A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of c...A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.展开更多
The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple ...The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.展开更多
To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through...To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through a combination of hydrothermal processes and sulfidation treatment.The unique bowlshaped FeCoS_(4)/S-HC composites exhibit excellent structural stability with a high specific surface area of 303.7 m^(2)·g^(-1) and a pore volume of 0.93 cm^(3)·g^(-1).When applied as anode material for lithium-ion batteries,the FeCoS_(4)@S-HC anode exhibits efficient lithium storage with high reversible specific capacity(970.2 mA·h·g^(-1) at 100 mA·g^(-1))and enhanced cycling stability(574 mA·h·g^(-1) at 0.2 A·g^(-1) after 350 cycles,a capacity retention of 84%).The excellent lithium storage is attributed to the fact that the bimetallic FeCoS_(4) nanoparticles with abundant active sites can accelerate the electrochemical reaction kinetics,and the bowl-shaped S-HC structure can provide a stable mechanical structure to suppress volume expansion.展开更多
In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morpholo...In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.展开更多
Rechargeable Li-S batteries(LSBs)are emerging as an important alternative to lithium-ion batteries(LIBs),owing to their high energy densities and low cost;yet sluggish redox kinetics of LiPSs results in inferior cycle...Rechargeable Li-S batteries(LSBs)are emerging as an important alternative to lithium-ion batteries(LIBs),owing to their high energy densities and low cost;yet sluggish redox kinetics of LiPSs results in inferior cycle life.Herein,we prepared multifunctional self-supporting hyphae carbon nanobelt(HCNB)as hosts by carbonization of hyphae balls of Rhizopus,which could increase the S loading of the cathode without sacrificing reaction kinetics.Trace platinum(Pt)nanoparticles were introduced into HCNBs(PtHCNBs)by ion-beam sputtering deposition.Based on the X-ray photoelectron spectroscopy analyses,the introduced trace Pt regulated the local electronic states of heteroatoms in HCNBs.Electrochemical kinetics investigation combined with operando Raman measurements revealed the accelerated reaction mechanics of sulfur species.Benefiting from the synergistic catalytic effect and the unique structures,the as-prepared PtHCNB/MWNCT/S cathodes delivered a stable capacity retention of 77%for 400 cycles at 0.5 C with a sulfur loading of 4.6 mg cm^(-2).More importantly,remarkable cycling performance was achieved with an high areal S loading of 7.6 mg cm^(-2).This finding offers a new strategy to prolong the cycle life of LSBs.展开更多
S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
Wind-induced sand erosion is a natural process, and can have several negative impacts on human health, environment, and economy. To mitigate the wind-induced sand erosion, an environmental friendly technique that help...Wind-induced sand erosion is a natural process, and can have several negative impacts on human health, environment, and economy. To mitigate the wind-induced sand erosion, an environmental friendly technique that helps to bind soil particles is desirable. The microbially induced calcium carbonate precipitation(MICP) treatment has lately become renowned and a viable alternative to enhance the binding of sand particles(especially against wind erosion). The efficiency of Sporosarcina pasteurii bacteria in inducing calcite formation can be influenced by various factors, including the type of growth media used for bacterial culture. Most of the studies have mainly validated the efficiency of S. pasteurii bacteria usually under single growth media for the MICP treatment. However, the efficiency of S. pasteurii under different growth media on calcite formation is rarely explored. The current study explores the effect of S.pasteurii bacteria on calcite formation under the presence of three different growth media, namely,molasses(MS), tryptic soy broth(TB), and nutrient broth(NB). The three growth media have been applied in the laboratory with and without bacterial solution(control samples). Altered cementation media concentrations(0.5 and 1.0 M) with different pore volumes(PVs), namely, 0.25, 0.50, and 1.00 PV were used in sand-filled tubes for 7 and 14 treatment cycles(1 cycle=24 h). The pH and EC were measured for 12-h period in every 2 h interval, to monitor values at the time of treatment at room temperature. The calcite precipitation was confirmed using SEM(scanning electron microscope), PXRD(powder X-ray diffraction), and calcimeter tests. It was observed that MS generates lower calcite precipitation as compared with NB and TB. However, MS has the advantage of being more economical and abundant(waste product from sugar mills and refineries) as compared with other growth media(NB and TB). It was observed that the minimum and the maximum calcite precipitation using MS is 5% and 12%, respectively.The findings using MS in the present study was compared with the literature and found that precipitation of calcite using MS is effective to stabilize soil against wind erosion.展开更多
Based on the measurements of petrological, petrophysical and elastic properties of the samples of different sedimentary facies in the fourth member of Sinian Dengying Formation (Deng 4 Member) in the Sichuan Basin, th...Based on the measurements of petrological, petrophysical and elastic properties of the samples of different sedimentary facies in the fourth member of Sinian Dengying Formation (Deng 4 Member) in the Sichuan Basin, the diagenetic processes of reservoirs of different sedimentary facies and their controls on the petrophysical properties were discussed. The results show that cracks and mineral composition jointly control the petrophysical properties, and both are significantly influenced by sedimentary environment and diagenesis. The microbial dolomite of mound-shoal facies mainly experienced multi-stage dolomitization, penecontemporaneous dissolution, tectonic rupture and hydrothermal/organic acid dissolution processes, giving rise to cracks and dissolved pores. The grannular dolomite of inter-mound-shoal bottomland or dolomitic lagoon facies mainly underwent mechanical compaction, burial dolomitization and tectonic-hydrothermal action, creating cracks and intercrystalline pores. The diagenesis related to crack development increases the pressure- and saturation-dependent effects of samples, leading to significant decrease in the compressional wave impedance and Poisson's ratio. Dolomitization changes the properties of mineral particles, resulting in a Poisson's ratio close to dolomite. The muddy, siliceous and calcareous sediments in the low-energy environment lead to the decrease of impedance and the differential change of Poisson's ratio (significantly increased or decreased). The samples with both cracks and dissolved pores show high P-wave velocity dispersion characteristics, and the P-wave velocity dispersion of samples with only fractures or pores is the lowest.展开更多
The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle p...Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle performance are still needed,aiming to the practical application.Herein,S/N/O tridoped carbon(SNOC)nanospheres are prepared by in-situ vulcanized polybenzoxazine.The S/N/O tridoped carbon matrix provides abundant active sites for potassium ion adsorption and effectively improves potassium storage capacity.Moreover,the SNOC nanospheres possess large carbon interlayer spacing and high specific surface area,which broaden the diffusion pathway of potassium ions and accelerate the electron transfer speed,resulting in excellent rate performance.As an anode for PIBs,SNOC shows attractive rate performance(438.5 mA h g^(-1) at 50 mA g^(-1) and 174.5 mA h g^(-1) at2000 mA g^(-1)),ultra-high reversible capacity(397.4 mA h g^(-1) at 100 mA g^(-1) after 700 cycles)and ultra-long cycling life(218.9 mA h g^(-1) at 2000 mA g^(-1) after 7300 cycles,123.1 mA h g^(-1) at3000 mA g^(-1) after 16500 cycles and full cell runs for 4000 cycles).Density functional theory calculation confirms that S/N/O tri-doping enhances the adsorption and diffusion of potassium ions,and in-situ Fourier-transform infrared explores explored the potassium storage mechanism of SNOC.展开更多
Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in seconda...Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.展开更多
How coral reefs with high productivity and biodiversity can flourish in oligotrophic tropical oceans has inspired substantial research on coral reef ecosystems.Increasing evidence shows that similar to water in an oas...How coral reefs with high productivity and biodiversity can flourish in oligotrophic tropical oceans has inspired substantial research on coral reef ecosystems.Increasing evidence shows that similar to water in an oasis in the desert,there are stable nutrient supplies to coral reefs in oligotrophic oceans.Here,with emphasis on the fluxes of organic matter,we summarize at the ecosystem level(1)the multiple input pathways of external nutrients,(2)the storage of nutrients in reef organisms,(3)the efficient retaining and recycling of dissolved and particulate organic matter within coral reef ecosystems,(4)the distinctly high phytoplankton productivity and biomass inside and near oceanic coral reefs,and(5)the export of reef-related organic carbon to adjacent open oceans.These properties enable coral reefs to function as ecological“pumps”for gathering nutrients across ecosystems and space,retaining and recycling nutrients within the ecosystem,supporting high phytoplankton productivity,and exporting organic carbon to adjacent open oceans.Particularly,the high phytoplankton productivity and biomass make waters around coral reefs potential hotspots of carbon export to ocean depths via the biological pump.We demonstrate that organic carbon influx is vital for coral reef ecosystems’carbon budget and carbon export.The concept of the coral reef ecological pump provides a framework to improve the understanding of the functioning of the coral reef ecosystem and its responses to disturbance.Prospects of the coral reef ecological pump in coral reef studies are discussed in changing oceans driven by human activities and global change in the Anthropocene.展开更多
Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodi...Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.展开更多
硬炭因资源丰富、结构稳定及安全性高等优势,已成为钠离子电池常用阳极材料。其中,煤基衍生硬炭受到了广泛的关注。本工作以长焰煤为碳源,硫脲为氮硫源,NaCl为模板,通过两步炭化工艺和杂原子掺杂相结合的方法合成了N和S共掺杂的煤基硬炭...硬炭因资源丰富、结构稳定及安全性高等优势,已成为钠离子电池常用阳极材料。其中,煤基衍生硬炭受到了广泛的关注。本工作以长焰煤为碳源,硫脲为氮硫源,NaCl为模板,通过两步炭化工艺和杂原子掺杂相结合的方法合成了N和S共掺杂的煤基硬炭(NSPC1200)。两步炭化过程在调节碳微晶结构和扩大层间距方面发挥了重要的作用。N和S的共掺杂调节了炭材料的电子结构,赋予其更多的活性位点;此外,引入NaCl作为模板有助于孔结构的构建,有利于电极和电解质之间的接触,从而实现Na+和电子的有效传输。在协同作用下,样品NSPC1200表现出优异的储钠能力,在20 mA g^(−1)电流密度下呈现314.2 mAh g^(−1)的可逆容量。即使在100 mA g^(−1)下循环200次,仍保持224.4 mAh g^(−1)的比容量。这项工作成功实现了策略性调整煤基炭材料微观结构的目标,最终获得了具有优异的电化学性能的硬炭阳极。展开更多
基金Supported by the Changcheng Scholars Program of Beijing(CIT&TCD 20150316)
文摘A series of Zn–Ca–Al oxides with different CaO and ZnO contents have been prepared and evaluated in the synthesis of propylene carbonate(PC) from 1,2-propylene glycol(PG) and urea in a batch reactor. The effect of catalyst composition, basicity and reaction process parameters such as temperature, catalyst dose, molar ratio of PG to urea, purge gas flow and reaction time has been studied to find suitable reaction conditions for the PC synthesis. The PC selectivity and yield under the desired conditions could reach 98.4% and 90.8%, respectively. The best performing catalyst also exhibited a good reusability without appreciable loss in the PC selectivity and yield after five consecutive reaction runs. In addition, a stepwise reaction pathway involving a 2-hydroxypropyl carbamate intermediate was proposed for the urea alcoholysis to PC in the presence of Zn–Ca–Al catalysts, according to the time dependences of reaction intermediates and products.
基金supported by the National Natural Science Foundation of China(52374301 and 22279030)the Fundamental Research Funds for the Central Universities(N2223037)+1 种基金Hebei Key Laboratory of Dielectric and Electrolyte Functional Material,Northeastern University at Qinhuangdao(HKDEFM2021201)the Performance subsidy fund for the Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(22567627H)。
文摘The interface mechanism between catalyst and carbon substrate has been the focus of research.In this paper,the FeCo alloy embedded N,S co-doped carbon substrate bifunctional catalyst(FeCo/S-NC)is obtained by a simple one-step pyrolysis strategy.The experimental results and density functional theory(DFT)calculation show that the formation of FeCo alloy is conducive to promoting electron transfer,and the introduction of S atom can enhance the interaction between FeCo alloy and carbon substrate,thus inhibiting the migration and agglomeration of particles on the surface of carbon material.The FeCo/SNC catalysts show outstanding performance for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).FeCo/S-NC shows a high half-wave potential(E_(1/2)=0.8823 V)for ORR and a low overpotential at 10 mA cm^(-2)(E_(j=10)=299 mV)for OER.In addition,compared with Pt/C+RuO_(2) assembled Zn-air battery(ZAB),the FeCo/S-NC assembled ZAB exhibits a larger power density(198.8 mW cm^(-2)),a higher specific capacity(786.1 mA h g_(zn)~(-1)),and ultra-stable cycle performance.These results confirm that the optimized composition and the interfacial interaction between catalyst and carbon substrate synergistically enhance the electrochemical performance.
基金financially supported by the National Natural Science Foundation of China(22379056,52102260)the Project funded by China Postdoctoral Science Foundation(2022M711545)the Carbon Peak and Carbon Neutrality Project(Breakthrough for Industry Prospect and Key Technologies)of Zhenjiang City(CG2023003)。
文摘To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through a combination of hydrothermal processes and sulfidation treatment.The unique bowlshaped FeCoS_(4)/S-HC composites exhibit excellent structural stability with a high specific surface area of 303.7 m^(2)·g^(-1) and a pore volume of 0.93 cm^(3)·g^(-1).When applied as anode material for lithium-ion batteries,the FeCoS_(4)@S-HC anode exhibits efficient lithium storage with high reversible specific capacity(970.2 mA·h·g^(-1) at 100 mA·g^(-1))and enhanced cycling stability(574 mA·h·g^(-1) at 0.2 A·g^(-1) after 350 cycles,a capacity retention of 84%).The excellent lithium storage is attributed to the fact that the bimetallic FeCoS_(4) nanoparticles with abundant active sites can accelerate the electrochemical reaction kinetics,and the bowl-shaped S-HC structure can provide a stable mechanical structure to suppress volume expansion.
文摘In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.
基金partially supported by grants from the National Natural Science Foundation of China(52072099)Team program of the Natural Science Foundation of Heilongjiang Province,China(No.TD2021E005)
文摘Rechargeable Li-S batteries(LSBs)are emerging as an important alternative to lithium-ion batteries(LIBs),owing to their high energy densities and low cost;yet sluggish redox kinetics of LiPSs results in inferior cycle life.Herein,we prepared multifunctional self-supporting hyphae carbon nanobelt(HCNB)as hosts by carbonization of hyphae balls of Rhizopus,which could increase the S loading of the cathode without sacrificing reaction kinetics.Trace platinum(Pt)nanoparticles were introduced into HCNBs(PtHCNBs)by ion-beam sputtering deposition.Based on the X-ray photoelectron spectroscopy analyses,the introduced trace Pt regulated the local electronic states of heteroatoms in HCNBs.Electrochemical kinetics investigation combined with operando Raman measurements revealed the accelerated reaction mechanics of sulfur species.Benefiting from the synergistic catalytic effect and the unique structures,the as-prepared PtHCNB/MWNCT/S cathodes delivered a stable capacity retention of 77%for 400 cycles at 0.5 C with a sulfur loading of 4.6 mg cm^(-2).More importantly,remarkable cycling performance was achieved with an high areal S loading of 7.6 mg cm^(-2).This finding offers a new strategy to prolong the cycle life of LSBs.
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金the Prestige Institute of Engineering, Management, and Research (PIEMR), Indore, India, for their support during the research work。
文摘Wind-induced sand erosion is a natural process, and can have several negative impacts on human health, environment, and economy. To mitigate the wind-induced sand erosion, an environmental friendly technique that helps to bind soil particles is desirable. The microbially induced calcium carbonate precipitation(MICP) treatment has lately become renowned and a viable alternative to enhance the binding of sand particles(especially against wind erosion). The efficiency of Sporosarcina pasteurii bacteria in inducing calcite formation can be influenced by various factors, including the type of growth media used for bacterial culture. Most of the studies have mainly validated the efficiency of S. pasteurii bacteria usually under single growth media for the MICP treatment. However, the efficiency of S. pasteurii under different growth media on calcite formation is rarely explored. The current study explores the effect of S.pasteurii bacteria on calcite formation under the presence of three different growth media, namely,molasses(MS), tryptic soy broth(TB), and nutrient broth(NB). The three growth media have been applied in the laboratory with and without bacterial solution(control samples). Altered cementation media concentrations(0.5 and 1.0 M) with different pore volumes(PVs), namely, 0.25, 0.50, and 1.00 PV were used in sand-filled tubes for 7 and 14 treatment cycles(1 cycle=24 h). The pH and EC were measured for 12-h period in every 2 h interval, to monitor values at the time of treatment at room temperature. The calcite precipitation was confirmed using SEM(scanning electron microscope), PXRD(powder X-ray diffraction), and calcimeter tests. It was observed that MS generates lower calcite precipitation as compared with NB and TB. However, MS has the advantage of being more economical and abundant(waste product from sugar mills and refineries) as compared with other growth media(NB and TB). It was observed that the minimum and the maximum calcite precipitation using MS is 5% and 12%, respectively.The findings using MS in the present study was compared with the literature and found that precipitation of calcite using MS is effective to stabilize soil against wind erosion.
基金Supported by the National Natural Science Foundation of China(41774136)。
文摘Based on the measurements of petrological, petrophysical and elastic properties of the samples of different sedimentary facies in the fourth member of Sinian Dengying Formation (Deng 4 Member) in the Sichuan Basin, the diagenetic processes of reservoirs of different sedimentary facies and their controls on the petrophysical properties were discussed. The results show that cracks and mineral composition jointly control the petrophysical properties, and both are significantly influenced by sedimentary environment and diagenesis. The microbial dolomite of mound-shoal facies mainly experienced multi-stage dolomitization, penecontemporaneous dissolution, tectonic rupture and hydrothermal/organic acid dissolution processes, giving rise to cracks and dissolved pores. The grannular dolomite of inter-mound-shoal bottomland or dolomitic lagoon facies mainly underwent mechanical compaction, burial dolomitization and tectonic-hydrothermal action, creating cracks and intercrystalline pores. The diagenesis related to crack development increases the pressure- and saturation-dependent effects of samples, leading to significant decrease in the compressional wave impedance and Poisson's ratio. Dolomitization changes the properties of mineral particles, resulting in a Poisson's ratio close to dolomite. The muddy, siliceous and calcareous sediments in the low-energy environment lead to the decrease of impedance and the differential change of Poisson's ratio (significantly increased or decreased). The samples with both cracks and dissolved pores show high P-wave velocity dispersion characteristics, and the P-wave velocity dispersion of samples with only fractures or pores is the lowest.
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金financially supported by the National Natural Science Foundation of China(21975069 and 21872045)the Key Project of Research and Development Plan of Hunan Province(2019SK2071)+1 种基金the Natural Science Foundation of Hunan Province,China(2020JJ4169)the State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Development and Reform Commission of Hunan Province。
文摘Carbonaceous materials are considered as ideal anode for potassium ion batteries(PIBs)due to their abundant resources and stable physical and chemical properties.However,improvements of reversible capacity and cycle performance are still needed,aiming to the practical application.Herein,S/N/O tridoped carbon(SNOC)nanospheres are prepared by in-situ vulcanized polybenzoxazine.The S/N/O tridoped carbon matrix provides abundant active sites for potassium ion adsorption and effectively improves potassium storage capacity.Moreover,the SNOC nanospheres possess large carbon interlayer spacing and high specific surface area,which broaden the diffusion pathway of potassium ions and accelerate the electron transfer speed,resulting in excellent rate performance.As an anode for PIBs,SNOC shows attractive rate performance(438.5 mA h g^(-1) at 50 mA g^(-1) and 174.5 mA h g^(-1) at2000 mA g^(-1)),ultra-high reversible capacity(397.4 mA h g^(-1) at 100 mA g^(-1) after 700 cycles)and ultra-long cycling life(218.9 mA h g^(-1) at 2000 mA g^(-1) after 7300 cycles,123.1 mA h g^(-1) at3000 mA g^(-1) after 16500 cycles and full cell runs for 4000 cycles).Density functional theory calculation confirms that S/N/O tri-doping enhances the adsorption and diffusion of potassium ions,and in-situ Fourier-transform infrared explores explored the potassium storage mechanism of SNOC.
基金financially supported by the Shenzhen Science and Technology Program(JCYJ20220530141012028),ChinaThe National Natural Science Foundation of China(22005178),China+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01),ChianThe fellowship of China Postdoctoral Science Foundation(2022M722333),Chianthe Jiangsu Funding Program for Excellent Postdoctoral Talent,Chian。
文摘Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.
基金The Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou) under contract No.GML2019ZD0405the National Natural Science Foundation of China under contract Nos41506150 and 41130855+3 种基金the Guangdong Basic and Applied Basic Research Foundation under contract No.2019A1515011645the National Science and Technology Basic Work Program of the Ministry of Science and Technology of China under contract No.2015FY110600the Science and Technology Planning Project of Guangdong Province,China under contract No.2020B1212060058the Development Fund of South China Sea Institute of Oceanology of the Chinese Academy of Sciences under contract No.SCSIO202204。
文摘How coral reefs with high productivity and biodiversity can flourish in oligotrophic tropical oceans has inspired substantial research on coral reef ecosystems.Increasing evidence shows that similar to water in an oasis in the desert,there are stable nutrient supplies to coral reefs in oligotrophic oceans.Here,with emphasis on the fluxes of organic matter,we summarize at the ecosystem level(1)the multiple input pathways of external nutrients,(2)the storage of nutrients in reef organisms,(3)the efficient retaining and recycling of dissolved and particulate organic matter within coral reef ecosystems,(4)the distinctly high phytoplankton productivity and biomass inside and near oceanic coral reefs,and(5)the export of reef-related organic carbon to adjacent open oceans.These properties enable coral reefs to function as ecological“pumps”for gathering nutrients across ecosystems and space,retaining and recycling nutrients within the ecosystem,supporting high phytoplankton productivity,and exporting organic carbon to adjacent open oceans.Particularly,the high phytoplankton productivity and biomass make waters around coral reefs potential hotspots of carbon export to ocean depths via the biological pump.We demonstrate that organic carbon influx is vital for coral reef ecosystems’carbon budget and carbon export.The concept of the coral reef ecological pump provides a framework to improve the understanding of the functioning of the coral reef ecosystem and its responses to disturbance.Prospects of the coral reef ecological pump in coral reef studies are discussed in changing oceans driven by human activities and global change in the Anthropocene.
基金support of the Guangdong Basic and Applied Basic Research Foundation(grant nos.2020A1515110705 and 2021A1515110245)the China Postdoctoral Science Foundation(grant nos.2020M682711 and 2020M682710)+2 种基金the National Program for Support of Topnotch Young Professionals(grant no.x2qsA4210090)the National Natural Science Foundation of China(grant no.31971614)the State Key Laboratory of Pulp and Paper Engineering(grant no.2020C03).
文摘Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.
文摘硬炭因资源丰富、结构稳定及安全性高等优势,已成为钠离子电池常用阳极材料。其中,煤基衍生硬炭受到了广泛的关注。本工作以长焰煤为碳源,硫脲为氮硫源,NaCl为模板,通过两步炭化工艺和杂原子掺杂相结合的方法合成了N和S共掺杂的煤基硬炭(NSPC1200)。两步炭化过程在调节碳微晶结构和扩大层间距方面发挥了重要的作用。N和S的共掺杂调节了炭材料的电子结构,赋予其更多的活性位点;此外,引入NaCl作为模板有助于孔结构的构建,有利于电极和电解质之间的接触,从而实现Na+和电子的有效传输。在协同作用下,样品NSPC1200表现出优异的储钠能力,在20 mA g^(−1)电流密度下呈现314.2 mAh g^(−1)的可逆容量。即使在100 mA g^(−1)下循环200次,仍保持224.4 mAh g^(−1)的比容量。这项工作成功实现了策略性调整煤基炭材料微观结构的目标,最终获得了具有优异的电化学性能的硬炭阳极。
