Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization

Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.

Chalcogen heteroatoms doped nickel-nitrogen-carbon single-atom catalysts with asymmetric coordination for efficient electrochemical CO_(2) reduction

The electronic configuration of central metal atoms in single-atom catalysts(SACs)is pivotal in electrochemical CO_(2) reduction reaction(eCO_(2)RR).Herein,chalcogen heteroatoms(e.g.,S,Se,and Te)were incorporated into the symmetric nickel-nitrogen-carbon(Ni-N_(4)-C)configuration to obtain Ni-X-N_(3)-C(X:S,Se,and Te)SACs with asymmetric coordination presented for central Ni atoms.Among these obtained Ni-X-N_(3)-C(X:S,Se,and Te)SACs,Ni-Se-N_(3)-C exhibited superior eCO_(2)RR activity,with CO selectivity reaching~98% at-0.70 V versus reversible hydrogen electrode(RHE).The Zn-CO_(2) battery integrated with Ni-Se-N_(3)-C as cathode and Zn foil as anode achieved a peak power density of 1.82 mW cm^(-2) and maintained remarkable rechargeable stability over 20 h.In-situ spectral investigations and theoretical calculations demonstrated that the chalcogen heteroatoms doped into the Ni-N_(4)-C configuration would break coordination symmetry and trigger charge redistribution,and then regulate the intermediate behaviors and thermodynamic reaction pathways for eCO_(2)RR.Especially,for Ni-Se-N_(3)-C,the introduced Se atoms could significantly raise the d-band center of central Ni atoms and thus remarkably lower the energy barrier for the rate-determining step of ^(*)COOH formation,contributing to the promising eCO_(2)RR performance for high selectivity CO production by competing with hydrogen evolution reaction.

From Rejection to Embracement:The Catholic Perception of Spiritism in Brazil

The history of the relationship between Spiritism and Catholicism in Brazil can be traced through pivotal moments in the trajectory of the First Republic and the religious field since the 19th century,reflecting Brazil’s evolution into a modern,urban,and industrial society.Introduced to Brazil in the 1880s,Spiritism initially faced severe opposition from the Catholic Church,being dismissed as superstition and demon worship due to its engagement with death and spirits.Unlike Christianity,Spiritism denies the divinity of Jesus,the resurrection,and the sanctity of Church sacraments,viewing demons and angels merely as disembodied souls at different spiritual stages.Early perceptions were further complicated by the mixing of Spiritism with African and indigenous rites,which led critics to associate it with madness and mental health threats.However,the relationship between Catholicism and Spiritism in Brazil has evolved positively,particularly following the popularization of Spiritism by figures like Chico Xavier.Modern Brazilian society,characterized by increased education and religious syncretism,has grown more tolerant of diverse practices and beliefs,diminishing historical prejudices against Spiritists.This qualitative study,drawing on scholarly research and first-hand interviews,reveals that Spiritism's acceptance among Brazilian Catholics is due to its convergence with contemporary social values and the evolving profile of the average Catholic.Despite possessing a religion-like character,Spiritism is seen less as a distinct religion and more as a complementary set of practices and beliefs that enhance Catholic faith.This phenomenon mirrors the integration of Agama Hindu practices,reinforcing rather than undermining traditional religious identities.

Exploring the growth value equity valuation model with data visualization

The Growth Value Model(GVM)proposed theoretical closed form formulas consist-ing of Return on Equity(ROE)and the Price-to-Book value ratio(P/B)for fair stock prices and expected rates of return.Although regression analysis can be employed to verify these theoretical closed form formulas,they cannot be explored by classical quintile or decile sorting approaches with intuition due to the essence of multi-factors and dynamical processes.This article uses visualization techniques to help intuitively explore GVM.The discerning findings and contributions of this paper is that we put forward the concept of the smart frontier,which can be regarded as the reasonable lower limit of P/B at a specific ROE by exploring fair P/B with ROE-P/B 2D dynamical process visualization.The coefficients in the formula can be determined by the quantile regression analysis with market data.The moving paths of the ROE and P/B in the cur-rent quarter and the subsequent quarters show that the portfolios at the lower right of the curve approaches this curve and stagnates here after the portfolios are formed.Furthermore,exploring expected rates of return with ROE-P/B-Return 3D dynamical process visualization,the results show that the data outside of the lower right edge of the“smart frontier”has positive quarterly return rates not only in the t+1 quarter but also in the t+2 quarter.The farther away the data in the t quarter is from the“smart frontier”,the larger the return rates in the t+1 and t+2 quarter.

In operando-formed interface between silver and perovskite oxide for efficient electroreduction of carbon dioxide to carbon monoxide

Electrochemical carbon dioxide(CO_(2))reduction(ECR)is a promising technology to produce valuable fuels and feedstocks from CO_(2).Despite large efforts to develop ECR catalysts,the investigation of the catalytic performance and electrochemical behavior of complex metal oxides,especially perovskite oxides,is rarely reported.Here,the inorganic perovskite oxide Ag-doped(La_(0.8)Sr_(0.2))_(0.95)Ag_(0.05)MnO_(3-δ)(LSA0.05M)is reported as an efficient electrocatalyst for ECR to CO for the first time,which exhibits a Faradaic efficiency(FE)of 84.3%,a remarkable mass activity of 75Ag^(-1)(normalized to the mass of Ag),and stability of 130 h at a moderate overpotential of 0.79 V.The LSA0.05M catalyst experiences structure reconstruction during ECR,creating the in operando-formed interface between the perovskite and the evolved Ag phase.The evolved Ag is uniformly distributed with a small particle size on the perovskite surface.Theoretical calculations indicate the reconstruction of LSA0.05M during ECR and reveal that the perovskite-Ag interface provides adsorption sites for CO_(2) and accelerates the desorption of the*CO intermediate to enhance ECR.This study presents a novel high-performance perovskite catalyst for ECR andmay inspire the future design of electrocatalysts via the in operando formation of metal-metal oxide interfaces.

Word sense disambiguation using semantic relatedness measurement

All human languages have words that can mean different things in different contexts, such words with multiple meanings are potentially “ambiguous”. The process of “deciding which of several meanings of a term is intended in a given context” is known as “word sense disambiguation (WSD)”. This paper presents a method of WSD that assigns a target word the sense that is most related to the senses of its neighbor words. We explore the use of measures of relatedness between word senses based on a novel hybrid approach. First, we investigate how to “literally” and “regularly” express a “concept”. We apply set algebra to WordNet’s synsets cooperating with WordNet’s word ontology. In this way we establish regular rules for constructing various representations (lexical notations) of a concept using Boolean operators and word forms in various synset(s) defined in WordNet. Then we establish a formal mechanism for quantifying and estimating the semantic relatedness between concepts—we facilitate “concept distribution statistics” to determine the degree of semantic relatedness between two lexically expressed con- cepts. The experimental results showed good performance on Semcor, a subset of Brown corpus. We observe that measures of semantic relatedness are useful sources of information for WSD.

Activity origin and alkalinity effect of electrocatalytic biomass oxidation on nickel nitride

Electro-oxidation of 5-hydroxymethylfurfural(HMFOR)is a promising green approach to realize the conversion of biomass into value-added chemicals.However,considering the complexity of the molecular structure of HMF,an in-depth understanding of the electrocatalytic behavior of HMFOR has rarely been investigated.Herein,the electrocatalytic mechanism of HMFOR on nickel nitride(Ni3 N)is elucidated by operando X-ray absorption spectroscopy(XAS),in situ Raman,quasi in situ X-ray photoelectron spectroscopy(XPS),and operando electrochemical impedance spectroscopy(EIS),respectively.The activity origin is proved to be Ni^(2+δ)N(OH)ads generated by the adsorbed hydroxyl group.Moreover,HMFOR on Ni3 N relates to a two-step reaction:Initially,the applied potential drives Ni atoms to lose electrons and adsorb OH-after 1.35 VRHE,giving rise to Ni^(2+δ)N(OH)ads with the electrophilic oxygen;then Ni^(2+δ)N(OH)ads seizes protons and electrons from HMF and leaves as H_(2) O spontaneously.Furthermore,the high electrolyte alkalinity favors the HMFOR process due to the increased active species(Ni^(2+δ)N(OH)ads)and the enhanced adsorption of HMF on the Ni3 N surface.This work could provide an in-depth understanding of the electrocatalytic mechanism of HMFOR on Ni3 N and demonstrate the alkalinity effect of the electrolyte on the electrocatalytic performance of HMFOR.

Electron-Deficient Zn-N_(6) Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting

Despite of suitable band structures for harvesting solar light and driving water redox reactions,polymeric carbon nitride(PCN)has suffered from poor charge transfer ability and sluggish surface reaction kinetics,which limit its photocatalytic activity for water splitting.Herein,atomically dispersed Zn-coordinated three-dimensional(3D)sponge-like PCN(Zn-PCN)is synthesized through a novel intermediate coordination strategy.Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N_(6) configura-tion featured with an electron-deficient state.Such an electronic configuration has been demonstrated contributive to promoted electron excitation,accelerated charge separation and transfer as well as reduced water redox barriers.Further benefited from the abundant surface active sites derived from the 3D porous structure,Zn-PCN realizes visible-light photocatalysis for overall water splitting with H_(2) and O_(2) simultaneously evolved at a stoichiometric ratio of 2:1.This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.

Nonlinear pushover analysis of infilled concrete frames

Six reinforced concrete frames with or without masonry infills were constructed and tested under horizontal cyclic loads. All six frames had identical details in which the transverse reinforcement in columns was provided by rectangular hoops that did not meet current ACI specifications for ductile frames. For comparison purposes, the columns in three of these frames were jacketed by carbon-fiber-reinforced-polymer （CFRP） sheets to avoid possible shear failure. A nonlinear pushover analysis, in which the force-deformation relationships of individual elements were developed based on ACI 318, FEMA 356, and Chen＇s model, was carried out for these frames and compared to test results. Both the failure mechanisms and impact of infills on the behaviors of these frames were examined in the study. Conclusions from the present analysis provide structural engineers with valuable information for evaluation and design of infilled concrete frame building structures.

Promoting surface reconstruction of NiFe layered double hydroxides via intercalating[Cr(C_(2)O_(4))_(3)]^(3-)for enhanced oxygen evolution

Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.

AXIAL HEAT CONDUCTION MODEL TO PREDICT MAXIMUM HEAT REMOVE OF MINIATURE HEAT PIPE BASED ON GREY MODEL THEORY

Computer chip is always accompanied by the increase of heat dissipation and miniaturization. The miniature heat pipes are widely used in notebook computer to resolve the heat dissipation problems. Maximum heat removed model of miniature heat pipes building by grey model is presented. In order to know the foundation for modeling, the smooth grade of error examination is inquired and the accuracy of grey relational grade is verified. The model can be used to select a suitable heat pipes to solve electric heat problems in the future. Final results show that the grey model only needs four experiment data and its error value is less than 10%, further, it is better than computational fluid dynamics （CFD） model.

Hepatitis B virus persistent infection-related single nucleotide polymorphisms in HLA regions are associated with viral load in hepatoma families

BACKGROUND Genome-wide association studies from Asia indicate that HLA-DP and HLA-DQ loci are important in persistent hepatitis B virus(HBV)infections.One of the key elements for HBV-related carcinogenesis is persistent viral replication and inflammation.AIM To examine genetic and nongenetic factors with persistent HBV infection and viral load in families with hepatocellular carcinoma(HCC).METHODS The HCC families included 301 hepatitis B surface antigen(HBsAg)carriers and 424 noncarriers born before the nationwide vaccination program was initiated in 1984.Five HBV-related single nucleotide polymorphisms(SNPs)—rs477515,rs9272105,rs9276370,rs7756516,and rs9277535—were genotyped.Factors associated with persistent HBV infection and viral load were analyzed by a generalized estimating equation.RESULTS In the first-stage persistent HBV study,all SNPs except rs9272105 were associated with persistent infection.A significantly higher area under the reciprocal operating characteristic curve for nongenetic factors vs genetic factors(P<0.001)suggests that the former play a major role in persistent HBV infection.In the second-stage viral load study,we added 8 HBsAg carriers born after 1984.The 309 HBsAg carriers were divided into low(n=162)and high viral load(n=147)groups with an HBV DNA cutoff of 105 cps/mL.Sex,relationship to the index case,rs477515,rs9272105,and rs7756516 were associated with viral load.Based on the receiver operating characteristic curve analysis,genetic and nongenetic factors affected viral load equally in the HCC family cohort(P=0.3117).CONCLUSION In these east Asian adults,the mechanism of persistent HBV infection-related SNPs was a prolonged viral replication phase.

Controllable synthesis of Fe–N4 species for acidic oxygen reduction

Controllable design and synthesis of catalysts with the target active sites are extremely important for their applications such as for the oxygen reduction reaction(ORR)in fuel cells.However,the controllably synthesizing electrocatalysts with a single type of active site still remains a grand challenge.In this study,we developed a facile and scalable method for fabricating highly efficient ORR electrocatalysts with sole atomic Fe-N4 species as the active site.Herein,the use of cost-effective highly porous carbon as the support not only could avoid the aggregation of the atomic Fe species but also a feasible approach to reduce the catalyst cost.The obtained atomic Fe-N4 in activated carbon(aFe@AC)shows excellent ORR activity.Its half-wave potential is 59 mV more negative but 47 mV more positive than that of the commercial Pt/C in acidic and alkaline electrolytes,respectively.The full cell performance test results show that the aFe@AC sample is a promising candidate for direct methanol fuel cells.This study provides a general method to prepare catalysts with a certain type of active site and definite numbers.

Electrochemically formed PtFeNi alloy nanoparticles on defective NiFe LDHs with charge transfer for efficient water splitting

Efficient and stable bifunctional electrocatalysts for water splitting is essential for producing hydrogen and alleviating huge energy consumption.Meanwhile,charge transfer engineering is an efficient approach to modulate the localized electronic properties of catalysts and tune the electrocatalytic performance.Herein,we tactfully fabricate PtFeNi alloys/NiFe layered double hydroxides(LDHs)heterostructure by an easily electrochemical way with a small amount of Pt.The experimental and theoretical results unravel that the charge transfer on the alloy clusters modulated by the defective substrates(NiFe LDHs),which synergistically optimizes the adsorption energy of the reaction intermediates.The electrocatalyst exhibits an ultra‐low overpotential of 81 and 243 mV at the current density of 100 mA cm^(–2) for hydrogen evolution and oxygen evolution,respectively.Furthermore,the overall water splitting indicates that PtFeNi alloys/NiFe LDHs presents an ultra‐low overpotential of 265 and 406 mV to reach the current density of 10 and 300 mA cm^(–2),respectively.It proves that the PtFeNi alloys/NiFe LDHs catalyst is an excellent dual‐function electrocatalyst for water splitting and promising for industrialization.This work provides a new electrochemical approach to construct the alloy heterostructure.The prepared heterostructures act as an ideal platform to investigate the charge re‐distribution behavior and to improve the electrocatalytic activity.

Evaluation of the sustainable development level of countries along the Belt and Road and its impact factors:Empirical analysis based on the Super-efficiency slacks-based measure and Tobit measure models

Sustainable development is an important component of the Belt and Road Initiative(BRI)and is of great significance for evaluating the levels of sustainable development of countries along this route(henceforth,BRI countries).Therefore,this study aims to identify the factors that influence the levels of sustainable development of BRI countries in a reasonable and objective manner.Eventually,this study employs the super efficiency slacks-based measure(Super-SBM)model,which considers unexpected outputs to measure the level of sustainable development of BRI countries.The dynamic change and composition of the sustainable development level of these countries are calculated using the global Malmquist-Luenberger index.Furthermore,the Tobit model is used to identify the factors influencing the level of sustainable development of BRI countries in general and in various categories.The empirical results suggest the following points.(a)The overall level of sustainable development of BRI countries is low,whereas those of high-income and middle-and high-income countries are relatively high.(b)The overall sustainable development levels of BRI countries declined to a certain extent in 2008 owing to the effect of the financial crisis,.However,the sustainable development level of other countries,barring low-income countries,has gradually increased since 2011.(c)Since 2008,technological progress has replaced technical efficiency as the main driving force behind the improvement of the sustainable development level of BRI countries.(d)A U-shaped relationship is observed between the economic and sustainable development levels of these countries.(e)The level of science and technology and the proportion of renewable energy consumption can promote the sustainable development of these countries.Moreover,a negative correlation exists between the level of opening to the outside world and that of sustainable development of countries that mainly export resource-based products and are dominated by labor-intensive export industries.Barring low-income countries,the energy structure plays an effective role in improving the level of sustainable development.Finally,the study presents suggestions for China in the process of coping with the sustainable development of relevant countries during its promotion of the BRI.

Molten salt assisted fabrication of Fe@Fe_(SA)-N-C oxygen electrocatalyst for high performance Zn-air battery

Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.

The Study and Application of the IoT in Pet Systems

The interaction between human and physical devices and devices in the real world is gaining more attention, and requires a natural and intuitive methodology to employ. According to this idea and living well, life has been a growing demand. Thus, how to raise pets in an easy way has been the main issue recently. This study examines the ability of computation, communication, and control technologies to improve human interaction with pets by the technology of the Internet of Things. This work addresses the improvement through the pet application of the ability of location-awareness, and to help the pet owners raise their pet on the activity and eating control easily. Extensive experiment results demonstrate that our proposed system performs significantly help on the kidney disease and reduce the symptoms. Our study not only presents the key improvement of the pet monitor system involved in the ideas of the Internet of Things, but also meets the demands of pet owners, who are out for works without any trouble.

Stretching instability of intrinsically curved semiflexible biopolymers:A lattice model approach

We apply a Monte Carlo simulation method to lattice systems to study the effect of an intrinsic curvature on the mechanical property of a semiflexible biopolymer.We find that when the intrinsic curvature is sufficiently large,the extension of a semiflexible biopolymer can undergo a first-order transition at finite temperature.The critical force increases with increasing intrinsic curvature.However,the relationship between the critical force and the bending rigidity is structuredependent.In a triangle lattice system,when the intrinsic curvature is smaller than a critical value,the critical force increases with the increasing bending rigidity first,and then decreases with the increasing bending rigidity.In a square lattice system,however,the critical force always decreases with the increasing bending rigidity.In contrast,when the intrinsic curvature is greater than the critical value,the larger bending rigidity always results in a larger critical force in both lattice systems.

Watermarking Scheme Based on Wavelet Transformation and Visual Cryptography

Based on the principles of the visual cryptography and the law of large numbers, the unexpanded shares are generated during the processes of embedding and verifying the hidden watermark. The watermark embedding is done in the frequency domain, which can be decoded by the human visual system （HVS） without the necessity of any complicated computation and the help of the original image. Experimental results indicated that our method had a good robustness on darkening, lightening, blurring, sharpening, noise, distorting, jitter, joint photographic experts group （JPEG） compression, and crop attacks.

Localization and recurrence of a quantum walk in a periodic potential on a line

We present a numerical study of a model of quantum walk in a periodic potential on a line. We take the simple view that different potentials have different affects on the way in which the coin state of the walker is changed. For simplicity and definiteness, we assume that the walker＇s coin state is unaffected at sites without the potential, and rotated in an unbiased way according to the Hadamard matrix at sites with the potential. This is the simplest and most natural model of a quantum walk in a periodic potential with two coins. Six generic cases of such quantum walks are studied numerically. It is found that, of the six cases, four cases display significant localization effect where the walker is confined in the neighborhood of the origin for a sufficiently long time. Associated with such a localization effect is the recurrence of the probability of the walker returning to the neighborhood of the origin.