Epitaxially grown III-nitride alloys are tightly bonded materials with mixed covalent-ionic bonds.This tight bonding presents tremendous challenges in developing III-nitride membranes,even though semiconductor membran...Epitaxially grown III-nitride alloys are tightly bonded materials with mixed covalent-ionic bonds.This tight bonding presents tremendous challenges in developing III-nitride membranes,even though semiconductor membranes can provide numerous advantages by removing thick,inflexible,and costly substrates.Herein,cavities with various sizes were introduced by overgrowing target layers,such as undoped GaN and green LEDs,on nanoporous templates prepared by electrochemical etching of n-type GaN.The large primary interfacial toughness was effectively reduced according to the design of the cavity density,and the overgrown target layers were then conveniently exfoliated by engineering tensile-stressed Ni layers.The resulting III-nitride membranes maintained high crystal quality even after exfoliation due to the use of GaN-based nanoporous templates with the same lattice constant.The microcavity-assisted crack propagation process developed for the current III-nitride membranes forms a universal process for developing various kinds of large-scale and high-quality semiconductor membranes.展开更多
Carbonate rocks are extensively used in civil infrastructure and play a critical role in geoenergy geoengineering,either as hydrocarbon reservoirs or potential repositories for CO_(2)geological storage.Carbonate genes...Carbonate rocks are extensively used in civil infrastructure and play a critical role in geoenergy geoengineering,either as hydrocarbon reservoirs or potential repositories for CO_(2)geological storage.Carbonate genesis and diagenetic overprint determine the properties of carbonate rocks.This study combines recent data gathered from Madison Limestone and an extensive dataset compiled from published sources to analyze the hydraulic and mechanical properties of limestone carbonate rocks.Physical models and data analyses recognize the inherently granular genesis of carbonate rocks and explain the strong dependency of physical properties on porosity.The asymptotically-correct power model in terms of(1-Ф/Ф*)a is a good approximation to global trends of unconfined stiffness E and unconfined compressive strength UCS,cohesive intercept in Mohr-Coulomb failure envelopes,and the brittle-toductile transition stress.This power model is the analytical solution for the mechanical properties of percolating granular structures.We adopted a limiting granular porosityФ*=0.5 for all models,which was consistent with the loosest packing of monosize spheres.The fitted power model has exponent(α=2)in agreement with percolation theory and highlights the sensitivity of mechanical properties to porosity.Data and models confirm a porosity-independent ratio between unconfined stiffness and strength,and the ratio follows a log-normal distribution with mean(E/UCS)≈300.The high angle of internal shear strength measured for carbonate rocks reflects delayed contact failure with increased confinement,and it is not sensitive to porosity.Permeability spans more than six orders of magnitude.Grain size controls pore size and determines the reference permeability k^(*)at the limiting porosityФ*=0.5.For a given grain size from fine to coarse-grained dominant carbonates,permeability is very sensitive to changes in porosity,suggesting preferential changes in the internal pore network during compaction.展开更多
Electrocatalytic splitting of water by means of renewable energy as the electricity supply is one of the most promising methods for storing green renewable energy as hydrogen. Although two-thirds of the earth’s surfa...Electrocatalytic splitting of water by means of renewable energy as the electricity supply is one of the most promising methods for storing green renewable energy as hydrogen. Although two-thirds of the earth’s surface is covered with water, there is inadequacy of freshwater in most parts of the world. Hence, splitting seawater instead of freshwater could be a truly sustainable alternative. However, direct seawater splitting faces challenges because of the complex composition of seawater. The composition, and hence, the local chemistry of seawater may vary depending on its origin, and in most cases, tracking of the side reactions and standardizing and customizing the catalytic process will be an extra challenge. The corrosion of catalysts and competitive side reactions due to the presence of various inorganic and organic pollutants create challenges for developing stable electro-catalysts. Hence, seawater splitting generally involves a two-step process, i.e., purification of seawater using reverse osmosis and then subsequent fresh water splitting. However, this demands two separate chambers and larger space, and increases complexity of the reactor design. Recently, there have been efforts to directly split seawater without the reverse osmosis step. Herein, we represent the most recent innovative approaches to avoid the two-step process, and compare the potential application of membrane-assisted and membrane-less electrolyzers in direct seawater splitting(DSS). We particularly discuss the device engineering, and propose a novel electrolyzer design strategies for concentration gradient based membrane-less microfluidic electrolyzer.展开更多
Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons...Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).展开更多
Nickel-rich transition-metal oxides are widely regarded as promising cathode materials for high-energydensity lithium-ion batteries for emerging electric vehicles. However, achieving high energy density in Ni-rich cat...Nickel-rich transition-metal oxides are widely regarded as promising cathode materials for high-energydensity lithium-ion batteries for emerging electric vehicles. However, achieving high energy density in Ni-rich cathodes is accompanied by substantial safety and cycle-life obstacles. The major issues of Ni-rich cathodes at high working potentials are originated from the unstable cathode-electrolyte interface, while the underlying mechanism of parasitic reactions towards surface reconstructions of cathode materials is not well understood. In this work, we controlled the Li_(2)CO_(3) impurity content on LiNi_(0.83)Mn_(0.1)Co_(0.07)O_(2) cathodes using air, tank-air, and O_(2) synthesis environments. Home-built high-precision leakage current and on-line electrochemical mass spectroscopy experiments verify that Li_(2)CO_(3) impurity is a significant promoter of parasitic reactions on Ni-rich cathodes. The rate of parasitic reactions is strongly correlated to Li_(2)CO_(3) content and severe performance deterioration of Ni83 cathodes.The post-mortem characterizations via high-resolution transition electron microscope and X-ray photoelectron spectroscopy depth profiles reveal that parasitic reactions promote more Ni reduction and O deficiency and even rock-salt phase transformation at the surface of cathode materials. Our observation suggests that surface reconstructions have a strong affiliation to parasitic reactions that create chemically acidic environment to etch away the lattice oxygen and offer the electrical charge to reduce the valence state of transition metal. Thus, this study advances our understanding on surface reconstructions of Nirich cathodes and prepares us for searching for rational strategies.展开更多
In the last few decades,deep learning(DL)has afforded solutions to macroscopic problems in petroleum engineering,but mechanistic problems at the microscale have not benefited from it.Mechanism studies have been the st...In the last few decades,deep learning(DL)has afforded solutions to macroscopic problems in petroleum engineering,but mechanistic problems at the microscale have not benefited from it.Mechanism studies have been the strong demands for the emerging projects,such as the gas storage and hydrate production,and for some problems encountered in the storage process,which are common found as the chemical interaction between injected gas and mineral,and the formation of hydrate.Emerging advances in DL technology enable solving molecular dynamics(MD)with quantum accuracy.The conventional quantum chemical method is computational expensive,whereas the classical MD method cannot guarantee high accuracy because of its empirical force field parameters.With the help of the DL force field,precision at the quantum chemistry level can be achieved in MD.Moreover,the DL force field promotes the computational speed compared with first-principles calculations.In this review,the basic knowledge of the molecular force field and deep neural network(DNN)is first introduced.Then,three representative opensource packages relevant to the DL force field are introduced.As the most common components in the development of oil and gas reservoirs,water and methane are studied from the aspects of computational efficiency and chemical reaction respectively,providing the foundation of oil and gas researches.However,in the oil and gas problems,the complex molecular topo structures and various element types set a high challenge for the DL techniques in MD.Regarding the computational efficiency,it needs improvement via GPU and parallel accelerations to compete with classical MD.Even with such difficulties,the booming of this technique in the area of petroleum engineering can be predictable.展开更多
Editorial Photonics technology remains a driving force in today’s scientific landscape,marked by continuous innovation and crossdisciplinary relevance.In an enlighting conversation with Light:Science&Applications...Editorial Photonics technology remains a driving force in today’s scientific landscape,marked by continuous innovation and crossdisciplinary relevance.In an enlighting conversation with Light:Science&Applications,Prof.Kei May Lau,a pioneer in photonics research,shares her deep insights on the evolution of technologies of LEDs,lasers,challenges of hetero-epitaxy,and the future of micro-LEDs and quantum dot lasers.Recently honored as a member of the US National Academy of Engineering(NAE)for her significant contributions to photonics and electronics using III-V semiconductors on silicon,Prof.Lau stands out as the sole Hong Kong scholar inducted into the NAE this year,joining 114 new and 21 international members.In this exclusive Light People interview,Prof.Lau shares her journey as a pioneering woman in engineering,her commitment to mentorship and academia,and her perspective on advancing female representation in science.The summary provided is distilled from Prof.Lau’s thoughtful responses during the interview.For a deeper exploration of Prof.Lau’s experiences and advice,the full interview is available in the Supplementary material.展开更多
On 21 May 2021(UTC),an MW 7.4 earthquake jolted the east Bayan Har block in the Tibetan Plateau.The earthquake received widespread attention as it is the largest event in the Tibetan Plateau and its surroundings since...On 21 May 2021(UTC),an MW 7.4 earthquake jolted the east Bayan Har block in the Tibetan Plateau.The earthquake received widespread attention as it is the largest event in the Tibetan Plateau and its surroundings since the 2008 Wenchuan earthquake,and especially in proximity to the seismic gaps on the east Kunlun fault.Here we use satellite interferometric synthetic aperture radar data and subpixel offset observations along the range directions to characterize the coseismic deformation of the earthquake.Range offset displacements depict clear surface ruptures with a total length of~170 km involving two possible activated fault segments in the earthquake.Coseismic modeling results indicate that the earthquake was dominated by left-lateral strike-slip motions of up to 7 m within the top 12 km of the crust.The well-resolved slip variations are characterized by five major slip patches along strike and 64%of shallow slip deficit,suggesting a young seismogenic structure.Spatial-temporal changes of the postseismic deformation are mapped from early 6-day and 24-day InSAR observations,and are well explained by time-dependent afterslip models.Analysis of Global Navigation Satellite System(GNSS)velocity profiles and strain rates suggests that the eastward extrusion of plateau is diffusely distributed across the east Bayan Har block,but exhibits significant lateral heterogeneities,as evidenced by magnetotelluric observations.The block-wide distributed deformation of the east Bayan Har block along with the significant co-and post-seismic stress loadings from the Madoi earthquake imply high seismic risks along regional faults,especially the Tuosuo Lake and Maqên-Maqu segments of the Kunlun fault that are known as seismic gaps.展开更多
Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinc...Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.展开更多
Direct photon to chemical energy conversion using semiconductor–electrocatalyst–electrolyte interfaces has been extensively investigated for more than a half century. Many studies have focused on screening materials...Direct photon to chemical energy conversion using semiconductor–electrocatalyst–electrolyte interfaces has been extensively investigated for more than a half century. Many studies have focused on screening materials for efficient photocatalysis. Photocatalytic efficiency has been improved during this period but is not sufficient for industrial commercialization. Detailed elucidation on the photocatalytic water splitting process leads to consecutive six reaction steps with the fundamental parameters involved: The photocatalysis is initiated involving photophysics derived from various semiconductor properties(1: photon absorption, 2: exciton separation). The generated charge carriers need to be transferred to surfaces effectively utilizing the interfaces(3: carrier diffusion, 4: carrier transport). Consequently, electrocatalysis finishes the process by producing products on the surface(5: catalytic efficiency, 6: mass transfer of reactants and products). Successful photocatalytic water splitting requires the enhancement of efficiency at each stage. Most critically, a fundamental understanding of the interfacial phenomena is highly desired for establishing 'photocatalysis by design' concepts, where the kinetic bottleneck within a process is identified by further improving the specific properties of photocatalytic materials as opposed to blind material screening. Theoretical modeling using the identified quantitative parameters can effectively predict the theoretically attainable photon-conversion yields. This article provides an overview of the state-of-the-art theoretical understanding of interfacial problems mainly developed in our laboratory.Photocatalytic water splitting(especially hydrogen evolution on metal surfaces) was selected as a topic,and the photophysical and electrochemical processes that occur at semiconductor–metal, semiconductor–electrolyte and metal–electrolyte interfaces are discussed.展开更多
We present a systematic computational study based on the density functional theory(DFT) aiming to high light the possible effects of one As doping atom on the structural, energetic, and electronic properties of differ...We present a systematic computational study based on the density functional theory(DFT) aiming to high light the possible effects of one As doping atom on the structural, energetic, and electronic properties of different isomers of Ge_(n+1) clusters with n = 1–20 atoms. By considering a large number of structures for each cluster size, the lowest-energy isomers are determined. The lowest-energy isomers reveal three-dimensional structures starting from n = 5. Their relative stability versus atomic size is examined based on the calculated binding energy, fragmentation energy, and second-order difference of energy. Doping Ge_(n+1) clusters with one As atom does not improve their stability. The electronic properties as a function of the atomic size are also discussed from the calculated HOMO–LUMO energy gap, vertical ionization potential, vertical electron affinity, and chemical hardness. The obtained results are significantly affected by the inclusion of one As atom into a Gen cluster.展开更多
Precise control over the charge carrier dynamics throughout the device can result in outstanding performance of perovskite solar cells(PSCs).Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)is the mo...Precise control over the charge carrier dynamics throughout the device can result in outstanding performance of perovskite solar cells(PSCs).Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)is the most actively studied hole transport material in p-i-n structured PSCs.However,charge transport in the PEDOT:PSS is limited and inefficient because of its low conductivity with the presence of the weak ionic conductor PSS.In addition,morphology of the underlying PEDOT:PSS layer in PSCs plays a crucial role in determining the optoelectronic quality of the active perovskite absorber layer.This work is focused on realization of a non-wetting conductive surface of hole transport layer suitable for the growth of larger perovskite crystalline domains.This is accomplished by employing a facile solventengineered(ethylene glycol and methanol)approach resulting in removal of the predominant PSS in PEDOT:PSS.The consequence of acquiring larger perovskite crystalline domains was observed in the charge carrier dynamics studies,with the achievement of higher charge carrier lifetime,lower charge transport time and lower transfer impedance in the solvent-engineered PEDOT:PSS-based PSCs.Use of this solventengineered treatment for the fabrication of MAPbI3 PSCs greatly increased the device stability witnessing a power conversion efficiency of 18.18%,which corresponds to^37%improvement compared to the untreated PEDOT:PSS based devices.展开更多
Carbon is the central element driving the evolution of our human society towards prosperity over several historical stages.As for now,we are in a stage of blossoming sciences and technologies related to carbon materia...Carbon is the central element driving the evolution of our human society towards prosperity over several historical stages.As for now,we are in a stage of blossoming sciences and technologies related to carbon materials,as a result of which our evergrowing energy demand has been largely satisfied.Yet,the expected rise of carbon energy consumption and the emerging environmental concerns have prevented us from being optimistic.To build a sufficiently powered future,we have been revolutionizing our ways of carbon energy utilization by discovering and designing new carbon structures,exploring and enhancing their unique physicochemical properties,and pursuing environmentally friendly strategies.Emerging structures such as graphene and sp-bonded C18 have allowed us to discover carbon’s promising properties such as energy storage and superconductivity,while green energy solutions such as fuel cells and CO2 reduction are working synergistically to purify the ecospheric carbon cycle.Therefore,this essay timely discusses related carbon sciences and technologies that have been the milestones shaping our energy consumption,based on which our energy future can be envisioned to be green and prosperous.展开更多
Progress in the design and fabrication of ultraviolet and deep-ultraviolet groupⅢ–nitride optoelectronic devices,based on aluminum gallium nitride and boron nitride and their alloys,and the heterogeneous integration...Progress in the design and fabrication of ultraviolet and deep-ultraviolet groupⅢ–nitride optoelectronic devices,based on aluminum gallium nitride and boron nitride and their alloys,and the heterogeneous integration with two-dimensional and oxide-based materials is reviewed.We emphasize wide-bandgap nitride compound semiconductors(i.e.,(B,Al,Ga)N)as the deep-ultraviolet materials of interest,and two-dimensional materials,namely graphene,two-dimensional boron nitride,and two-dimensional transition metal dichalcogenides,along with gallium oxide,as the hybrid integrated materials.We examine their crystallographic properties and elaborate on the challenges that hinder the realization of efficient and reliable ultraviolet and deep-ultraviolet devices.In this article we provide an overview of aluminum nitride,sapphire,and gallium oxide as platforms for deep-ultraviolet optoelectronic devices,in which we criticize the status of sapphire as a platform for efficient deep-ultraviolet devices and detail advancements in device growth and fabrication on aluminum nitride and gallium oxide substrates.A critical review of the current status of deep-ultraviolet light emission and detection materials and devices is provided.展开更多
Classical continuum mechanics which leads to a local continuum model,encounters challenges when the discontinuity appears,while peridynamics that falls into the category of nonlocal continuum mechanics suffers from a ...Classical continuum mechanics which leads to a local continuum model,encounters challenges when the discontinuity appears,while peridynamics that falls into the category of nonlocal continuum mechanics suffers from a high computational cost.A hybrid model coupling classical continuum mechanics with peridynamics can avoid both disadvantages.This paper describes the hybrid model and its adaptive coupling approach which dynamically updates the coupling domains according to crack propagations for brittle materials.Then this hybrid local/nonlocal continuum model is applied to fracture simulation.Some numerical examples like a plate with a hole,Brazilian disk,notched plate and beam,are performed for verification and validation.In addition,a peridynamic software is introduced,which was recently developed for the simulation of the hybrid local/nonlocal continuum model.展开更多
An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to reg...An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to regulate the p H of the solution and slow down the release of OH^-, effectively regulating the phase, nanostructure, interlayer spacing, surface area, thickness, and the performance of binary Ni –Co hydroxide. The ion-slow-release mechanism is conducive to the formation of α-phase with larger interlayer spacing and thinner flakes rather than β-phase. Attributed to the enlarged interlayer spacing, thinner nanosheets, and more exposed active sites, the resultant α-phase hydroxides(NCNS-5.2), displayed much lower over potential of 285 mV with respect to the dense-stacked β-phase hydroxides(362 mV) for OER at 10 mA/cm^2. It also exhibited high specific capacitance of 1474.2 F/g, when tested at 0.5 A/g within a voltage range of 0–0.45 Vvs. Hg/Hg O. This composite was also stable for water oxidation reaction and supercapacitor. The proof-of-concept of using controlled-release agent may provide suggestive insights for the material innovation and a variety of applications.展开更多
A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyt...A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert.The electrolyte comprises primarily ZnCl_(2) and LiCl as an additive,both of which are inexpensive salts.The O-H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn-Cl superhalides,as suggested by integrated characterization and simulation.As a result,the average Coulombic efficiency of zincmetal anode is raised to an unprecedented>99.7%at 1mA cm^(−2).In the new electrolyte,the plating/stripping processes leave the zinc-metal anode dendrite-free,and the zinc-metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm^(−2) at 2mA cm^(−2).Furthermore,the high Coulombic efficiency of zinc-metal anode in the ZnCl_(2)-LiCl mixture electrolyte is demonstrated in full cells with a limited anode.The V_(2)O_(5)·H_(2)O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles,and the LiMn_(2)O_(4)||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.展开更多
Porous carbon has been applied for lithium-sulfur battery cathodes,and carbonized metal-organic framework(MOF)is advantageous in tuning the morphology.Herein,we have systematically synthesized water-distorted MOF(WDM)...Porous carbon has been applied for lithium-sulfur battery cathodes,and carbonized metal-organic framework(MOF)is advantageous in tuning the morphology.Herein,we have systematically synthesized water-distorted MOF(WDM)derived porous carbon via controlling the proportion of both water in a mixed solvent(dimethylformamide and water)and ligand in MOF-5 precursors(metal and ligand),which is categorized by its morphology(i.e.Cracked stone(closed),Tassel(open)and Intermediate(semi-open)).For example,decrease in water and increase in ligand content induce Cracked stone WDMs which showed the highest specific surface area(2742-2990 m^(2)/g)and pore volume(2.81-3.28 cm^(3)/g)after carbonization.Morphological effect of carbonized WDMs(CWDMs)on battery performance was examined by introducing electrolytes with different sulfur reduction mechanisms(i.e.DOL/DME and ACN_(2) LiTFSITTE):Closed framework effectively confines polysulfide,whereas open framework enhances electrolyte accessibility.The initial capacities of the batteries were in the following order:Cracked stone>Intermediate>Tassel for DOL/DME and Intermediate>Tassel>Cracked stone for ACN_(2) LiTFSI-TTE.To note,Intermediate CWDM exhibited the highest initial capacity and retained capacity after 100 cycles(1398 and 747 mAh/g)in ACN_(2) LiTFSI-TTE electrolyte having advantages from both open and closed frameworks.In sum,we could correlate cathode morphology(openness and pore structure)and electrolyte type(i.e.polysulfide solubility)with lithium-sulfur battery performance.展开更多
Recently,there has been renewed interest in interface engineering as a means to further push the performance of perovskite solar cells closer to the Schockly-Queisser limit.Herein,for the first time we employ a multi-...Recently,there has been renewed interest in interface engineering as a means to further push the performance of perovskite solar cells closer to the Schockly-Queisser limit.Herein,for the first time we employ a multi-functional 4-chlorobenzoic acid to produce a self-assembled monolayer on a perovskite surface.With this interlayer we observe passivation of perovskite surface defects and a significant suppression of non-radiative charge recombination.Furthermore,at the surface of the interlayer we observe,charge dipoles which tune the energy level alignment,enabling a larger energetic driving force for hole extraction.The perovskite surface becomes more hydrophilic due to the presence of the interlayer.Consequently,we observe an improvement in open-circuit voltage from 1.08 to 1.16 V,a power conversion efficiency improvement from 18%to 21%and an improved stability under ambient conditions.Our work highlights the potential of SAMs to engineer the photo-electronic properties and stability of perovskite interfaces to achieve high-performance light harvesting devices.展开更多
Phosphogypsum (PG) is a by-product of the chemical reaction called the "wet process" whereby sul-phuric acid reacts with phosphate rock (PR) to produce phosphoric acid, needed for fertilizer production. Thro...Phosphogypsum (PG) is a by-product of the chemical reaction called the "wet process" whereby sul-phuric acid reacts with phosphate rock (PR) to produce phosphoric acid, needed for fertilizer production. Through the wet process, some impurities naturally present in the PR become incorporated in PG, including U decay-series radionuclides, are the main important concern which could have an effect on the surrounding environment and pre-vent its safe utilization. In order to determine the distribution and bioavailability of radionuclides to the surrounding environment, we used a sequential leaching of PG samples from Aqaba and Eshidiya fertilizer industry. The results showed that the percentages of 226Ra and 210Pb in PG are over those in the corresponding phosphate rocks (PG/PR), where 85% of the 226Ra and 85% of the 210Pb fractionate to PG. The sequential extraction results exhibited that most of 226Ra and 210Pb are bound in the residual phase (non-CaSO4) fraction ranging from 45%-65% and 55%-75%, respectively, whereas only 10%-15% and 10%-20% respectively of these radionuclides are distributed in the most labile fraction. The results obtained from this study showed that radionuclides are not incorporated with gypsum itself and may not form a threat to the surrounding environment.展开更多
基金The work was supported by King Abdullah University of Science and Technology(KAUST)baseline funding BAS/1/1614-01-01 and King Abdulaziz City for Science and Technology(Grant No.KACST TIC R2-FP-008)This work was also supported by Korea Photonics Technology Institute(Project No.193300029).
文摘Epitaxially grown III-nitride alloys are tightly bonded materials with mixed covalent-ionic bonds.This tight bonding presents tremendous challenges in developing III-nitride membranes,even though semiconductor membranes can provide numerous advantages by removing thick,inflexible,and costly substrates.Herein,cavities with various sizes were introduced by overgrowing target layers,such as undoped GaN and green LEDs,on nanoporous templates prepared by electrochemical etching of n-type GaN.The large primary interfacial toughness was effectively reduced according to the design of the cavity density,and the overgrown target layers were then conveniently exfoliated by engineering tensile-stressed Ni layers.The resulting III-nitride membranes maintained high crystal quality even after exfoliation due to the use of GaN-based nanoporous templates with the same lattice constant.The microcavity-assisted crack propagation process developed for the current III-nitride membranes forms a universal process for developing various kinds of large-scale and high-quality semiconductor membranes.
基金This research was supported by the KAUST Endowment at King Abdullah University of Science and Technology,Saudi Arabia.We thank Gabrielle.E.Abelskamp in Energy GeoEngineering Laboratory at King Abdullah University of Science and Technology for editing the manuscript.
文摘Carbonate rocks are extensively used in civil infrastructure and play a critical role in geoenergy geoengineering,either as hydrocarbon reservoirs or potential repositories for CO_(2)geological storage.Carbonate genesis and diagenetic overprint determine the properties of carbonate rocks.This study combines recent data gathered from Madison Limestone and an extensive dataset compiled from published sources to analyze the hydraulic and mechanical properties of limestone carbonate rocks.Physical models and data analyses recognize the inherently granular genesis of carbonate rocks and explain the strong dependency of physical properties on porosity.The asymptotically-correct power model in terms of(1-Ф/Ф*)a is a good approximation to global trends of unconfined stiffness E and unconfined compressive strength UCS,cohesive intercept in Mohr-Coulomb failure envelopes,and the brittle-toductile transition stress.This power model is the analytical solution for the mechanical properties of percolating granular structures.We adopted a limiting granular porosityФ*=0.5 for all models,which was consistent with the loosest packing of monosize spheres.The fitted power model has exponent(α=2)in agreement with percolation theory and highlights the sensitivity of mechanical properties to porosity.Data and models confirm a porosity-independent ratio between unconfined stiffness and strength,and the ratio follows a log-normal distribution with mean(E/UCS)≈300.The high angle of internal shear strength measured for carbonate rocks reflects delayed contact failure with increased confinement,and it is not sensitive to porosity.Permeability spans more than six orders of magnitude.Grain size controls pore size and determines the reference permeability k^(*)at the limiting porosityФ*=0.5.For a given grain size from fine to coarse-grained dominant carbonates,permeability is very sensitive to changes in porosity,suggesting preferential changes in the internal pore network during compaction.
基金King Abdullah University of Science and Technology for funding through the funding grant (BAS/1/1413-01-01)the Engineering and Physical Sciences Research Council (EPSRC,EP/V027433/1)+1 种基金the Royal Society (RGSR1211080IESR2212115)。
文摘Electrocatalytic splitting of water by means of renewable energy as the electricity supply is one of the most promising methods for storing green renewable energy as hydrogen. Although two-thirds of the earth’s surface is covered with water, there is inadequacy of freshwater in most parts of the world. Hence, splitting seawater instead of freshwater could be a truly sustainable alternative. However, direct seawater splitting faces challenges because of the complex composition of seawater. The composition, and hence, the local chemistry of seawater may vary depending on its origin, and in most cases, tracking of the side reactions and standardizing and customizing the catalytic process will be an extra challenge. The corrosion of catalysts and competitive side reactions due to the presence of various inorganic and organic pollutants create challenges for developing stable electro-catalysts. Hence, seawater splitting generally involves a two-step process, i.e., purification of seawater using reverse osmosis and then subsequent fresh water splitting. However, this demands two separate chambers and larger space, and increases complexity of the reactor design. Recently, there have been efforts to directly split seawater without the reverse osmosis step. Herein, we represent the most recent innovative approaches to avoid the two-step process, and compare the potential application of membrane-assisted and membrane-less electrolyzers in direct seawater splitting(DSS). We particularly discuss the device engineering, and propose a novel electrolyzer design strategies for concentration gradient based membrane-less microfluidic electrolyzer.
基金the financial support from the National Natural Science Foundation of China(22108044,22208061)the Research and Development Program in Key Fields of Guangdong Province(2020B1111380002)+1 种基金the Basic Research and Applicable Basic Research in Guangzhou City(202201010290)the financial support from the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery(2021GDKLPRB07)。
文摘Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).
基金supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Officesupported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office, under Contract No. DE-SC0012704+1 种基金supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357supported by the Vehicle Technologies Office of the U.S. Department of Energy。
文摘Nickel-rich transition-metal oxides are widely regarded as promising cathode materials for high-energydensity lithium-ion batteries for emerging electric vehicles. However, achieving high energy density in Ni-rich cathodes is accompanied by substantial safety and cycle-life obstacles. The major issues of Ni-rich cathodes at high working potentials are originated from the unstable cathode-electrolyte interface, while the underlying mechanism of parasitic reactions towards surface reconstructions of cathode materials is not well understood. In this work, we controlled the Li_(2)CO_(3) impurity content on LiNi_(0.83)Mn_(0.1)Co_(0.07)O_(2) cathodes using air, tank-air, and O_(2) synthesis environments. Home-built high-precision leakage current and on-line electrochemical mass spectroscopy experiments verify that Li_(2)CO_(3) impurity is a significant promoter of parasitic reactions on Ni-rich cathodes. The rate of parasitic reactions is strongly correlated to Li_(2)CO_(3) content and severe performance deterioration of Ni83 cathodes.The post-mortem characterizations via high-resolution transition electron microscope and X-ray photoelectron spectroscopy depth profiles reveal that parasitic reactions promote more Ni reduction and O deficiency and even rock-salt phase transformation at the surface of cathode materials. Our observation suggests that surface reconstructions have a strong affiliation to parasitic reactions that create chemically acidic environment to etch away the lattice oxygen and offer the electrical charge to reduce the valence state of transition metal. Thus, this study advances our understanding on surface reconstructions of Nirich cathodes and prepares us for searching for rational strategies.
基金We would like to express appreciation to the following financial support:National Natural Scientific Foundation of China(Grants No.51936001)King Abdullah University of Science and Technology(KAUST)through the grants BAS/1/1351-01,URF/1/4074-01,and URF/1/3769-01.
文摘In the last few decades,deep learning(DL)has afforded solutions to macroscopic problems in petroleum engineering,but mechanistic problems at the microscale have not benefited from it.Mechanism studies have been the strong demands for the emerging projects,such as the gas storage and hydrate production,and for some problems encountered in the storage process,which are common found as the chemical interaction between injected gas and mineral,and the formation of hydrate.Emerging advances in DL technology enable solving molecular dynamics(MD)with quantum accuracy.The conventional quantum chemical method is computational expensive,whereas the classical MD method cannot guarantee high accuracy because of its empirical force field parameters.With the help of the DL force field,precision at the quantum chemistry level can be achieved in MD.Moreover,the DL force field promotes the computational speed compared with first-principles calculations.In this review,the basic knowledge of the molecular force field and deep neural network(DNN)is first introduced.Then,three representative opensource packages relevant to the DL force field are introduced.As the most common components in the development of oil and gas reservoirs,water and methane are studied from the aspects of computational efficiency and chemical reaction respectively,providing the foundation of oil and gas researches.However,in the oil and gas problems,the complex molecular topo structures and various element types set a high challenge for the DL techniques in MD.Regarding the computational efficiency,it needs improvement via GPU and parallel accelerations to compete with classical MD.Even with such difficulties,the booming of this technique in the area of petroleum engineering can be predictable.
文摘Editorial Photonics technology remains a driving force in today’s scientific landscape,marked by continuous innovation and crossdisciplinary relevance.In an enlighting conversation with Light:Science&Applications,Prof.Kei May Lau,a pioneer in photonics research,shares her deep insights on the evolution of technologies of LEDs,lasers,challenges of hetero-epitaxy,and the future of micro-LEDs and quantum dot lasers.Recently honored as a member of the US National Academy of Engineering(NAE)for her significant contributions to photonics and electronics using III-V semiconductors on silicon,Prof.Lau stands out as the sole Hong Kong scholar inducted into the NAE this year,joining 114 new and 21 international members.In this exclusive Light People interview,Prof.Lau shares her journey as a pioneering woman in engineering,her commitment to mentorship and academia,and her perspective on advancing female representation in science.The summary provided is distilled from Prof.Lau’s thoughtful responses during the interview.For a deeper exploration of Prof.Lau’s experiences and advice,the full interview is available in the Supplementary material.
基金supported by the Natural Science Foundation of Jiangsu Province(Grant No.SBK2020043202)by Key Laboratory of Geospace Environment and Geodesy,Ministry of Education,Wuhan University(No.19-01-08).
文摘On 21 May 2021(UTC),an MW 7.4 earthquake jolted the east Bayan Har block in the Tibetan Plateau.The earthquake received widespread attention as it is the largest event in the Tibetan Plateau and its surroundings since the 2008 Wenchuan earthquake,and especially in proximity to the seismic gaps on the east Kunlun fault.Here we use satellite interferometric synthetic aperture radar data and subpixel offset observations along the range directions to characterize the coseismic deformation of the earthquake.Range offset displacements depict clear surface ruptures with a total length of~170 km involving two possible activated fault segments in the earthquake.Coseismic modeling results indicate that the earthquake was dominated by left-lateral strike-slip motions of up to 7 m within the top 12 km of the crust.The well-resolved slip variations are characterized by five major slip patches along strike and 64%of shallow slip deficit,suggesting a young seismogenic structure.Spatial-temporal changes of the postseismic deformation are mapped from early 6-day and 24-day InSAR observations,and are well explained by time-dependent afterslip models.Analysis of Global Navigation Satellite System(GNSS)velocity profiles and strain rates suggests that the eastward extrusion of plateau is diffusely distributed across the east Bayan Har block,but exhibits significant lateral heterogeneities,as evidenced by magnetotelluric observations.The block-wide distributed deformation of the east Bayan Har block along with the significant co-and post-seismic stress loadings from the Madoi earthquake imply high seismic risks along regional faults,especially the Tuosuo Lake and Maqên-Maqu segments of the Kunlun fault that are known as seismic gaps.
基金This work is supported by NSFC(21773242,21935010)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB20000000)+1 种基金National Key Research and Development Program of China(2018YFA0208600)King Abdullah University of Science and Technology.J.Dong acknowledges financial support from Youth Innovation Promotion Association of Chinese Academy of Sciences(2018017).
文摘Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.
基金supported by funding from King Abdullah University of Science and Technology(KAUST)
文摘Direct photon to chemical energy conversion using semiconductor–electrocatalyst–electrolyte interfaces has been extensively investigated for more than a half century. Many studies have focused on screening materials for efficient photocatalysis. Photocatalytic efficiency has been improved during this period but is not sufficient for industrial commercialization. Detailed elucidation on the photocatalytic water splitting process leads to consecutive six reaction steps with the fundamental parameters involved: The photocatalysis is initiated involving photophysics derived from various semiconductor properties(1: photon absorption, 2: exciton separation). The generated charge carriers need to be transferred to surfaces effectively utilizing the interfaces(3: carrier diffusion, 4: carrier transport). Consequently, electrocatalysis finishes the process by producing products on the surface(5: catalytic efficiency, 6: mass transfer of reactants and products). Successful photocatalytic water splitting requires the enhancement of efficiency at each stage. Most critically, a fundamental understanding of the interfacial phenomena is highly desired for establishing 'photocatalysis by design' concepts, where the kinetic bottleneck within a process is identified by further improving the specific properties of photocatalytic materials as opposed to blind material screening. Theoretical modeling using the identified quantitative parameters can effectively predict the theoretically attainable photon-conversion yields. This article provides an overview of the state-of-the-art theoretical understanding of interfacial problems mainly developed in our laboratory.Photocatalytic water splitting(especially hydrogen evolution on metal surfaces) was selected as a topic,and the photophysical and electrochemical processes that occur at semiconductor–metal, semiconductor–electrolyte and metal–electrolyte interfaces are discussed.
文摘We present a systematic computational study based on the density functional theory(DFT) aiming to high light the possible effects of one As doping atom on the structural, energetic, and electronic properties of different isomers of Ge_(n+1) clusters with n = 1–20 atoms. By considering a large number of structures for each cluster size, the lowest-energy isomers are determined. The lowest-energy isomers reveal three-dimensional structures starting from n = 5. Their relative stability versus atomic size is examined based on the calculated binding energy, fragmentation energy, and second-order difference of energy. Doping Ge_(n+1) clusters with one As atom does not improve their stability. The electronic properties as a function of the atomic size are also discussed from the calculated HOMO–LUMO energy gap, vertical ionization potential, vertical electron affinity, and chemical hardness. The obtained results are significantly affected by the inclusion of one As atom into a Gen cluster.
基金supported by NSF MRI (1428992)NASA EPSCoR (NNX15AM83A)+3 种基金U.S.–Egypt Science and Technology (S&T) Joint FundSDBoR R&D ProgramEDA University Center Program (ED18DEN3030025)supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC0206CH11357.
文摘Precise control over the charge carrier dynamics throughout the device can result in outstanding performance of perovskite solar cells(PSCs).Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)is the most actively studied hole transport material in p-i-n structured PSCs.However,charge transport in the PEDOT:PSS is limited and inefficient because of its low conductivity with the presence of the weak ionic conductor PSS.In addition,morphology of the underlying PEDOT:PSS layer in PSCs plays a crucial role in determining the optoelectronic quality of the active perovskite absorber layer.This work is focused on realization of a non-wetting conductive surface of hole transport layer suitable for the growth of larger perovskite crystalline domains.This is accomplished by employing a facile solventengineered(ethylene glycol and methanol)approach resulting in removal of the predominant PSS in PEDOT:PSS.The consequence of acquiring larger perovskite crystalline domains was observed in the charge carrier dynamics studies,with the achievement of higher charge carrier lifetime,lower charge transport time and lower transfer impedance in the solvent-engineered PEDOT:PSS-based PSCs.Use of this solventengineered treatment for the fabrication of MAPbI3 PSCs greatly increased the device stability witnessing a power conversion efficiency of 18.18%,which corresponds to^37%improvement compared to the untreated PEDOT:PSS based devices.
基金DOE Office of Energy Efficiency and Renewable Energy,Vehicle Technologies OfficeDOE Office of Science by UChicago Argonne,Grant/Award Number:DE‐AC02‐06CH11357。
文摘Carbon is the central element driving the evolution of our human society towards prosperity over several historical stages.As for now,we are in a stage of blossoming sciences and technologies related to carbon materials,as a result of which our evergrowing energy demand has been largely satisfied.Yet,the expected rise of carbon energy consumption and the emerging environmental concerns have prevented us from being optimistic.To build a sufficiently powered future,we have been revolutionizing our ways of carbon energy utilization by discovering and designing new carbon structures,exploring and enhancing their unique physicochemical properties,and pursuing environmentally friendly strategies.Emerging structures such as graphene and sp-bonded C18 have allowed us to discover carbon’s promising properties such as energy storage and superconductivity,while green energy solutions such as fuel cells and CO2 reduction are working synergistically to purify the ecospheric carbon cycle.Therefore,this essay timely discusses related carbon sciences and technologies that have been the milestones shaping our energy consumption,based on which our energy future can be envisioned to be green and prosperous.
基金financial support from the King Abdulaziz City for Science and Technology (KACST) under grant no. KACST TIC R2-FP-008partially supported by the King Abdullah University of Science and Technology (KAUST) baseline funding no. BAS/1/1614-01-01MBE equipment funding no. C/M-20000-12-001-77 and KCR/1/4055-01-01
文摘Progress in the design and fabrication of ultraviolet and deep-ultraviolet groupⅢ–nitride optoelectronic devices,based on aluminum gallium nitride and boron nitride and their alloys,and the heterogeneous integration with two-dimensional and oxide-based materials is reviewed.We emphasize wide-bandgap nitride compound semiconductors(i.e.,(B,Al,Ga)N)as the deep-ultraviolet materials of interest,and two-dimensional materials,namely graphene,two-dimensional boron nitride,and two-dimensional transition metal dichalcogenides,along with gallium oxide,as the hybrid integrated materials.We examine their crystallographic properties and elaborate on the challenges that hinder the realization of efficient and reliable ultraviolet and deep-ultraviolet devices.In this article we provide an overview of aluminum nitride,sapphire,and gallium oxide as platforms for deep-ultraviolet optoelectronic devices,in which we criticize the status of sapphire as a platform for efficient deep-ultraviolet devices and detail advancements in device growth and fabrication on aluminum nitride and gallium oxide substrates.A critical review of the current status of deep-ultraviolet light emission and detection materials and devices is provided.
基金The authors gratefully acknowledge the financial support received from KAUST baseline,the National Natural Science Foundation(11872016)the Fundamental Research Funds of Dalian University of Technology(Grant No.DUT17RC(3)092)for the completion of this work.
文摘Classical continuum mechanics which leads to a local continuum model,encounters challenges when the discontinuity appears,while peridynamics that falls into the category of nonlocal continuum mechanics suffers from a high computational cost.A hybrid model coupling classical continuum mechanics with peridynamics can avoid both disadvantages.This paper describes the hybrid model and its adaptive coupling approach which dynamically updates the coupling domains according to crack propagations for brittle materials.Then this hybrid local/nonlocal continuum model is applied to fracture simulation.Some numerical examples like a plate with a hole,Brazilian disk,notched plate and beam,are performed for verification and validation.In addition,a peridynamic software is introduced,which was recently developed for the simulation of the hybrid local/nonlocal continuum model.
基金supported by the National Natural Science Foundation of China(21476145)
文摘An OH^--slow-release strategy was established to controllably tune the( α-and β-) phase of nickel cobalt binary hydroxide in the presence of ammonium chloride. Ammonium chloride is added to the ionic solution to regulate the p H of the solution and slow down the release of OH^-, effectively regulating the phase, nanostructure, interlayer spacing, surface area, thickness, and the performance of binary Ni –Co hydroxide. The ion-slow-release mechanism is conducive to the formation of α-phase with larger interlayer spacing and thinner flakes rather than β-phase. Attributed to the enlarged interlayer spacing, thinner nanosheets, and more exposed active sites, the resultant α-phase hydroxides(NCNS-5.2), displayed much lower over potential of 285 mV with respect to the dense-stacked β-phase hydroxides(362 mV) for OER at 10 mA/cm^2. It also exhibited high specific capacitance of 1474.2 F/g, when tested at 0.5 A/g within a voltage range of 0–0.45 Vvs. Hg/Hg O. This composite was also stable for water oxidation reaction and supercapacitor. The proof-of-concept of using controlled-release agent may provide suggestive insights for the material innovation and a variety of applications.
基金XJ thanks Oregon State University for AID program support.J-XJ thanks the financial support from the National Natural Science Foundation of China(21574077 and 21304055)111 project(B14041)+3 种基金the Fundamental Research Funds for the Central Universities(GK201801001)CZ is supported by a fellowship from the China Scholarship Council(201706870033)CF is grateful to the U.S.National Science Foundation CAREER grant(CHE-1455353)the support of the femtosecond stimulated Raman instrumentation and the NSF MRI grant(DMR-1920368)for additional support.
文摘A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert.The electrolyte comprises primarily ZnCl_(2) and LiCl as an additive,both of which are inexpensive salts.The O-H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn-Cl superhalides,as suggested by integrated characterization and simulation.As a result,the average Coulombic efficiency of zincmetal anode is raised to an unprecedented>99.7%at 1mA cm^(−2).In the new electrolyte,the plating/stripping processes leave the zinc-metal anode dendrite-free,and the zinc-metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm^(−2) at 2mA cm^(−2).Furthermore,the high Coulombic efficiency of zinc-metal anode in the ZnCl_(2)-LiCl mixture electrolyte is demonstrated in full cells with a limited anode.The V_(2)O_(5)·H_(2)O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles,and the LiMn_(2)O_(4)||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea by the Korea government(MEST)(grant number NRF2019R1A2C4069922)the“LG Research Fund for New Faculty”by LG Chem。
文摘Porous carbon has been applied for lithium-sulfur battery cathodes,and carbonized metal-organic framework(MOF)is advantageous in tuning the morphology.Herein,we have systematically synthesized water-distorted MOF(WDM)derived porous carbon via controlling the proportion of both water in a mixed solvent(dimethylformamide and water)and ligand in MOF-5 precursors(metal and ligand),which is categorized by its morphology(i.e.Cracked stone(closed),Tassel(open)and Intermediate(semi-open)).For example,decrease in water and increase in ligand content induce Cracked stone WDMs which showed the highest specific surface area(2742-2990 m^(2)/g)and pore volume(2.81-3.28 cm^(3)/g)after carbonization.Morphological effect of carbonized WDMs(CWDMs)on battery performance was examined by introducing electrolytes with different sulfur reduction mechanisms(i.e.DOL/DME and ACN_(2) LiTFSITTE):Closed framework effectively confines polysulfide,whereas open framework enhances electrolyte accessibility.The initial capacities of the batteries were in the following order:Cracked stone>Intermediate>Tassel for DOL/DME and Intermediate>Tassel>Cracked stone for ACN_(2) LiTFSI-TTE.To note,Intermediate CWDM exhibited the highest initial capacity and retained capacity after 100 cycles(1398 and 747 mAh/g)in ACN_(2) LiTFSI-TTE electrolyte having advantages from both open and closed frameworks.In sum,we could correlate cathode morphology(openness and pore structure)and electrolyte type(i.e.polysulfide solubility)with lithium-sulfur battery performance.
基金supported by the National Natural Science Foundation of China(Grant Nos.52073115,61874048,12073009)the Project of Science and Technology Development Plan of Jilin Province(Grant No.20200201085JC).
文摘Recently,there has been renewed interest in interface engineering as a means to further push the performance of perovskite solar cells closer to the Schockly-Queisser limit.Herein,for the first time we employ a multi-functional 4-chlorobenzoic acid to produce a self-assembled monolayer on a perovskite surface.With this interlayer we observe passivation of perovskite surface defects and a significant suppression of non-radiative charge recombination.Furthermore,at the surface of the interlayer we observe,charge dipoles which tune the energy level alignment,enabling a larger energetic driving force for hole extraction.The perovskite surface becomes more hydrophilic due to the presence of the interlayer.Consequently,we observe an improvement in open-circuit voltage from 1.08 to 1.16 V,a power conversion efficiency improvement from 18%to 21%and an improved stability under ambient conditions.Our work highlights the potential of SAMs to engineer the photo-electronic properties and stability of perovskite interfaces to achieve high-performance light harvesting devices.
文摘Phosphogypsum (PG) is a by-product of the chemical reaction called the "wet process" whereby sul-phuric acid reacts with phosphate rock (PR) to produce phosphoric acid, needed for fertilizer production. Through the wet process, some impurities naturally present in the PR become incorporated in PG, including U decay-series radionuclides, are the main important concern which could have an effect on the surrounding environment and pre-vent its safe utilization. In order to determine the distribution and bioavailability of radionuclides to the surrounding environment, we used a sequential leaching of PG samples from Aqaba and Eshidiya fertilizer industry. The results showed that the percentages of 226Ra and 210Pb in PG are over those in the corresponding phosphate rocks (PG/PR), where 85% of the 226Ra and 85% of the 210Pb fractionate to PG. The sequential extraction results exhibited that most of 226Ra and 210Pb are bound in the residual phase (non-CaSO4) fraction ranging from 45%-65% and 55%-75%, respectively, whereas only 10%-15% and 10%-20% respectively of these radionuclides are distributed in the most labile fraction. The results obtained from this study showed that radionuclides are not incorporated with gypsum itself and may not form a threat to the surrounding environment.