Microbial fuel cells have already been used as biosensors to monitor assimilable organic carbon(AOC).However,their signal production from AOC is known to be completely suppressed by dissoved oxygen(DO).In this study,t...Microbial fuel cells have already been used as biosensors to monitor assimilable organic carbon(AOC).However,their signal production from AOC is known to be completely suppressed by dissoved oxygen(DO).In this study,two identical microbial electrolysis cell(MEC)based biosensors were inoculated with marine sediment and operated at two different anodic potentials,namely-300 mV and+250 mV relative to Ag/AgCl.The MEC biosensor operated under positive anodic potential conditions had electrochemically active microbial communities on the anode,including members of the Shewanellaceae,Pseudoalteromonadaceae,and Clostridiaceae families.However,the strictly anaerobic members of the Desulfuromonadaceae,Desulfobulbaceae and Desulfobacteraceae families were found only in the negative anodic potential MEC biosensor.The positive anodic potential MEC biosensor showed several other advantages as well,such as faster start-up,significantly higher maximum current production,fivefold improvement in the AOC detection limit,and tolerance of low dissolved oxygen,compared to those obtained from the negative anodic potential MEC biosensor.The developed positive anodic potential MEC biosensor can thus be used as a real-time and inexpensive detector of AOC concentrations in high saline and low DO seawater.展开更多
Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s...Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.展开更多
A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐cry...A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐crystal X‐ray analysis,Fourier transform infrared spectroscopy,thermogravimetric analyses,CNH elemental analysis and UV‐Vis diffuse reflectance spectroscopy.BUC‐21exhibited an excellent performance for photocatalytic Cr(VI)reduction with a conversion efficiency of96%,better than that of commercial P25(39%),under UV light irradiation for30min.BUC‐21could also be used to conduct photocatalytic degradation of organic dyes including methylene blue,rhodamine B,methyl orange and reactive red X‐3B.Also,the photocatalytic activity of BUC‐21remained high across a wide pH range from2.0to12.0.It is interesting to note,however,that BUC‐21was unable to achieve simultaneous reduction of Cr(VI)and degradation of an organic pollutant in a mixed matrix,which can be attributed to the competition between Cr(VI)and the organic dyes for access to the photo‐excited electrons.展开更多
Ground improvement has been used on many construction sites to densify granular materials, in other word, to improve soil properties and reduce potential settlement. This work presents a case study of ground improveme...Ground improvement has been used on many construction sites to densify granular materials, in other word, to improve soil properties and reduce potential settlement. This work presents a case study of ground improvement using rapid impact compaction (RIC). The research site comprises the construction of workshop and depots as part of railway development project at Batu Gajah-Ipoh, Malaysia. In-situ testing results show that the subsurface soil comprises mainly of sand and silty sand through the investigated depth extended to 10 m. Groundwater is approximately 0.5 m below the ground surface. Evaluation of improvement was based on the results of pre- and post-improvement cone penetration test (CPT). Interpretation software has been used to infer soil properties. Load test was conducted to estimate soil settlement. It is found that the technique succeeds in improving soil properties namely the relative density increases from 45% to 70%, the friction angle of soil is increased by an average of 3°, and the soil settlement is reduced by 50%: The technique succeeds in improving soil properties to approximately 5.0 m in depth depending on soil uniformity with depth.展开更多
Composite materials composed of LiMnO2, a typical electrode material for lithium ion battery, and a chiral cyanide-bridged Ni(Ⅱ)-Fe(Ⅲ) coordination polymer [NiL2][Fe(CN)6]·4H2O (Ni-Fe, H-form) (L = (1...Composite materials composed of LiMnO2, a typical electrode material for lithium ion battery, and a chiral cyanide-bridged Ni(Ⅱ)-Fe(Ⅲ) coordination polymer [NiL2][Fe(CN)6]·4H2O (Ni-Fe, H-form) (L = (1R,2R)-(-)-1,2-cyclohexane-diamine) or its deuterium isomer, [NiL2][Fe(CN)6]·4D2O (Ni-Fe, D-form) have been prepared by the various ratios (w/w) of Ni-Fe:LiMnO2 = 10:0 (pure Ni-Fe), 9:1, 8:2, 7:3, 6:4, 5:5, 4:6, 3:7, 2:8, 1:9 and 0:10 (pure LiMnO2). Gradual shift of IR (infrared) spectra by changing the ratios and losing difference between H-form and D-form of Ni-Fe due to isotope effects revealed adsorption of Ni-Fe onto LiMnO2 to form composite materials. Formation of composite materials of Ni-Fe and LiMnO2 could be also proved losing ferromagnetic behavior of LiMnO2 on increasing of the ratios of Ni-Fe in each composite. In contrast to smoothly positive thermal expansion of pure LiMnO2 along the crystallographic b axis, variable temperature powder XRD (X-ray diffraction) patterns at 100-300 K of the composite materials exhibited thermally-accessible lattice distortion along the b axis with different ratios. It is also proved deviation of ideal linear correlation of an evaluation function, In K = a/T + b (where, K = (d(T) - d(0))/d(T), d(T) denotes nλ/(sin 2θ) at T (K)).展开更多
Based on a previous investigation,a simulation model was used for optimization of coproduction of ethyl acetate and n-butyl acetate by reactive distillation.An experimental setup was established to verify the simulate...Based on a previous investigation,a simulation model was used for optimization of coproduction of ethyl acetate and n-butyl acetate by reactive distillation.An experimental setup was established to verify the simulated results.The effects of various operating variables,such as ethanol feed location,acetic acid feed location,feed stage of reaction mixture of acetic acid and n-butanol,reflux ratio of ethyl acetate reactive distillation column,and distillate to feed ratio of n-butyl acetate column,on the ethanol/n-butanol conversions,ethyl acetate/n-butyl acetate purity,and energy consumption were investigated.The optimal results in the simulation study are as follows:ethanol feed location,15th stage;acetic acid feed location,eighth stage;feed location of reaction mixture of acetic acid and n-butanol,eighth stage;reflux ratio of ethyl acetate reactive distillation column,2.0;and distillate to feed ratio of n-butyl acetate,0.6.展开更多
Porous biomaterials are widely used as bone replacement materials because of thers high biocompatibility and osteoconductivity property. Understanding of their porous structure (i.e. geometrical and topological charac...Porous biomaterials are widely used as bone replacement materials because of thers high biocompatibility and osteoconductivity property. Understanding of their porous structure (i.e. geometrical and topological characteristic) and studying how to the body fluid flow through them are essential to investigate the degradation behaviour at the surface-liquid interface. This research develops a numerical model to simulate the porous structure of biomaterials based on the stochastic approach in pore size distribution and interconnectivity.展开更多
The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical applicatio...The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical application requires 2eORR electrocatalysts with high activity and selectivity.Herein,we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers(Ni-NPs/BCCF)via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2 e-ORR to H_(2)O_(2).By tuning the amount of Ni precursor,the best electrocatalytic performance toward 2 eORR was achieved for Ni-NPs/BCCF-20.7,affording a high H_(2)O_(2) selectivity of ~90% and an onset potential of 0.75 V vs.reversible hydrogen electrode(RHE)in an alkaline electrolyte.Ni-NPs/BCCF-20.7 achieved the largest H_(2)O_(2) yield rate of 162.7±13.7 mmol gcat^(-1)h^(-1) and the highest Faradaic efficiency of 93.9%±4.2% at 0.2 and 0.5 V vs.RHE from the bulk ORR system,respectively.Theoretical calculations revealed the more favorable"end-on"adsorption configuration of molecular oxygen on the exposed Ni(111)plane,which can effectively suppress the O-O bond dissociation,resulting in high selectivity for H_(2)O_(2) generation.展开更多
In nature hummingbirds face floral resources whose availability, quality and quantity can vary spatially and temporally. Thus, they must constantly make foraging decisions about which patches, plants and flowers to vi...In nature hummingbirds face floral resources whose availability, quality and quantity can vary spatially and temporally. Thus, they must constantly make foraging decisions about which patches, plants and flowers to visit, partly as a function of the nectar reward. The uncertainty of these decisions would possibly be reduced if an individual could remember locations or use visual cues to avoid revisiting recently depleted flowers. In the present study, we carried out field experiments with white-eared hummingbirds Hylocharis leucotis, to evaluate their use of locations or visual cues when foraging on natural flowers Penstemon roseus. We evaluated the use of spatial memory by observing birds while they were foraging between two plants and within a single plant. Our results showed that hummingbirds prefer to use location when foraging in two plants, but they also use visual cues to efficiently locate unvisited rewarded flowers when they feed on a single plant. However, in absence of visual cues, in both experiments birds mainly used the location of previously visited flowers to make subsequent visits. Our data suggest that hummingbirds are capable of learning and employing this flexibility depending on the faced environmental conditions and the information acquired in previous visits [Current Zoology 57 (4): 468-476, 2011].展开更多
Employing unsymmetrical 2-mercapto-5-methyl-1,3,4-thiadiazole and 2,2′-bipyridine as mixed ligands, a new low-dimensional coordination polymer [Zn(MMTA) 2 (2,2′-bipy)] n (MMTA = 2-mercapto-5-methyl-1,3,4-thiadiazole...Employing unsymmetrical 2-mercapto-5-methyl-1,3,4-thiadiazole and 2,2′-bipyridine as mixed ligands, a new low-dimensional coordination polymer [Zn(MMTA) 2 (2,2′-bipy)] n (MMTA = 2-mercapto-5-methyl-1,3,4-thiadiazole, 2,2′-bipy = 2,2′-bipyridine), has been synthesized under solvothermal condition and characterized by single crystal X-ray diffraction. This compound crys- tallizes in the noncentrosymmetric space group Cc, with cell parameters: a = 8.291(4) , b = 15.483(9) , c = 15.620(6) , = 96.00(5)°, V = 1994.1(2) 3 , and Z = 4. The mixed ligands link the zinc center into a mononuclear unit, which is futher linked by weak C-H···N and C-H···S hydrogen bonds into a three-dimensional noncentrosymmetric framework. The compound exhibits intense photoluminescence and distinct NLO properties at room temperature. The intensity of the green light produced by the powder sample of the compound is about 3.2 times that produced by KDP powder. On the basis of the results of TG analysis, the structure is thermally stable up to ~260 °C.展开更多
Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped ...Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped graphene(BG)-supported bimetallic oxides of Co and Ni were obtained and served as OER electrocatalysts.Surprisingly,the annealed Co-Ni-Ox/BG with a Co/Ni ratio of 1:1 exhibits high performance toward oxygen evolution in alkaline electrolyte.The overpotential is only 310 mV at the current density of 10 mA cm-2,superior to many mono-metallic oxides reported before,and even comparable to the commercial RuO2.The regulation of charge distribution in bimetallic oxides and the strong synergistic coupling effects together contribute to the superior electrocatalytic performance of the Co-Ni-Ox/BG toward OER.This study also offers several effective ways to design high-performance OER electrocatalysts for water splitting.展开更多
Two-dimensional(2D)mesoporous metal-oxide(hydroxide)nanomaterials with defects are promising towards the realization of efficient electrocatalysis.Herein,we report a facile and effective one-pot solvothermal route to ...Two-dimensional(2D)mesoporous metal-oxide(hydroxide)nanomaterials with defects are promising towards the realization of efficient electrocatalysis.Herein,we report a facile and effective one-pot solvothermal route to synthesize mesoporous Mo_(x)-Co-O hybrid nanosheets(NSs)which is composed of crystalline Mo_(4)O_(11) and amorphous cobalt hydroxide.Due to the corrosion of 1-octylamine at high temperatures,abundant mesoporous holes are created in situ over the Mo_(x)-Co-O hybrid NSs during the solvothermal process,which is beneficial to increasing the electrochemical surface area.The dimension of the Mox-Co-O NSs,size of mesoporous and the concentration of defects can be easily modulated by controlling the molar ratio of Mo/Co.Electrochemical measurements reveal that the 2D mesoporous Mo_(x)-Co-O NSs show an excellent activity for the oxygen evolution reaction with the highest catalytic activity of η_(10)=276 mV at 10 mA cm^(−2)in 1 mol L^(−1)KOH.Enhanced adsorption of intermediates and abundant oxygen vacancies achieved by appropriate Mo doping are the two main factors that contribute to the excellent catalytic activity of Mo_(0.2)-Co-O NSs.This work,with the construction of 2D metal-oxide(hydroxide)crystallineamorphous nanomaterials possessing abundant holes,oxygen vacancies and enhanced adsorption of intermediates,provides important insight on the design of more efficient catalysts.展开更多
Energy crisis and environmental problems urgently drive the proposal of new strategies to improve human wellbeing and assist sustainable development.To this end,scientists have explored many metal oxides-based photoca...Energy crisis and environmental problems urgently drive the proposal of new strategies to improve human wellbeing and assist sustainable development.To this end,scientists have explored many metal oxides-based photocatalysts with high stability,low cost,earth abundance,and potentially high catalytic activity relevant for key applications such as H2O splitting,CO2 reduction,N2 fixation,and advanced oxidation of pollutants.In these metal oxides,oxygen vacancies(OVs)are ubiquitous and intrinsic defects with pronounced impacts on the physicochemical properties of the catalysts,which may open new opportunities for obtaining efficient metal oxides.The thorough understanding of the structural and electronic nature of OVs is necessary to determine how they serve as catalytically active sites.In this review,we summarize the origin of OVs,the strategies to introduce OVs,as well as the fundamental structure-activity relationships to relate these crystal defects to catalyst properties including light absorption,charge separation,etc.We emphasize the mechanism of OVs formation and their effects on the intrinsic catalytic characteristics of the metal oxides.We also present some multicomponent catalytic platforms where OVs contribute to catalysis via synergy.Finally,opportunities and challenges on engineering defects in photocatalysts are summarized to highlight the future directions of this research field.展开更多
基金Zhenjiang City Key R&D Plan Modern Agriculture Project(No.SH2021017)Zhenjiang“Jinshan Talents”Project 2021Jiangsu Province“Six Talent Peak”Program(No.XCL-111)。
文摘Microbial fuel cells have already been used as biosensors to monitor assimilable organic carbon(AOC).However,their signal production from AOC is known to be completely suppressed by dissoved oxygen(DO).In this study,two identical microbial electrolysis cell(MEC)based biosensors were inoculated with marine sediment and operated at two different anodic potentials,namely-300 mV and+250 mV relative to Ag/AgCl.The MEC biosensor operated under positive anodic potential conditions had electrochemically active microbial communities on the anode,including members of the Shewanellaceae,Pseudoalteromonadaceae,and Clostridiaceae families.However,the strictly anaerobic members of the Desulfuromonadaceae,Desulfobulbaceae and Desulfobacteraceae families were found only in the negative anodic potential MEC biosensor.The positive anodic potential MEC biosensor showed several other advantages as well,such as faster start-up,significantly higher maximum current production,fivefold improvement in the AOC detection limit,and tolerance of low dissolved oxygen,compared to those obtained from the negative anodic potential MEC biosensor.The developed positive anodic potential MEC biosensor can thus be used as a real-time and inexpensive detector of AOC concentrations in high saline and low DO seawater.
文摘Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.
基金supported by the National Natural Science Foundation of China(51578034)the Beijing Natural Science Foundation&Scientific Research Key Program of Beijing Municipal Commission of Education(KZ201410016018)+1 种基金Beijing Talent Project(2016023)Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(IDHT20170508)~~
文摘A new coordination polymer,Zn(bpy)L(BUC‐21),(H2L=cis‐1,3‐dibenzyl‐2‐imidazolidone‐4,5‐dicarboxylic acid,bpy=4,4′‐bipyridine),has been synthesized under hydrothermal conditions,and characterized by single‐crystal X‐ray analysis,Fourier transform infrared spectroscopy,thermogravimetric analyses,CNH elemental analysis and UV‐Vis diffuse reflectance spectroscopy.BUC‐21exhibited an excellent performance for photocatalytic Cr(VI)reduction with a conversion efficiency of96%,better than that of commercial P25(39%),under UV light irradiation for30min.BUC‐21could also be used to conduct photocatalytic degradation of organic dyes including methylene blue,rhodamine B,methyl orange and reactive red X‐3B.Also,the photocatalytic activity of BUC‐21remained high across a wide pH range from2.0to12.0.It is interesting to note,however,that BUC‐21was unable to achieve simultaneous reduction of Cr(VI)and degradation of an organic pollutant in a mixed matrix,which can be attributed to the competition between Cr(VI)and the organic dyes for access to the photo‐excited electrons.
基金Projects(RG148/12AET,RG086/10AET) supported by the UMRG,MalaysiaProject(PS05812010B) supported by the Post Graduate Research Fund,Malaysia
文摘Ground improvement has been used on many construction sites to densify granular materials, in other word, to improve soil properties and reduce potential settlement. This work presents a case study of ground improvement using rapid impact compaction (RIC). The research site comprises the construction of workshop and depots as part of railway development project at Batu Gajah-Ipoh, Malaysia. In-situ testing results show that the subsurface soil comprises mainly of sand and silty sand through the investigated depth extended to 10 m. Groundwater is approximately 0.5 m below the ground surface. Evaluation of improvement was based on the results of pre- and post-improvement cone penetration test (CPT). Interpretation software has been used to infer soil properties. Load test was conducted to estimate soil settlement. It is found that the technique succeeds in improving soil properties namely the relative density increases from 45% to 70%, the friction angle of soil is increased by an average of 3°, and the soil settlement is reduced by 50%: The technique succeeds in improving soil properties to approximately 5.0 m in depth depending on soil uniformity with depth.
文摘Composite materials composed of LiMnO2, a typical electrode material for lithium ion battery, and a chiral cyanide-bridged Ni(Ⅱ)-Fe(Ⅲ) coordination polymer [NiL2][Fe(CN)6]·4H2O (Ni-Fe, H-form) (L = (1R,2R)-(-)-1,2-cyclohexane-diamine) or its deuterium isomer, [NiL2][Fe(CN)6]·4D2O (Ni-Fe, D-form) have been prepared by the various ratios (w/w) of Ni-Fe:LiMnO2 = 10:0 (pure Ni-Fe), 9:1, 8:2, 7:3, 6:4, 5:5, 4:6, 3:7, 2:8, 1:9 and 0:10 (pure LiMnO2). Gradual shift of IR (infrared) spectra by changing the ratios and losing difference between H-form and D-form of Ni-Fe due to isotope effects revealed adsorption of Ni-Fe onto LiMnO2 to form composite materials. Formation of composite materials of Ni-Fe and LiMnO2 could be also proved losing ferromagnetic behavior of LiMnO2 on increasing of the ratios of Ni-Fe in each composite. In contrast to smoothly positive thermal expansion of pure LiMnO2 along the crystallographic b axis, variable temperature powder XRD (X-ray diffraction) patterns at 100-300 K of the composite materials exhibited thermally-accessible lattice distortion along the b axis with different ratios. It is also proved deviation of ideal linear correlation of an evaluation function, In K = a/T + b (where, K = (d(T) - d(0))/d(T), d(T) denotes nλ/(sin 2θ) at T (K)).
基金Supported by the National Natural Science Foundation of China(21376053)
文摘Based on a previous investigation,a simulation model was used for optimization of coproduction of ethyl acetate and n-butyl acetate by reactive distillation.An experimental setup was established to verify the simulated results.The effects of various operating variables,such as ethanol feed location,acetic acid feed location,feed stage of reaction mixture of acetic acid and n-butanol,reflux ratio of ethyl acetate reactive distillation column,and distillate to feed ratio of n-butyl acetate column,on the ethanol/n-butanol conversions,ethyl acetate/n-butyl acetate purity,and energy consumption were investigated.The optimal results in the simulation study are as follows:ethanol feed location,15th stage;acetic acid feed location,eighth stage;feed location of reaction mixture of acetic acid and n-butanol,eighth stage;reflux ratio of ethyl acetate reactive distillation column,2.0;and distillate to feed ratio of n-butyl acetate,0.6.
基金Funded by"973" project which serial number is G19990 6 4 70 1
文摘Porous biomaterials are widely used as bone replacement materials because of thers high biocompatibility and osteoconductivity property. Understanding of their porous structure (i.e. geometrical and topological characteristic) and studying how to the body fluid flow through them are essential to investigate the degradation behaviour at the surface-liquid interface. This research develops a numerical model to simulate the porous structure of biomaterials based on the stochastic approach in pore size distribution and interconnectivity.
基金financially supported by the National Natural Science Foundation of China(51872292)China Postdoctoral Science Foundation(E04BFGCV)the CASHIPS Director’s Fund(YZJJ2021QN18)。
文摘The decentralized production of H_(2)O_(2) via a twoelectron oxygen reduction reaction(2e^(-)ORR)has emerged as a promising alternative to the energy-intensive anthraquinone(AQ)process.However,its practical application requires 2eORR electrocatalysts with high activity and selectivity.Herein,we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers(Ni-NPs/BCCF)via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2 e-ORR to H_(2)O_(2).By tuning the amount of Ni precursor,the best electrocatalytic performance toward 2 eORR was achieved for Ni-NPs/BCCF-20.7,affording a high H_(2)O_(2) selectivity of ~90% and an onset potential of 0.75 V vs.reversible hydrogen electrode(RHE)in an alkaline electrolyte.Ni-NPs/BCCF-20.7 achieved the largest H_(2)O_(2) yield rate of 162.7±13.7 mmol gcat^(-1)h^(-1) and the highest Faradaic efficiency of 93.9%±4.2% at 0.2 and 0.5 V vs.RHE from the bulk ORR system,respectively.Theoretical calculations revealed the more favorable"end-on"adsorption configuration of molecular oxygen on the exposed Ni(111)plane,which can effectively suppress the O-O bond dissociation,resulting in high selectivity for H_(2)O_(2) generation.
文摘In nature hummingbirds face floral resources whose availability, quality and quantity can vary spatially and temporally. Thus, they must constantly make foraging decisions about which patches, plants and flowers to visit, partly as a function of the nectar reward. The uncertainty of these decisions would possibly be reduced if an individual could remember locations or use visual cues to avoid revisiting recently depleted flowers. In the present study, we carried out field experiments with white-eared hummingbirds Hylocharis leucotis, to evaluate their use of locations or visual cues when foraging on natural flowers Penstemon roseus. We evaluated the use of spatial memory by observing birds while they were foraging between two plants and within a single plant. Our results showed that hummingbirds prefer to use location when foraging in two plants, but they also use visual cues to efficiently locate unvisited rewarded flowers when they feed on a single plant. However, in absence of visual cues, in both experiments birds mainly used the location of previously visited flowers to make subsequent visits. Our data suggest that hummingbirds are capable of learning and employing this flexibility depending on the faced environmental conditions and the information acquired in previous visits [Current Zoology 57 (4): 468-476, 2011].
基金supported by the National Natural Science Foundation of China (20701023 & 51102138)the Natural Science Foundation of Shandong Province, China (BS2010NJ004 &2009ZRB019KH)
文摘Employing unsymmetrical 2-mercapto-5-methyl-1,3,4-thiadiazole and 2,2′-bipyridine as mixed ligands, a new low-dimensional coordination polymer [Zn(MMTA) 2 (2,2′-bipy)] n (MMTA = 2-mercapto-5-methyl-1,3,4-thiadiazole, 2,2′-bipy = 2,2′-bipyridine), has been synthesized under solvothermal condition and characterized by single crystal X-ray diffraction. This compound crys- tallizes in the noncentrosymmetric space group Cc, with cell parameters: a = 8.291(4) , b = 15.483(9) , c = 15.620(6) , = 96.00(5)°, V = 1994.1(2) 3 , and Z = 4. The mixed ligands link the zinc center into a mononuclear unit, which is futher linked by weak C-H···N and C-H···S hydrogen bonds into a three-dimensional noncentrosymmetric framework. The compound exhibits intense photoluminescence and distinct NLO properties at room temperature. The intensity of the green light produced by the powder sample of the compound is about 3.2 times that produced by KDP powder. On the basis of the results of TG analysis, the structure is thermally stable up to ~260 °C.
基金the financial supports from the National Natural Science Foundation of China(21902062 and 21705056)the Natural Science Foundation of Shandong Province(ZR2019YQ10 and ZR2018PB009)+1 种基金the Young Taishan Scholars Program(tsqn201812080)the Open Funds of the State Key Laboratory of Electroanalytical Chemistry(SKLEAC201901)。
文摘Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped graphene(BG)-supported bimetallic oxides of Co and Ni were obtained and served as OER electrocatalysts.Surprisingly,the annealed Co-Ni-Ox/BG with a Co/Ni ratio of 1:1 exhibits high performance toward oxygen evolution in alkaline electrolyte.The overpotential is only 310 mV at the current density of 10 mA cm-2,superior to many mono-metallic oxides reported before,and even comparable to the commercial RuO2.The regulation of charge distribution in bimetallic oxides and the strong synergistic coupling effects together contribute to the superior electrocatalytic performance of the Co-Ni-Ox/BG toward OER.This study also offers several effective ways to design high-performance OER electrocatalysts for water splitting.
基金the National Key R&D Program of China(2020YFB1505802)the Ministry of Science and Technology(2017YFA0208200)+1 种基金the National Natural Science Foundation of China(22025108,U21A20327,and 22121001)the Start-up Funds from Xiamen University.
文摘Two-dimensional(2D)mesoporous metal-oxide(hydroxide)nanomaterials with defects are promising towards the realization of efficient electrocatalysis.Herein,we report a facile and effective one-pot solvothermal route to synthesize mesoporous Mo_(x)-Co-O hybrid nanosheets(NSs)which is composed of crystalline Mo_(4)O_(11) and amorphous cobalt hydroxide.Due to the corrosion of 1-octylamine at high temperatures,abundant mesoporous holes are created in situ over the Mo_(x)-Co-O hybrid NSs during the solvothermal process,which is beneficial to increasing the electrochemical surface area.The dimension of the Mox-Co-O NSs,size of mesoporous and the concentration of defects can be easily modulated by controlling the molar ratio of Mo/Co.Electrochemical measurements reveal that the 2D mesoporous Mo_(x)-Co-O NSs show an excellent activity for the oxygen evolution reaction with the highest catalytic activity of η_(10)=276 mV at 10 mA cm^(−2)in 1 mol L^(−1)KOH.Enhanced adsorption of intermediates and abundant oxygen vacancies achieved by appropriate Mo doping are the two main factors that contribute to the excellent catalytic activity of Mo_(0.2)-Co-O NSs.This work,with the construction of 2D metal-oxide(hydroxide)crystallineamorphous nanomaterials possessing abundant holes,oxygen vacancies and enhanced adsorption of intermediates,provides important insight on the design of more efficient catalysts.
基金financially supported by the National Natural Science Foundation of China(U1905215,51772053 and 51672046)。
文摘Energy crisis and environmental problems urgently drive the proposal of new strategies to improve human wellbeing and assist sustainable development.To this end,scientists have explored many metal oxides-based photocatalysts with high stability,low cost,earth abundance,and potentially high catalytic activity relevant for key applications such as H2O splitting,CO2 reduction,N2 fixation,and advanced oxidation of pollutants.In these metal oxides,oxygen vacancies(OVs)are ubiquitous and intrinsic defects with pronounced impacts on the physicochemical properties of the catalysts,which may open new opportunities for obtaining efficient metal oxides.The thorough understanding of the structural and electronic nature of OVs is necessary to determine how they serve as catalytically active sites.In this review,we summarize the origin of OVs,the strategies to introduce OVs,as well as the fundamental structure-activity relationships to relate these crystal defects to catalyst properties including light absorption,charge separation,etc.We emphasize the mechanism of OVs formation and their effects on the intrinsic catalytic characteristics of the metal oxides.We also present some multicomponent catalytic platforms where OVs contribute to catalysis via synergy.Finally,opportunities and challenges on engineering defects in photocatalysts are summarized to highlight the future directions of this research field.