogel,they bring much better impedance matching.At a molar ratio of 1:1,a desirable balance between attenuation ability and impedance matching is observed.In this context,the Mo_(2)C/r GO aerogel displays strong reflection loss and broad response bandwidth,even with a small applied thickness(1.7 mm)and low filler loading(9.0wt%).The positive effects of Mo_(2)C nanoparticles on multifunctional properties may render Mo_(2)C/r GO aerogels promising candidates for high-performance EWAMs under harsh conditions.展开更多
Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter...Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ppm.Here,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of SS1.To regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)so-lution.The eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs biosynthesis.Our work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.展开更多
Developing high-performance nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR) is crucial for a variety of renewable energy conversion and storage systems. Toward that end, rational catalyst ...Developing high-performance nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR) is crucial for a variety of renewable energy conversion and storage systems. Toward that end, rational catalyst design principles that lead to highly active catalytic centers and enhanced active site accessibility are undoubtedly of paramount importance. Here, we used Prussian blue nano- particles to anchor Fe/Fe3C species to nitrogen-doped reduced graphene oxide aerogels as ORR catalysts. The strong interaction between nanosized Fe3C and the graphitic carbon shell led to synergistic effects in the ORR, and the protection of the carbon shell guaranteed stability of the catalyst. As a result, the aerogel electrocatalyst displayed outstanding activity in the ORR on par with the state-of-the-art Pt/C catalyst at the same mass loading in alkaline media, good performance in acidic media, and excellent stability and crossover tolerance that rivaled that of the best nonprecious-metal ORR electrocatalysts reported to date.展开更多
Thiamine derivatives that are cheap, readily available, non-toxic and green are used as heterogeneous catalyst for the generation of cyclic carbonates through cycloaddition of CO_2 to epoxides without the need of co-c...Thiamine derivatives that are cheap, readily available, non-toxic and green are used as heterogeneous catalyst for the generation of cyclic carbonates through cycloaddition of CO_2 to epoxides without the need of co-catalyst and solvent. The interaction between thiamine hydrochloride(VB_1-Cl) and substrates(CO_2 and propylene oxide) was proven by ultraviolet-visible spectroscopy and ~1H nuclear magnetic resonance analysis, and it is deduced that the synergistic action among multi-functional groups(hydroxyl, halide anion and amine) is a favorable factor for cycloaddition reaction. A series of VB_1/GO aerogels were facilely prepared through the addition of aqueous VB_1 derivatives to a suspension of GO in ethanol at room temperature. It was found that the aerogel generated through the interaction of VB_1-Cl with GO shows catalytic activity and stability higher than those of VB_1-Cl. It is because the electrostatic interaction between GO and VB_1-Cl enhances the nucleophilicity and leaving ability of anion. The effects of reaction temperature, catalyst loading, CO_2 pressure and reaction time on CO_2 cycloaddition to propylene oxide were thoroughly studied.展开更多
Organic–inorganic hybrid perovskites are quite promising candidates in the field of electromagnetic wave (EMW) absorption due to their unique physicochemical properties. However, it is still a considerable challenge ...Organic–inorganic hybrid perovskites are quite promising candidates in the field of electromagnetic wave (EMW) absorption due to their unique physicochemical properties. However, it is still a considerable challenge to satisfy the light weight, broad bandwidth, and strong absorption properties simultaneously. Herein, the solution of methylammonium lead iodide (MAPbI3) perovskites was infiltrated into the pores of reduced graphene oxide (rGO) aerogels. After drying, a series of MAPbI3/rGO composite aerogel (MGA) materials were synthesized by anchoring the MAPbI3 perovskite nanoparticles to rGO sheets with the assistance of rGO templates. Through the adjustment of component ratios, excellent EMW absorption properties are obtained with the synergistic effects of polarization loss, conduction loss, and multiple reflection and scattering of MAPbI3 and rGO. The porous structure of the aerogel and the suitable group distribution ratio allowed the MGA-4 samples to obtain excellent impedance matching and ultra-low density of ∼ 7.69 mg·cm−3. At a low filling ratio of 15 wt.%, the MGA-4 sample simultaneously achieves highly efficient and broadband EMW absorption performance at a thin thickness. The MGA-4 sample obtained a minimum reflection loss value of −64.35 dB and the effective absorption bandwidth (EAB) value of 5.4 GHz at a thickness of 2.08 mm and a maximum EAB (EABmax) value of 6.2 GHz under 2.22 mm. The MGA-5 sample obtained a maximum EAB value of 6.4 GHz with the thinckness of 2.16 mm. Furthermore, the simulation results of the radar cross-section (RCS) verified the component-optimized composites are capable of achieving excellent EMW attenuation. This paper provides a new approach and valuable reference for the development of hybrid perovskite-based microwave absorption materials with lightweight, ultra-broadband, and strong absorption properties.展开更多
Porous carbon aerogel material has gained an increasing attraction for developing supercapacitor electrodes due to its cost-effective synthesis process and relatively high electrochemical performance.However,the envir...Porous carbon aerogel material has gained an increasing attraction for developing supercapacitor electrodes due to its cost-effective synthesis process and relatively high electrochemical performance.However,the environmental performances of supercapacitor electrodes produced from different carbon aerogel materials are never comparatively studied,hindering our knowledge of supercapacitor electrode production in a sustainable pattern.In this study,nitrogen-doped biochar aerogel-based electrode(BA-electrode)produced from Entermorpha prolifera was simulated to investigate the environmental performance by using life cycle assessment method.For comparison,the assessment of graphene oxide aerogel-based electrode(GOA-electrode)was also carried out.It can be observed that the life cycle global warming potential for the BA-electrode was lower than that of GOA-electrode with a reduction of 53.1‒68.1%.In comparison with GOA-electrode,the BA-electrodes endowed smaller impacts on environment in majority of impact categories.Moreover,in comparison with GOA-electrode,the environmental damages of BA-electrode were greatly decreased by 35.8‒56.4%(human health),44.9‒62.6%(ecosystems),and 87.0‒91.2%(resources),respectively.The production stages of GOA and graphene oxide and stages of nitrogen-doped biochar aerogel production and Entermorpha prolifera drying were identified as the hotspots of environmental impact/dam-age for the GOA-electrode and BA-electrode,respectively.Overall,this finding highlights the efficient utilization of algae feedstock to construct a green and sustainable technical route of supercapacitor electrode production.展开更多
基金supported by the National Natural Science Foundation of China (U1232119, 21403172)the Sichuan Youth Science and Technology Foundation (2013JQ0034, 2014JQ0017)the Innovative Research Team of Sichuan Province (2016TD0011)~~
文摘Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.
基金supported by the China Postdoctoral Science Foundation(No.2021MD703944)the Fund of Science and Technology on Near-Surface Detection Laboratory(No.6142414211808)+1 种基金the Director Fund of State Key Laboratory of Pulsed Power Laser Technology(No.SKL2021ZR06)the National Natural Science Foundation of China(No.21776053)。
文摘Reduced graphene oxide(rGO)aerogels are emerging as very attractive scaffolds for high-performance electromagnetic wave absorption materials(EWAMs)due to their intrinsic conductive networks and intricate interior microstructure,as well as good compatibility with other electromagnetic(EM)components.Herein,we realized the decoration of rGO aerogel with Mo_(2)C nanoparticles by sequential hydrothermal assembly,freeze-drying,and high-temperature pyrolysis.Results show that Mo_(2)C nanoparticle loading can be easily controlled by the ammonium molybdate to glucose molar ratio.The hydrophobicity and thermal insulation of the rGO aerogel are effectively improved upon the introduction of Mo_(2)C nanoparticles,and more importantly,these nanoparticles regulate the EM properties of the rGO aerogel to a large extent.Although more Mo_(2)C nanoparticles may decrease the overall attenuation ability of the rGO aerogel,they bring much better impedance matching.At a molar ratio of 1:1,a desirable balance between attenuation ability and impedance matching is observed.In this context,the Mo_(2)C/r GO aerogel displays strong reflection loss and broad response bandwidth,even with a small applied thickness(1.7 mm)and low filler loading(9.0wt%).The positive effects of Mo_(2)C nanoparticles on multifunctional properties may render Mo_(2)C/r GO aerogels promising candidates for high-performance EWAMs under harsh conditions.
基金supported by the National Key Research and Development Program of China(No.2018YFA0901300)the Na-tional Natural Science Foundation of China(Nos.NSFC 32071411,NSFC 32001034,and NSFC 31701569)+1 种基金the Young Science and Tech-nology Talents Growth Project of Education Department of Guizhou Province(No.KY[2018]445)Key Laboratory of Wuliangye-flavor Liquor Solid-state Fermentation,China National Light Indus-try(No.2021JJ013).
文摘Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ppm.Here,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of SS1.To regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)so-lution.The eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs biosynthesis.Our work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.
文摘Developing high-performance nonprecious-metal electrocatalysts for the oxygen reduction reaction (ORR) is crucial for a variety of renewable energy conversion and storage systems. Toward that end, rational catalyst design principles that lead to highly active catalytic centers and enhanced active site accessibility are undoubtedly of paramount importance. Here, we used Prussian blue nano- particles to anchor Fe/Fe3C species to nitrogen-doped reduced graphene oxide aerogels as ORR catalysts. The strong interaction between nanosized Fe3C and the graphitic carbon shell led to synergistic effects in the ORR, and the protection of the carbon shell guaranteed stability of the catalyst. As a result, the aerogel electrocatalyst displayed outstanding activity in the ORR on par with the state-of-the-art Pt/C catalyst at the same mass loading in alkaline media, good performance in acidic media, and excellent stability and crossover tolerance that rivaled that of the best nonprecious-metal ORR electrocatalysts reported to date.
文摘Thiamine derivatives that are cheap, readily available, non-toxic and green are used as heterogeneous catalyst for the generation of cyclic carbonates through cycloaddition of CO_2 to epoxides without the need of co-catalyst and solvent. The interaction between thiamine hydrochloride(VB_1-Cl) and substrates(CO_2 and propylene oxide) was proven by ultraviolet-visible spectroscopy and ~1H nuclear magnetic resonance analysis, and it is deduced that the synergistic action among multi-functional groups(hydroxyl, halide anion and amine) is a favorable factor for cycloaddition reaction. A series of VB_1/GO aerogels were facilely prepared through the addition of aqueous VB_1 derivatives to a suspension of GO in ethanol at room temperature. It was found that the aerogel generated through the interaction of VB_1-Cl with GO shows catalytic activity and stability higher than those of VB_1-Cl. It is because the electrostatic interaction between GO and VB_1-Cl enhances the nucleophilicity and leaving ability of anion. The effects of reaction temperature, catalyst loading, CO_2 pressure and reaction time on CO_2 cycloaddition to propylene oxide were thoroughly studied.
基金financial support from the National Natural Science Foundation of China(No.52103223)the Natural Science Basic Research Program of Shaanxi(No.2023-JC-YB-413)+2 种基金the Natural Science Foundation of Heilongjiang Province of China(No.YQ2023E027)the Key Laboratory of Functional Molecular Solids,Ministry of Education(No.FMS20230010)the Fundamental Research Funds for the Central Universities(Nos.3072024GH2605,3072024XX2613,and 3072024XX2616).
文摘Organic–inorganic hybrid perovskites are quite promising candidates in the field of electromagnetic wave (EMW) absorption due to their unique physicochemical properties. However, it is still a considerable challenge to satisfy the light weight, broad bandwidth, and strong absorption properties simultaneously. Herein, the solution of methylammonium lead iodide (MAPbI3) perovskites was infiltrated into the pores of reduced graphene oxide (rGO) aerogels. After drying, a series of MAPbI3/rGO composite aerogel (MGA) materials were synthesized by anchoring the MAPbI3 perovskite nanoparticles to rGO sheets with the assistance of rGO templates. Through the adjustment of component ratios, excellent EMW absorption properties are obtained with the synergistic effects of polarization loss, conduction loss, and multiple reflection and scattering of MAPbI3 and rGO. The porous structure of the aerogel and the suitable group distribution ratio allowed the MGA-4 samples to obtain excellent impedance matching and ultra-low density of ∼ 7.69 mg·cm−3. At a low filling ratio of 15 wt.%, the MGA-4 sample simultaneously achieves highly efficient and broadband EMW absorption performance at a thin thickness. The MGA-4 sample obtained a minimum reflection loss value of −64.35 dB and the effective absorption bandwidth (EAB) value of 5.4 GHz at a thickness of 2.08 mm and a maximum EAB (EABmax) value of 6.2 GHz under 2.22 mm. The MGA-5 sample obtained a maximum EAB value of 6.4 GHz with the thinckness of 2.16 mm. Furthermore, the simulation results of the radar cross-section (RCS) verified the component-optimized composites are capable of achieving excellent EMW attenuation. This paper provides a new approach and valuable reference for the development of hybrid perovskite-based microwave absorption materials with lightweight, ultra-broadband, and strong absorption properties.
基金the National Natural Science Foundation of China(51808303,51672143,21976185 and 21501105)Science and Technology Support Plan for Youth Innovation of Colleges in Shandong Province(DC2000000961)Taishan Scholar Program,Outstanding Youth of Natural Science in Shandong Province(JQ201713).
文摘Porous carbon aerogel material has gained an increasing attraction for developing supercapacitor electrodes due to its cost-effective synthesis process and relatively high electrochemical performance.However,the environmental performances of supercapacitor electrodes produced from different carbon aerogel materials are never comparatively studied,hindering our knowledge of supercapacitor electrode production in a sustainable pattern.In this study,nitrogen-doped biochar aerogel-based electrode(BA-electrode)produced from Entermorpha prolifera was simulated to investigate the environmental performance by using life cycle assessment method.For comparison,the assessment of graphene oxide aerogel-based electrode(GOA-electrode)was also carried out.It can be observed that the life cycle global warming potential for the BA-electrode was lower than that of GOA-electrode with a reduction of 53.1‒68.1%.In comparison with GOA-electrode,the BA-electrodes endowed smaller impacts on environment in majority of impact categories.Moreover,in comparison with GOA-electrode,the environmental damages of BA-electrode were greatly decreased by 35.8‒56.4%(human health),44.9‒62.6%(ecosystems),and 87.0‒91.2%(resources),respectively.The production stages of GOA and graphene oxide and stages of nitrogen-doped biochar aerogel production and Entermorpha prolifera drying were identified as the hotspots of environmental impact/dam-age for the GOA-electrode and BA-electrode,respectively.Overall,this finding highlights the efficient utilization of algae feedstock to construct a green and sustainable technical route of supercapacitor electrode production.