Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts ...Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.展开更多
Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of...Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of photothermal catalytic removal of volatile organic compounds(VOCs)by nano-catalysts in recent years is systematically reviewed.First,the fundamentals of photothermal catalysis and the fabrication of catalysts are described,and the design strategy of optimizing photothermal catalysis performance is proposed.Second,the performance for VOC degradation with photothermal catalysis is evaluated and compared for the batch and continuous systems.Particularly,the catalytic mechanism of VOC oxidation is systematically introduced based on experimental and theoretical study.Finally,the future limitations and challenges have been discussed,and potential research directions and priorities are highlighted.A broad view of recent photothermal catalyst fabrication,applications,challenges,and prospects can be systemically provided by this review.展开更多
Alcohol fuel electro-reforming is promising for green hydrogen generation while developing efficient bifunctional catalysts for alcohol fuel electrolysis is still very tricky.Herein,we for the first time proposed the ...Alcohol fuel electro-reforming is promising for green hydrogen generation while developing efficient bifunctional catalysts for alcohol fuel electrolysis is still very tricky.Herein,we for the first time proposed the electron-enriched Pt induced by CoSe_(2)has an efficient bi-functional catalytic ability for alcohol fuels electro-reforming of hydrogen in acid electrolytes.The theoretical calculation revealed the advantages of electron-enriched Pt surface for the adsorption of intermediate,which is well supported by spectroscopic analysis and CO-stripping techniques.Largely improved catalytic performances of activity,durability,and kinetics are demonstrated compared to the conventional alloy system and commercial Pt/C catalyst,due to the efficient synergism of Pt and CoSe_(2);the peak current density of Pt/CoSe_(2)for methanol(ethanol)oxidation is 87.61(48.27)m A cm^(-2),which is about 3.3(2.0)times higher than that of Pt/C catalyst and 2.0(1.5)times that of the traditional PtCo alloy catalysts.Impressively,about 80%of the initial current was found after 1000 cycles of stability test for alcohol fuel oxidation of Pt/CoSe_(2)catalyst,higher than that of Pt/C(ca.50%)and PtCo catalyst(65%).When Pt/CoSe_(2)catalyst serviced as bi-functional catalysts for electrolyzer,a low cell potential of 0.65(0.78)V for methanol(ethanol)electrolysis was required to reach 10 m A cm^(-2),which was about 1030(900)m V less than that of conventional water electrolysis using Pt/C as the catalyst.The current result is instructive for the design of novel bifunctional catalyst and the understanding of hydrogen generation via alcohol fuel electro-reforming.展开更多
A series of SiO2/β-Zn4Sb3 core-shell composite particles with 3, 6, 9, and 12 nm of SiO2 shell in thickness were prepared by coatingβ-Zn4Sb3 microparticles with SiO2 nanoparticles formed by hydrolyzing the tetraetho...A series of SiO2/β-Zn4Sb3 core-shell composite particles with 3, 6, 9, and 12 nm of SiO2 shell in thickness were prepared by coatingβ-Zn4Sb3 microparticles with SiO2 nanoparticles formed by hydrolyzing the tetraethoxysilane in alcohol-alkali-water solution. SiO2/β-Zn4Sb3 nanocomposite thermoelectric materials were fabricated with these core-shell composite particles by spark plasma sintering (SPS) method. Microstructure, phase composition, and thermoelectric properties of SiO2/β-Zn4Sb3 nanocomposite thermoelectric materials were systemically investigated. The results show thatβ-Zn4Sb3 microparticles are uniformly coated by SiO2 nanoparticles, and no any phase transformation reaction takes place during SPS process. The electrical and thermal conductivity gradually decreases, and the Seebeck coefficient increases compared to that ofβ-Zn4Sb3 bulk material, but the increment of Seebeck coefficient in high temperature range remarkably increases. The thermal conductivity of SiO2/β-Zn4Sb3 nanocomposite material with 12 nm of SiO2 shell is the lowest and only 0.56 W·m^-1·K^-1 at 460 K. As a result, the ZT value of the SiO2/β-Zn4Sb3 nanocomposite material reaches 0.87 at 700 K and increases by 30%.展开更多
Direct liquid fuel cells(DLFCs) have received increasing attention because of their high energy densities,instant recharging abilities, simple cell structure, and facile storage and transport. The main challenge for t...Direct liquid fuel cells(DLFCs) have received increasing attention because of their high energy densities,instant recharging abilities, simple cell structure, and facile storage and transport. The main challenge for the commercialization of DLFCs is the high loading requirement of platinum group metals(PGMs) as catalysts. Atomically dispersed catalysts(ADCs) have been brought into recent focus for DLFCs due to their well-defined active sites, high selectivity, maximal atom-utilization, and anti-poisoning property. In this review, we summarized the structure–property relationship for unveiling the underlying mechanisms of ADCs for DLFCs. More specifically, different types of fuels used in DLFCs such as methanol, formic acid,and ethanol were discussed. At last, we highlighted current challenges, research directions, and future outlooks towards the practical application of DLFCs.展开更多
BACKGROUND: Numerous studies have shown that tumor necrosis factor α (TNF-α) is closely correlated with spinal cord injury (SCI), but the mechanisms of TNF-α and therapeutic treatments for SCI are still poorly...BACKGROUND: Numerous studies have shown that tumor necrosis factor α (TNF-α) is closely correlated with spinal cord injury (SCI), but the mechanisms of TNF-α and therapeutic treatments for SCI are still poorly understood. OBJECTIVE: To determine the role of TNF-α in the pathogenesis of SCI. DESIGN, TIME AND SETTING: An in vivo experiment based on genetically engineered animals was performed at the Medical University of South Carolina, Charleston, South Carolina, USA, between June 2007 and October 2008. MATERIALS: TNF-α transgenic rats (Xenogen Biosciences in Cranbury, New Jersey, USA) were utilized in this study. METHODS: TNF-α transgenic (tg) and wild-type (WT) rats underwent a complete single-level laminectomy at the 10^th thoracic vertebra (T10). MAIN OUTCOME MEASURES: Motor function of rat hindlimb was assessed using the Basso, Beattie, and Bresnahan hindlimb locomotor rating scale. Histological evaluation of spinal cord tissue loss was conducted. Immunohistochemistry for astrocytes, microglia/macrophages, and TNF receptors (TNFRs) was performed on spinal cord tissue sections. TNF-α mRNA expression was detected by real-time polymerase chain reaction. The concentrations of nerve growth factor (NGF) and brain-derived neurotrophic factor (BDNF) in the supernatant were determined using an enzyme-linked immunosorbent assay kit for rat NGF or BDNF, respectively. The rats were injected subcutaneously with etanercept to verify that TNF-α was the direct effect of the modulation of behavioral and neurodegenerative outcomes in the TNF-α tg rats. RESULTS: TNF-α tg rats showed higher expression of TNF-α mRNA in the spinal cord prior to SCI. TNF-α tg rats showed worse motor deficits than WT rats in the acute period (〈 3 days) after SCI (P 〈 0.01), while in the chronic period, TNF-α tg rats exhibited persistent elevated baseline levels of TNF-α mRNA and improved recovery in motor function and tissue healing compared to WT rats (P 〈 0.01 ). Following SCI, the number of microglia/macrophages in TNF-α tg rat was always greater than in WT rat (P 〈 0.01). There were no significant differences in NGF and BDNF levels in the supernatant of spinal cord homogenates. TNFR1 expression was significantly greater in the TNF-α tg rats compared to the WT rats (P 〈 0.01). However, TNFR2 expression did not reveal a significant increase in the TNF-α tg rats compared to the WT rats. Finally, treatment with etanercept reduced injury acutely, but exacerbated the injury chronically. CONCLUSION: Overexpression of TNF-α is deleterious in the acute phase, but beneficial in the chronic phase in the response to SCI. The role of TNF-α post-injury may depend on TNF-α expression in the spinal cord and its differential binding to TNFRI. Our observations may have clinical relevance that antagonists or inhibitors of TNF-α could be administered within the early time window post-injury, and appropriate amounts of TNF-α could be administered during the chronic stage, in order to improve the final neurological recovery in patients with SCI.展开更多
Copper oxides and its salts are now widely used as pesticides to control fungal and bacterial diseases of field crops. Copper toxicity is often a major contributor of human health problems caused through accumulation ...Copper oxides and its salts are now widely used as pesticides to control fungal and bacterial diseases of field crops. Copper toxicity is often a major contributor of human health problems caused through accumulation of excess copper ions in various organs via drinking water, fruits and vegetables. So, detection and estimation of cupric ions in biological organs, drinking water, fruits and vegetables are extremely important. Recently, a fluorescence based sensor using coumarin dye (high quantum yield) has been proposed to detect micromolar Cu++ ion in biological organs. But major problem with coumarin dye is that it is insoluble in water and undergoes dye-dye aggregation in organic solvents. We proposed here a synthetic scheme of preparation of graphene oxide conjugated coumarin dye derivative which would be water dispersible and expected to be an ideal candidate for Cu2+ ion estimation in biological organs and drinking water.展开更多
Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of bot...Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of both metal-air batteries and fuel cells,and precious metals are the dominant catalysts carrying out the ORR in their cathodes.However,how to manipulate the electronic structure of precious metals as active sites to further promote ORR performance and maximize the utilization rate is still under development.Metal oxide serves as suitable and promising support that can strongly interact with precious metals for both activity and durability enhancement.Herein,we present recent research updates on strong precious metal-metal oxide interaction(SPMMOI)utilized in ORR.We start by introducing the background of ORR,the issues to be solved,and its practical applications followed by a thorough discussion of the reaction mechanism and comprehensive evaluation protocols of performance.We then provide a complete understanding of theworking principle of SPMMOI and highlight the related advances.Finally,we summarize the merits of the precious metal-metal oxide systemand propose the research direction aswell as some urgent problems to be addressed in the future.展开更多
Seawater electrolysis(SWE)provides a promising and efficient pathway to produce green hydrogen.However,the current SWE technology confronts a lot of challenges,such as the sluggish reaction kinetics on the anode side,...Seawater electrolysis(SWE)provides a promising and efficient pathway to produce green hydrogen.However,the current SWE technology confronts a lot of challenges,such as the sluggish reaction kinetics on the anode side,and a lot of impurities and ions in seawater that poison the active sites of the catalyst and block membrane pores.In addition,the existence of chloride ions(Cl−)in seawater will strongly compete with oxygen evolution reaction(OER)by the chlorine oxidation/evolution reaction(ClOR/ClER)on the anode side as a result of the extremely similar thermodynamic potentials.Thus,to move SWE much closer to commercialization,it is highly desirable to enhance not only the activity of electrocatalysts but also the selectivity and stability of efficient OER to restrain ClOR/ClER.At the same time,the additive of electrolytes and the unique structural design of the electrolyzer also promote the development of SWE.In this review,the fundamental mechanisms for SWE and water electrolysis are first introduced and compared.Then,the design principles of efficient catalysts,electrolytes,surface/interface engineering,and novelty reaction device are critically,comprehensively summarized and analyzed.Finally,perspectives,challenges,and opportunities to develop and boost SWE technologies are proposed.展开更多
Rh single atom catalysts(SACs)have been insensitively investigated recently due to the maximum utilization efficiency of Rh,one of the most expensive precious metals.Although great efforts have been made in the develo...Rh single atom catalysts(SACs)have been insensitively investigated recently due to the maximum utilization efficiency of Rh,one of the most expensive precious metals.Although great efforts have been made in the development and application of Rh SACs,there are few reports on the precise control of the local coordination environment of Rh single sites on CeO_(2) and their catalytic performance for N_(2)O decomposition.Herein,Rh/CeO_(2) catalysts with different Rh-O coordination numbers(CNs)were successfully prepared using different CeO_(2) supports and a simple incipient wetness impregnation(IWI)method.It is observed that the Rh/CeO_(2) catalyst with slightly higher CN of Rh-O(Rh/CeO_(2)-H)prepared from CeO_(2) shows much higher N_(2)O decomposition activity than the catalyst with lower CN of Rh-O(Rh/CeO_(2)-L)obtained from Ce(OH)_(x).The Rh species within Rh/CeO_(2)-H are found to be more reactive than those within Rh/CeO_(2)-L,which can better facilitate the O_(2)desorption once formed during N_(2)O deco mposition.In additio n,more surface oxygen vacancies are present on Rh/CeO_(2)-H than on Rh/CeO_(2)-L,well explaining the superior N_(2)O adsorption and activation capability on the former catalyst.It is concluded that more abundant oxygen vacancies and reactive Rh single atom sites with slightly higher CN of Rh-O and significantly higher reducibility altogether contribute to the superior N_(2)O decomposition activity on the Rh/CeO_(2)-H catalyst.展开更多
Organic electrochemical transistors(OECTs)have been hailed as highly sensitive biomolecular sensors among organic electronic devices due to their superior stability in an aqueous environment and high transconductance....Organic electrochemical transistors(OECTs)have been hailed as highly sensitive biomolecular sensors among organic electronic devices due to their superior stability in an aqueous environment and high transconductance.At the same time,plasmon based sensors are known to provide high sensitivity for biosensing due to the highly localized plasmonic field.Here we report a plasmonic OECT(POET)device that synchronizes the advantages of OECTs and plasmonic sensors on a single platform.The platform is fabricated by a simple,cost-effective,and high-throughput nanoimprinting process,which allows plasmonic resonance peak tuning to a given visible wavelength of interest for versatile biosensing.With glucose sensing as proof,a five-times sensitivity enhancement is obtained for POET compared to a regular(non-plasmonic)OECT.Thus,the POET paves the way to a new paradigm of optoelectronic sensors that combines the inherent high sensitivity of OECTs and localized plasmonic field to sense a vast realm of biomolecules.展开更多
Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto t...Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto the edges of two-dimensional(2D)1Tphase MoS_(2)(Pt1/1T-MOS_(2)SAC)as a proof-of-concept catalyst can efficiently convert biomass-derived MAH to SA with 100%conversion and 100%selectivity under mild conditions.The kinetic data and characterization results suggest that the catalytic performance of the edge-anchored Pt1/1T-MoS_(2)SAC originates from the facile H_(2)dissociation induced by the electron-deficient Pt1atoms and the pocket-like configuration of Pt1active site confines the adsorption configuration of MAH by the steric effect.The strategy of fabricating edge-confined catalysts offers a new direction to design novel SACs for biomass-derived transformations.展开更多
The disability,mortality and costs due to ionizing radiation(IR)-induced osteoporotic bone fractures are sub-stantial and no effective therapy exists.Ionizing radiation increases cellular oxidative damage,causing an i...The disability,mortality and costs due to ionizing radiation(IR)-induced osteoporotic bone fractures are sub-stantial and no effective therapy exists.Ionizing radiation increases cellular oxidative damage,causing an imbalance in bone turnover that is primarily driven via heightened activity of the bone-resorbing osteoclast.We demonstrate that rats exposed to sublethal levels of IR develop fragile,osteoporotic bone.At reactive surface sites,cerium ions have the ability to easily undergo redox cycling:drastically adjusting their electronic con-figurations and versatile catalytic activities.These properties make cerium oxide nanomaterials fascinating.We show that an engineered artificial nanozyme composed of cerium oxide,and designed to possess a higher fraction of trivalent(Ce^(3+))surface sites,mitigates the IR-induced loss in bone area,bone architecture,and strength.These investigations also demonstrate that our nanozyme furnishes several mechanistic avenues of protection and selectively targets highly damaging reactive oxygen species,protecting the rats against IR-induced DNA damage,cellular senescence,and elevated osteoclastic activity in vitro and in vivo.Further,we reveal that our nanozyme is a previously unreported key regulator of osteoclast formation derived from macrophages while also directly targeting bone progenitor cells,favoring new bone formation despite its exposure to harmful levels of IR in vitro.These findings open a new approach for the specific prevention of IR-induced bone loss using synthesis-mediated designer multifunctional nanomaterials.展开更多
Benchtop tissue cultures have become increasingly complex in recent years,as more on-a-chip biological technologies,such as microphysiological systems(MPS),are developed to incorporate cellular constructs that more ac...Benchtop tissue cultures have become increasingly complex in recent years,as more on-a-chip biological technologies,such as microphysiological systems(MPS),are developed to incorporate cellular constructs that more accurately represent their respective biological systems.Such MPs have begun facilitating major breakthroughs in biological research and are poised to shape the field in the coming decades.These biological systems require integrated sensing modalities to procure complex,multiplexed datasets with unprecedented combinatorial biological detail.In this work,we expanded upon our polymer-metal biosensor approach by demonstrating a facile technology for compound biosensing that was characterized through custom modeling approaches.As reported herein,we developed a compound chip with 3D microelectrodes,3D microfluidics,interdigitated electrodes(IDEs)and a microheater.The chip was subsequently tested using the electrical/electrochemical characterization of 3D microelectrodes with 1 kHz impedance and phase recordings and IDE-based high-frequency(-1 MHz frequencies)impedimetric analysis of differential localized temperature recordings,both of which were modeled through equivalent electrical circuits for process parameter extraction.Additionally,a simplified antibody-conjugation strategy Was employed for a similar IDE-based analysis of the implications of a key analyte(L-glutamine)binding to the equivalent electrical circuit.Finally,acute microfluidic perfusion modeling was performed to demonstrate the ease of microfluidics integration into such a polymer-metal biosensor platform for potential complimentary localized chemical stimulation.Overall,our work demonstrates the design,development,and characterization of an accessibly designed polymer-metal compound biosensor for electrogenic cellular constructs to facilitate comprehensive MPS data collection.展开更多
Intensification of pollution loading worldwide has promoted an escalation of different types of disease-causing microorganisms, such as harmful algal blooms(HABs), instigating detrimental impacts on the quality of rec...Intensification of pollution loading worldwide has promoted an escalation of different types of disease-causing microorganisms, such as harmful algal blooms(HABs), instigating detrimental impacts on the quality of receiving surface waters. Formation of unwanted disinfection by-products(DBPs) resulting from conventional disinfection technologies reveals the need for the development of new sustainable alternatives. Quaternary Ammonium Compounds(QACs) are cationic surfactants widely known for their effective biocidal properties at the ppm level. In this study, a novel silica-based antimicrobial nanofilm was developed using a composite of silica-modified QAC(Fixed-Quat) and applied to a fiberglass mesh as an active surface via sol–gel technique. The synthesized Fixed-Quat nanocoating was found to be effective against E. coli with an inactivation rate of 1.3 × 10^(-3) log reduction/cm min. The Fixed-Quat coated fiberglass mesh also demonstrated successful control of Microcystis aeruginosa with more than 99% inactivation after 10 hr of exposure.The developed antimicrobial mesh was also evaluated with wild-type microalgal species collected in a water body experiencing HABs, obtaining a 97% removal efficiency. Overall,the silica-functionalized Fixed-Quat nanocoating showed promising antimicrobial properties for water disinfection and HABs control, while decreasing concerns related to DBPs formation and the possible release of toxic nanomaterials into the environment.展开更多
Challenges in nanoscale characterization call for non-invasive, yet sensitive subsurface characterization of low-density materials such as polymers. In this work, we present new evidence that mode-synthesizing atomic ...Challenges in nanoscale characterization call for non-invasive, yet sensitive subsurface characterization of low-density materials such as polymers. In this work, we present new evidence that mode-synthesizing atomic force microscopy can be used to detect minute changes in low-density materials, such as those engendered in electro-sensitive polymers during electron beam lithography, surpassing all common nanoscale mechanical techniques. Moreover, we propose 3D reconstruction of the exposed polymer regions using successive high-resolution frames acquired at incremental depths inside the sample. In addition, the results clearly show the influence of increasing dwell time on the depth profile of the nano-sized exposed regions. Hence, the simple approach described here can be used for achieving sensitive nanoscale tomography of soft materials with promising applications in material sciences and biology.展开更多
A number of mitigation techniques exist to reduce the emissions of pollutant gases and greenhouse gases(GHGs) from anaerobic storage of livestock manure. Nanoparticle(NP)application is a promising mitigating treatment...A number of mitigation techniques exist to reduce the emissions of pollutant gases and greenhouse gases(GHGs) from anaerobic storage of livestock manure. Nanoparticle(NP)application is a promising mitigating treatment option for pollutant gases, but limited research is available on the mode of NP application and their effectiveness in gaseous emission reduction. In this study, zinc silica nanogel(ZnSNL), copper silica nanogel(CuSNL), and N-acetyl cysteine(NACL) coated zinc oxide quantum dot(Qdot) NPs were compared to a control lacking NPs. All three NPs tested significantly reduced gas production and concentrations compared to non-treated manure. Overall, cumulative gas volumes were reduced by 92.73%–95.83%, and concentrations reduced by 48.98%–99.75% for H_2S, and 20.24%–99.82% for GHGs. Thus, application of NPs is a potential treatment option for mitigating pollutant and GHG emissions from anaerobically stored manure.展开更多
Devising an electrocatalyst with brilliant efficiency and satisfactory durability for hydrogen production is of considerable demand,especially for large-scale application.Herein,we adopt a multi-step consequential ind...Devising an electrocatalyst with brilliant efficiency and satisfactory durability for hydrogen production is of considerable demand,especially for large-scale application.Herein,we adopt a multi-step consequential induced strategy to construct a bifunctional electrocatalyst for the overall water splitting.Graphene oxide(GO)was used as a carbon matrix and in situ oxygen source,which was supported by the octahedral PtNi alloy to form the PtxNiy-GO precursor.When calcinating in Ar atmosphere,the oxygen in GO induced the surface segregation of Ni from the PtNi octahedron to form a core-shell structure of Ptx@Niy.Then,the surface-enriched Ni continuously induced the reformation of C in reduced graphene oxide(rGO)to enhance the degree of graphitization.This multi-step induction formed a nanocatalyst Pt_(x)@Ni_(y)-rGO which has very high catalytic efficiency and stability.By optimizing the feeding ratio of PtNi(Pt:Ni=1:2),the electrolytic overall water splitting at 10 mA·cm^(-2) can be driven by an electrolytic voltage of as low as 1.485 V,and hydrogen evolution reaction(HER)only needs an overpotential of 37 mV in 1.0 M KOH aqueous solution.Additionally,the catalyst exhibited consistent existence form in both HER and oxygen evolution reaction(OER),which was verified by switching the anode and cathode of the cell in the electrolysis of water.This work provides a new idea for the synthesis and evaluation of the bifunctional catalysts for water splitting.展开更多
Functional surfaces that can control light across the electromagnetic spectrum are highly desirable.Plasmonic nanostructures can assume this role by exhibiting dimension-tunable resonances that span multiple electroma...Functional surfaces that can control light across the electromagnetic spectrum are highly desirable.Plasmonic nanostructures can assume this role by exhibiting dimension-tunable resonances that span multiple electromagnetic regimes.However,changing these structural parameters often impacts the higher-order resonances and spectral features in lower-wavelength domains.In this study,we discuss a cavity-coupled plasmonic system with resonances that are tunable across the 3–5 or 8–14μm infrared bands while retaining near-invariant spectral properties in the visible domain.This result is accomplished by regime-dependent resonance mechanisms and their dependence on independent structural parameters.Through the identification and constraint of key parameters,we demonstrate multispectral data encoding,where images,viewable in the infrared spectral domain,appear as uniform areas of color in the visible domain—effectively hiding the information.Fabricated by large area nanoimprint lithography and compatible with flexible surfaces,the proposed system can produce multifunctional coatings for thermal management,camouflage,and anti-counterfeiting.展开更多
基金supported by the National Natural Science Foundation of China(No.21972124,22102105)a project funded by the Priority Academic Program Development of Jiangsu Higher Education InstitutionL.Feng also thanks the support of the Six Talent Peaks Project of Jiangsu Province(XCL-070-2018).
文摘Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.
文摘实现绿色甲醇电解制氢需要高效的双功能催化剂。本文采用热处理结合乙二醇还原法成功制备了MoP-NC纳米球负载的超细Pt纳米粒子(平均粒径为2.53 nm)复合催化剂(Pt/MoP-NC)用于高效甲醇电解制氢。MoP-NC纳米球不仅能提高Pt纳米粒子的分散性并且增强Pt的抗中毒能力。电化学测试表明Pt/MoP-NC催化剂在酸性甲醇氧化反应(MOR)和析氢反应(HER)中具有较高的催化性能;其中,MOR的正向扫描峰值电流密度为90.7 m A·cm^(-2),是商业Pt/C催化剂的3.2倍,在10 mA·cm^(-2)的电流密度下,HER的过电位低至30 m V,与商业Pt/C接近。由Pt/MoP-NC||Pt/MoP-NC组装的两电极电解槽驱动10 mA·cm^(-2)的电流密度仅需要0.67 V的电压,比相同条件下电解水的电压低1.02 V,大大降低了能量输入。Pt/MoP-NC的高催化性能主要来源于Pt活性中心与相邻层状多孔球形结构的MoP-NC载体之间电子效应及配体效应引起的抗一氧化碳中毒能力的提升和含氧物种的容易生成。
基金sponsored financially by the National Natural Science Foundation of China (No.21906104 and No.12175145)the Shanghai Rising-Star Program (21QA1406600).
文摘Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of photothermal catalytic removal of volatile organic compounds(VOCs)by nano-catalysts in recent years is systematically reviewed.First,the fundamentals of photothermal catalysis and the fabrication of catalysts are described,and the design strategy of optimizing photothermal catalysis performance is proposed.Second,the performance for VOC degradation with photothermal catalysis is evaluated and compared for the batch and continuous systems.Particularly,the catalytic mechanism of VOC oxidation is systematically introduced based on experimental and theoretical study.Finally,the future limitations and challenges have been discussed,and potential research directions and priorities are highlighted.A broad view of recent photothermal catalyst fabrication,applications,challenges,and prospects can be systemically provided by this review.
基金supported by the National Natural Science Foundation of China(21972124,22102105)a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionthe support of the Six Talent Peaks Project of Jiangsu Province(XCL-070-2018)。
文摘Alcohol fuel electro-reforming is promising for green hydrogen generation while developing efficient bifunctional catalysts for alcohol fuel electrolysis is still very tricky.Herein,we for the first time proposed the electron-enriched Pt induced by CoSe_(2)has an efficient bi-functional catalytic ability for alcohol fuels electro-reforming of hydrogen in acid electrolytes.The theoretical calculation revealed the advantages of electron-enriched Pt surface for the adsorption of intermediate,which is well supported by spectroscopic analysis and CO-stripping techniques.Largely improved catalytic performances of activity,durability,and kinetics are demonstrated compared to the conventional alloy system and commercial Pt/C catalyst,due to the efficient synergism of Pt and CoSe_(2);the peak current density of Pt/CoSe_(2)for methanol(ethanol)oxidation is 87.61(48.27)m A cm^(-2),which is about 3.3(2.0)times higher than that of Pt/C catalyst and 2.0(1.5)times that of the traditional PtCo alloy catalysts.Impressively,about 80%of the initial current was found after 1000 cycles of stability test for alcohol fuel oxidation of Pt/CoSe_(2)catalyst,higher than that of Pt/C(ca.50%)and PtCo catalyst(65%).When Pt/CoSe_(2)catalyst serviced as bi-functional catalysts for electrolyzer,a low cell potential of 0.65(0.78)V for methanol(ethanol)electrolysis was required to reach 10 m A cm^(-2),which was about 1030(900)m V less than that of conventional water electrolysis using Pt/C as the catalyst.The current result is instructive for the design of novel bifunctional catalyst and the understanding of hydrogen generation via alcohol fuel electro-reforming.
基金Funded by the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing of Wuhan University of Technology (No. WUT2007M01)
文摘A series of SiO2/β-Zn4Sb3 core-shell composite particles with 3, 6, 9, and 12 nm of SiO2 shell in thickness were prepared by coatingβ-Zn4Sb3 microparticles with SiO2 nanoparticles formed by hydrolyzing the tetraethoxysilane in alcohol-alkali-water solution. SiO2/β-Zn4Sb3 nanocomposite thermoelectric materials were fabricated with these core-shell composite particles by spark plasma sintering (SPS) method. Microstructure, phase composition, and thermoelectric properties of SiO2/β-Zn4Sb3 nanocomposite thermoelectric materials were systemically investigated. The results show thatβ-Zn4Sb3 microparticles are uniformly coated by SiO2 nanoparticles, and no any phase transformation reaction takes place during SPS process. The electrical and thermal conductivity gradually decreases, and the Seebeck coefficient increases compared to that ofβ-Zn4Sb3 bulk material, but the increment of Seebeck coefficient in high temperature range remarkably increases. The thermal conductivity of SiO2/β-Zn4Sb3 nanocomposite material with 12 nm of SiO2 shell is the lowest and only 0.56 W·m^-1·K^-1 at 460 K. As a result, the ZT value of the SiO2/β-Zn4Sb3 nanocomposite material reaches 0.87 at 700 K and increases by 30%.
基金financial supports from the National Science Foundation under Grant Nos. CBET-1949840 and CMMI-1851674financial support from the Preeminent Postdoctoral Program (P3) of the University of Central Florida。
文摘Direct liquid fuel cells(DLFCs) have received increasing attention because of their high energy densities,instant recharging abilities, simple cell structure, and facile storage and transport. The main challenge for the commercialization of DLFCs is the high loading requirement of platinum group metals(PGMs) as catalysts. Atomically dispersed catalysts(ADCs) have been brought into recent focus for DLFCs due to their well-defined active sites, high selectivity, maximal atom-utilization, and anti-poisoning property. In this review, we summarized the structure–property relationship for unveiling the underlying mechanisms of ADCs for DLFCs. More specifically, different types of fuels used in DLFCs such as methanol, formic acid,and ethanol were discussed. At last, we highlighted current challenges, research directions, and future outlooks towards the practical application of DLFCs.
基金the ES016774-01A1VA Merit Award and National Science Foundation EPSCoR grant, No. EPS-0132573+1 种基金EPS-0447660 (MSK)NS050452-05 (JJH)
文摘BACKGROUND: Numerous studies have shown that tumor necrosis factor α (TNF-α) is closely correlated with spinal cord injury (SCI), but the mechanisms of TNF-α and therapeutic treatments for SCI are still poorly understood. OBJECTIVE: To determine the role of TNF-α in the pathogenesis of SCI. DESIGN, TIME AND SETTING: An in vivo experiment based on genetically engineered animals was performed at the Medical University of South Carolina, Charleston, South Carolina, USA, between June 2007 and October 2008. MATERIALS: TNF-α transgenic rats (Xenogen Biosciences in Cranbury, New Jersey, USA) were utilized in this study. METHODS: TNF-α transgenic (tg) and wild-type (WT) rats underwent a complete single-level laminectomy at the 10^th thoracic vertebra (T10). MAIN OUTCOME MEASURES: Motor function of rat hindlimb was assessed using the Basso, Beattie, and Bresnahan hindlimb locomotor rating scale. Histological evaluation of spinal cord tissue loss was conducted. Immunohistochemistry for astrocytes, microglia/macrophages, and TNF receptors (TNFRs) was performed on spinal cord tissue sections. TNF-α mRNA expression was detected by real-time polymerase chain reaction. The concentrations of nerve growth factor (NGF) and brain-derived neurotrophic factor (BDNF) in the supernatant were determined using an enzyme-linked immunosorbent assay kit for rat NGF or BDNF, respectively. The rats were injected subcutaneously with etanercept to verify that TNF-α was the direct effect of the modulation of behavioral and neurodegenerative outcomes in the TNF-α tg rats. RESULTS: TNF-α tg rats showed higher expression of TNF-α mRNA in the spinal cord prior to SCI. TNF-α tg rats showed worse motor deficits than WT rats in the acute period (〈 3 days) after SCI (P 〈 0.01), while in the chronic period, TNF-α tg rats exhibited persistent elevated baseline levels of TNF-α mRNA and improved recovery in motor function and tissue healing compared to WT rats (P 〈 0.01 ). Following SCI, the number of microglia/macrophages in TNF-α tg rat was always greater than in WT rat (P 〈 0.01). There were no significant differences in NGF and BDNF levels in the supernatant of spinal cord homogenates. TNFR1 expression was significantly greater in the TNF-α tg rats compared to the WT rats (P 〈 0.01). However, TNFR2 expression did not reveal a significant increase in the TNF-α tg rats compared to the WT rats. Finally, treatment with etanercept reduced injury acutely, but exacerbated the injury chronically. CONCLUSION: Overexpression of TNF-α is deleterious in the acute phase, but beneficial in the chronic phase in the response to SCI. The role of TNF-α post-injury may depend on TNF-α expression in the spinal cord and its differential binding to TNFRI. Our observations may have clinical relevance that antagonists or inhibitors of TNF-α could be administered within the early time window post-injury, and appropriate amounts of TNF-α could be administered during the chronic stage, in order to improve the final neurological recovery in patients with SCI.
文摘Copper oxides and its salts are now widely used as pesticides to control fungal and bacterial diseases of field crops. Copper toxicity is often a major contributor of human health problems caused through accumulation of excess copper ions in various organs via drinking water, fruits and vegetables. So, detection and estimation of cupric ions in biological organs, drinking water, fruits and vegetables are extremely important. Recently, a fluorescence based sensor using coumarin dye (high quantum yield) has been proposed to detect micromolar Cu++ ion in biological organs. But major problem with coumarin dye is that it is insoluble in water and undergoes dye-dye aggregation in organic solvents. We proposed here a synthetic scheme of preparation of graphene oxide conjugated coumarin dye derivative which would be water dispersible and expected to be an ideal candidate for Cu2+ ion estimation in biological organs and drinking water.
文摘Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of both metal-air batteries and fuel cells,and precious metals are the dominant catalysts carrying out the ORR in their cathodes.However,how to manipulate the electronic structure of precious metals as active sites to further promote ORR performance and maximize the utilization rate is still under development.Metal oxide serves as suitable and promising support that can strongly interact with precious metals for both activity and durability enhancement.Herein,we present recent research updates on strong precious metal-metal oxide interaction(SPMMOI)utilized in ORR.We start by introducing the background of ORR,the issues to be solved,and its practical applications followed by a thorough discussion of the reaction mechanism and comprehensive evaluation protocols of performance.We then provide a complete understanding of theworking principle of SPMMOI and highlight the related advances.Finally,we summarize the merits of the precious metal-metal oxide systemand propose the research direction aswell as some urgent problems to be addressed in the future.
基金the National Science Foundation under grant no.CBET-1949840 and ACS PRF(65481-ND10)the National Natural Science Foundation of China(grant no.22102105)a start-up grant from Northeast Normal University(NENU).
文摘Seawater electrolysis(SWE)provides a promising and efficient pathway to produce green hydrogen.However,the current SWE technology confronts a lot of challenges,such as the sluggish reaction kinetics on the anode side,and a lot of impurities and ions in seawater that poison the active sites of the catalyst and block membrane pores.In addition,the existence of chloride ions(Cl−)in seawater will strongly compete with oxygen evolution reaction(OER)by the chlorine oxidation/evolution reaction(ClOR/ClER)on the anode side as a result of the extremely similar thermodynamic potentials.Thus,to move SWE much closer to commercialization,it is highly desirable to enhance not only the activity of electrocatalysts but also the selectivity and stability of efficient OER to restrain ClOR/ClER.At the same time,the additive of electrolytes and the unique structural design of the electrolyzer also promote the development of SWE.In this review,the fundamental mechanisms for SWE and water electrolysis are first introduced and compared.Then,the design principles of efficient catalysts,electrolytes,surface/interface engineering,and novelty reaction device are critically,comprehensively summarized and analyzed.Finally,perspectives,challenges,and opportunities to develop and boost SWE technologies are proposed.
基金Project supported by the Startup Fund(F.L.)from the University of Central Florida(UCF)National Science Foundation grants(CHE-1955343,DMR-1920050).
文摘Rh single atom catalysts(SACs)have been insensitively investigated recently due to the maximum utilization efficiency of Rh,one of the most expensive precious metals.Although great efforts have been made in the development and application of Rh SACs,there are few reports on the precise control of the local coordination environment of Rh single sites on CeO_(2) and their catalytic performance for N_(2)O decomposition.Herein,Rh/CeO_(2) catalysts with different Rh-O coordination numbers(CNs)were successfully prepared using different CeO_(2) supports and a simple incipient wetness impregnation(IWI)method.It is observed that the Rh/CeO_(2) catalyst with slightly higher CN of Rh-O(Rh/CeO_(2)-H)prepared from CeO_(2) shows much higher N_(2)O decomposition activity than the catalyst with lower CN of Rh-O(Rh/CeO_(2)-L)obtained from Ce(OH)_(x).The Rh species within Rh/CeO_(2)-H are found to be more reactive than those within Rh/CeO_(2)-L,which can better facilitate the O_(2)desorption once formed during N_(2)O deco mposition.In additio n,more surface oxygen vacancies are present on Rh/CeO_(2)-H than on Rh/CeO_(2)-L,well explaining the superior N_(2)O adsorption and activation capability on the former catalyst.It is concluded that more abundant oxygen vacancies and reactive Rh single atom sites with slightly higher CN of Rh-O and significantly higher reducibility altogether contribute to the superior N_(2)O decomposition activity on the Rh/CeO_(2)-H catalyst.
基金J.T.acknowledges the National Science Foundation(CAREER:ECCS-1351757)for financial support.
文摘Organic electrochemical transistors(OECTs)have been hailed as highly sensitive biomolecular sensors among organic electronic devices due to their superior stability in an aqueous environment and high transconductance.At the same time,plasmon based sensors are known to provide high sensitivity for biosensing due to the highly localized plasmonic field.Here we report a plasmonic OECT(POET)device that synchronizes the advantages of OECTs and plasmonic sensors on a single platform.The platform is fabricated by a simple,cost-effective,and high-throughput nanoimprinting process,which allows plasmonic resonance peak tuning to a given visible wavelength of interest for versatile biosensing.With glucose sensing as proof,a five-times sensitivity enhancement is obtained for POET compared to a regular(non-plasmonic)OECT.Thus,the POET paves the way to a new paradigm of optoelectronic sensors that combines the inherent high sensitivity of OECTs and localized plasmonic field to sense a vast realm of biomolecules.
基金financially supported by the National Natural Science Foundation of China(Nos.21908079,21872145 and U21A20326)Jiangsu Specially-Appointed Professor Fund(No.1046010241211400)+4 种基金Natural Science Foundation of Jiangsu Province(Nos.BK20211239,BK20221541 and BK20201345)the State Key Laboratory of Fine ChemicalsDalian University of Technology(No.KF2005)Dalian Institute of Chemical Physics(No.DICP 1201943)the Central Laboratory,School of Chemical and Material Engineering,Jiangnan University。
文摘Selective hydrogenation of biomass-derived maleic anhydride(MAH)to succinic anhydride(SA)is valuable but remains a challenge due to the complicated reaction network.We here report that single Pt atoms decorated onto the edges of two-dimensional(2D)1Tphase MoS_(2)(Pt1/1T-MOS_(2)SAC)as a proof-of-concept catalyst can efficiently convert biomass-derived MAH to SA with 100%conversion and 100%selectivity under mild conditions.The kinetic data and characterization results suggest that the catalytic performance of the edge-anchored Pt1/1T-MoS_(2)SAC originates from the facile H_(2)dissociation induced by the electron-deficient Pt1atoms and the pocket-like configuration of Pt1active site confines the adsorption configuration of MAH by the steric effect.The strategy of fabricating edge-confined catalysts offers a new direction to design novel SACs for biomass-derived transformations.
基金University of Central Florida(ER Award:#25089A06)We would also like to acknowledge the National Science Foundation(NSF)Major Research Instrumentation(MRI)Program(Grant ID:ECCS:1726636)for the XPS measurements presented in this manuscript+6 种基金MM acknowledges the University of Huddersfield(UoH)EPSRC-DTP competition 2018–19(EP/R513234/1)for funding SMVice Chancellor’s Scholarship Scheme for funding KMTAnalysis was performed on the Orion computing facility at the UoH.Calculations were run on the ARCHER and ARCHER2 UK National Supercomputing Services via our membership of the UK HEC Materials Chemistry Consortium(MCCEPSRC EP/L000202,EP/R029431)AA acknowledges NIH NCI(Grant R01CA045424),Research Excellence Fund(REF)Center for Biomedical Research for support.AA also acknowledges the National Science Foundation(NSF)instrumentation award(CHE-1920110)JA’s work was supported by the National Aeronautics and Space Administration[grant No.80NSSC21M0309]issued through the NASA Office of STEM Engagement.
文摘The disability,mortality and costs due to ionizing radiation(IR)-induced osteoporotic bone fractures are sub-stantial and no effective therapy exists.Ionizing radiation increases cellular oxidative damage,causing an imbalance in bone turnover that is primarily driven via heightened activity of the bone-resorbing osteoclast.We demonstrate that rats exposed to sublethal levels of IR develop fragile,osteoporotic bone.At reactive surface sites,cerium ions have the ability to easily undergo redox cycling:drastically adjusting their electronic con-figurations and versatile catalytic activities.These properties make cerium oxide nanomaterials fascinating.We show that an engineered artificial nanozyme composed of cerium oxide,and designed to possess a higher fraction of trivalent(Ce^(3+))surface sites,mitigates the IR-induced loss in bone area,bone architecture,and strength.These investigations also demonstrate that our nanozyme furnishes several mechanistic avenues of protection and selectively targets highly damaging reactive oxygen species,protecting the rats against IR-induced DNA damage,cellular senescence,and elevated osteoclastic activity in vitro and in vivo.Further,we reveal that our nanozyme is a previously unreported key regulator of osteoclast formation derived from macrophages while also directly targeting bone progenitor cells,favoring new bone formation despite its exposure to harmful levels of IR in vitro.These findings open a new approach for the specific prevention of IR-induced bone loss using synthesis-mediated designer multifunctional nanomaterials.
文摘Benchtop tissue cultures have become increasingly complex in recent years,as more on-a-chip biological technologies,such as microphysiological systems(MPS),are developed to incorporate cellular constructs that more accurately represent their respective biological systems.Such MPs have begun facilitating major breakthroughs in biological research and are poised to shape the field in the coming decades.These biological systems require integrated sensing modalities to procure complex,multiplexed datasets with unprecedented combinatorial biological detail.In this work,we expanded upon our polymer-metal biosensor approach by demonstrating a facile technology for compound biosensing that was characterized through custom modeling approaches.As reported herein,we developed a compound chip with 3D microelectrodes,3D microfluidics,interdigitated electrodes(IDEs)and a microheater.The chip was subsequently tested using the electrical/electrochemical characterization of 3D microelectrodes with 1 kHz impedance and phase recordings and IDE-based high-frequency(-1 MHz frequencies)impedimetric analysis of differential localized temperature recordings,both of which were modeled through equivalent electrical circuits for process parameter extraction.Additionally,a simplified antibody-conjugation strategy Was employed for a similar IDE-based analysis of the implications of a key analyte(L-glutamine)binding to the equivalent electrical circuit.Finally,acute microfluidic perfusion modeling was performed to demonstrate the ease of microfluidics integration into such a polymer-metal biosensor platform for potential complimentary localized chemical stimulation.Overall,our work demonstrates the design,development,and characterization of an accessibly designed polymer-metal compound biosensor for electrogenic cellular constructs to facilitate comprehensive MPS data collection.
基金supported by Citrus Disease Research and Extension(CDRE)(grant no.2016-70016-24828/project accusation no.1008984)from the USDA National Institute of Food and Agriculture
文摘Intensification of pollution loading worldwide has promoted an escalation of different types of disease-causing microorganisms, such as harmful algal blooms(HABs), instigating detrimental impacts on the quality of receiving surface waters. Formation of unwanted disinfection by-products(DBPs) resulting from conventional disinfection technologies reveals the need for the development of new sustainable alternatives. Quaternary Ammonium Compounds(QACs) are cationic surfactants widely known for their effective biocidal properties at the ppm level. In this study, a novel silica-based antimicrobial nanofilm was developed using a composite of silica-modified QAC(Fixed-Quat) and applied to a fiberglass mesh as an active surface via sol–gel technique. The synthesized Fixed-Quat nanocoating was found to be effective against E. coli with an inactivation rate of 1.3 × 10^(-3) log reduction/cm min. The Fixed-Quat coated fiberglass mesh also demonstrated successful control of Microcystis aeruginosa with more than 99% inactivation after 10 hr of exposure.The developed antimicrobial mesh was also evaluated with wild-type microalgal species collected in a water body experiencing HABs, obtaining a 97% removal efficiency. Overall,the silica-functionalized Fixed-Quat nanocoating showed promising antimicrobial properties for water disinfection and HABs control, while decreasing concerns related to DBPs formation and the possible release of toxic nanomaterials into the environment.
文摘Challenges in nanoscale characterization call for non-invasive, yet sensitive subsurface characterization of low-density materials such as polymers. In this work, we present new evidence that mode-synthesizing atomic force microscopy can be used to detect minute changes in low-density materials, such as those engendered in electro-sensitive polymers during electron beam lithography, surpassing all common nanoscale mechanical techniques. Moreover, we propose 3D reconstruction of the exposed polymer regions using successive high-resolution frames acquired at incremental depths inside the sample. In addition, the results clearly show the influence of increasing dwell time on the depth profile of the nano-sized exposed regions. Hence, the simple approach described here can be used for achieving sensitive nanoscale tomography of soft materials with promising applications in material sciences and biology.
文摘A number of mitigation techniques exist to reduce the emissions of pollutant gases and greenhouse gases(GHGs) from anaerobic storage of livestock manure. Nanoparticle(NP)application is a promising mitigating treatment option for pollutant gases, but limited research is available on the mode of NP application and their effectiveness in gaseous emission reduction. In this study, zinc silica nanogel(ZnSNL), copper silica nanogel(CuSNL), and N-acetyl cysteine(NACL) coated zinc oxide quantum dot(Qdot) NPs were compared to a control lacking NPs. All three NPs tested significantly reduced gas production and concentrations compared to non-treated manure. Overall, cumulative gas volumes were reduced by 92.73%–95.83%, and concentrations reduced by 48.98%–99.75% for H_2S, and 20.24%–99.82% for GHGs. Thus, application of NPs is a potential treatment option for mitigating pollutant and GHG emissions from anaerobically stored manure.
基金supported by the National Natural Science Foundation of China(No.21872020)1226 Engineering Health Major Project(Nos.BWS17J028 and AWS16J018)Fundamental Research Funds for the Central Universities(No.N180705004).
文摘Devising an electrocatalyst with brilliant efficiency and satisfactory durability for hydrogen production is of considerable demand,especially for large-scale application.Herein,we adopt a multi-step consequential induced strategy to construct a bifunctional electrocatalyst for the overall water splitting.Graphene oxide(GO)was used as a carbon matrix and in situ oxygen source,which was supported by the octahedral PtNi alloy to form the PtxNiy-GO precursor.When calcinating in Ar atmosphere,the oxygen in GO induced the surface segregation of Ni from the PtNi octahedron to form a core-shell structure of Ptx@Niy.Then,the surface-enriched Ni continuously induced the reformation of C in reduced graphene oxide(rGO)to enhance the degree of graphitization.This multi-step induction formed a nanocatalyst Pt_(x)@Ni_(y)-rGO which has very high catalytic efficiency and stability.By optimizing the feeding ratio of PtNi(Pt:Ni=1:2),the electrolytic overall water splitting at 10 mA·cm^(-2) can be driven by an electrolytic voltage of as low as 1.485 V,and hydrogen evolution reaction(HER)only needs an overpotential of 37 mV in 1.0 M KOH aqueous solution.Additionally,the catalyst exhibited consistent existence form in both HER and oxygen evolution reaction(OER),which was verified by switching the anode and cathode of the cell in the electrolysis of water.This work provides a new idea for the synthesis and evaluation of the bifunctional catalysts for water splitting.
基金supported by the National Science Foundation(NSF)under grant noECCS-1509729the Northrop Grumman University Research Program。
文摘Functional surfaces that can control light across the electromagnetic spectrum are highly desirable.Plasmonic nanostructures can assume this role by exhibiting dimension-tunable resonances that span multiple electromagnetic regimes.However,changing these structural parameters often impacts the higher-order resonances and spectral features in lower-wavelength domains.In this study,we discuss a cavity-coupled plasmonic system with resonances that are tunable across the 3–5 or 8–14μm infrared bands while retaining near-invariant spectral properties in the visible domain.This result is accomplished by regime-dependent resonance mechanisms and their dependence on independent structural parameters.Through the identification and constraint of key parameters,we demonstrate multispectral data encoding,where images,viewable in the infrared spectral domain,appear as uniform areas of color in the visible domain—effectively hiding the information.Fabricated by large area nanoimprint lithography and compatible with flexible surfaces,the proposed system can produce multifunctional coatings for thermal management,camouflage,and anti-counterfeiting.