The presence of numerous uncertainties in hybrid decision information systems(HDISs)renders attribute reduction a formidable task.Currently available attribute reduction algorithms,including those based on Pawlak attr...The presence of numerous uncertainties in hybrid decision information systems(HDISs)renders attribute reduction a formidable task.Currently available attribute reduction algorithms,including those based on Pawlak attribute importance,Skowron discernibility matrix,and information entropy,struggle to effectively manages multiple uncertainties simultaneously in HDISs like the precise measurement of disparities between nominal attribute values,and attributes with fuzzy boundaries and abnormal values.In order to address the aforementioned issues,this paper delves into the study of attribute reduction withinHDISs.First of all,a novel metric based on the decision attribute is introduced to solve the problem of accurately measuring the differences between nominal attribute values.The newly introduced distance metric has been christened the supervised distance that can effectively quantify the differences between the nominal attribute values.Then,based on the newly developed metric,a novel fuzzy relationship is defined from the perspective of“feedback on parity of attribute values to attribute sets”.This new fuzzy relationship serves as a valuable tool in addressing the challenges posed by abnormal attribute values.Furthermore,leveraging the newly introduced fuzzy relationship,the fuzzy conditional information entropy is defined as a solution to the challenges posed by fuzzy attributes.It effectively quantifies the uncertainty associated with fuzzy attribute values,thereby providing a robust framework for handling fuzzy information in hybrid information systems.Finally,an algorithm for attribute reduction utilizing the fuzzy conditional information entropy is presented.The experimental results on 12 datasets show that the average reduction rate of our algorithm reaches 84.04%,and the classification accuracy is improved by 3.91%compared to the original dataset,and by an average of 11.25%compared to the other 9 state-of-the-art reduction algorithms.The comprehensive analysis of these research results clearly indicates that our algorithm is highly effective in managing the intricate uncertainties inherent in hybrid data.展开更多
Attribute reduction through the combined approach of Rough Sets(RS)and algebraic topology is an open research topic with significant potential for applications.Several research works have introduced a strong relations...Attribute reduction through the combined approach of Rough Sets(RS)and algebraic topology is an open research topic with significant potential for applications.Several research works have introduced a strong relationship between RS and topology spaces for the attribute reduction problem.However,the mentioned recent methods followed a strategy to construct a new measure for attribute selection.Meanwhile,the strategy for searching for the reduct is still to select each attribute and gradually add it to the reduct.Consequently,those methods tended to be inefficient for high-dimensional datasets.To overcome these challenges,we use the separability property of Hausdorff topology to quickly identify distinguishable attributes,this approach significantly reduces the time for the attribute filtering stage of the algorithm.In addition,we propose the concept of Hausdorff topological homomorphism to construct candidate reducts,this method significantly reduces the number of candidate reducts for the wrapper stage of the algorithm.These are the two main stages that have the most effect on reducing computing time for the attribute reduction of the proposed algorithm,which we call the Cluster Filter Wrapper algorithm based on Hausdorff Topology.Experimental validation on the UCI Machine Learning Repository Data shows that the proposed method achieves efficiency in both the execution time and the size of the reduct.展开更多
Attribute reduction is a research hotspot in rough set theory. Traditional heuristic attribute reduction methods add the most important attribute to the decision attribute set each time, resulting in multiple redundan...Attribute reduction is a research hotspot in rough set theory. Traditional heuristic attribute reduction methods add the most important attribute to the decision attribute set each time, resulting in multiple redundant attribute calculations, high time consumption, and low reduction efficiency. In this paper, based on the idea of sequential three-branch decision classification domain, attributes are treated as objects of three-branch division, and attributes are divided into core attributes, relatively necessary attributes, and unnecessary attributes using attribute importance and thresholds. Core attributes are added to the decision attribute set, unnecessary attributes are rejected from being added, and relatively necessary attributes are repeatedly divided until the reduction result is obtained. Experiments were conducted on 8 groups of UCI datasets, and the results show that, compared to traditional reduction methods, the method proposed in this paper can effectively reduce time consumption while ensuring classification performance.展开更多
For neighborhood rough set attribute reduction algorithms based on dependency degree,a neighborhood computation method incorporating attribute weight values and a neighborhood rough set attribute reduction algorithm u...For neighborhood rough set attribute reduction algorithms based on dependency degree,a neighborhood computation method incorporating attribute weight values and a neighborhood rough set attribute reduction algorithm using discernment as the heuristic information was proposed.The reduction algorithm comprehensively considers the dependency degree and neighborhood granulation degree of attributes,allowing for a more accurate measurement of the importance degrees of attributes.Example analyses and experimental results demonstrate the feasibility and effectiveness of the algorithm.展开更多
This resolution 5 (25−1 factorial) study aimed to ascertain an understanding of the interactions between different geometries on the resulting Radar Cross Section (RCS) of a target. The results of the study are in lin...This resolution 5 (25−1 factorial) study aimed to ascertain an understanding of the interactions between different geometries on the resulting Radar Cross Section (RCS) of a target. The results of the study are in line with the general understanding of the impact different geometries have on RCS but show that geometries can also influence the variance of measured RCS, and typical attributes that reduce RCS increase the variance of the measured RCS. Notably, an increased angle between the front face of a plate and the direction of the radar signal decreased RCS but increased the variance of the RCS measured.展开更多
It is well-known that attribute reduction is a crucial action of rough set.The significant characteristic of attribute reduction is that it can reduce the dimensions of data with clear semantic explanations.Normally,t...It is well-known that attribute reduction is a crucial action of rough set.The significant characteristic of attribute reduction is that it can reduce the dimensions of data with clear semantic explanations.Normally,the learning performance of attributes in derived reduct is much more crucial.Since related measures of rough set dominate the whole process of identifying qualified attributes and deriving reduct,those measures may have a direct impact on the performance of selected attributes in reduct.However,most previous researches about attribute reduction take measures related to either supervised perspective or unsupervised perspective,which are insufficient to identify attributes with superior learning performance,such as stability and accuracy.In order to improve the classification stability and classification accuracy of reduct,in this paper,a novel measure is proposed based on the fusion of supervised and unsupervised perspectives:(1)in terms of supervised perspective,approximation quality is helpful in quantitatively characterizing the relationship between attributes and labels;(2)in terms of unsupervised perspective,conditional entropy is helpful in quantitatively describing the internal structure of data itself.In order to prove the effectiveness of the proposed measure,18 University of CaliforniaIrvine(UCI)datasets and 2 Yale face datasets have been employed in the comparative experiments.Finally,the experimental results show that the proposed measure does well in selecting attributes which can provide distinguished classification stabilities and classification accuracies.展开更多
Attribute reduction,as one of the essential applications of the rough set,has attracted extensive attention from scholars.Information granulation is a key step of attribute reduction,and its efficiency has a significa...Attribute reduction,as one of the essential applications of the rough set,has attracted extensive attention from scholars.Information granulation is a key step of attribute reduction,and its efficiency has a significant impact on the overall efficiency of attribute reduction.The information granulation of the existing neighborhood rough set models is usually a single layer,and the construction of each information granule needs to search all the samples in the universe,which is inefficient.To fill such gap,a new neighborhood rough set model is proposed,which aims to improve the efficiency of attribute reduction by means of two-layer information granulation.The first layer of information granulation constructs a mapping-equivalence relation that divides the universe into multiple mutually independent mapping-equivalence classes.The second layer of information granulation views each mapping-equivalence class as a sub-universe and then performs neighborhood informa-tion granulation.A model named mapping-equivalence neighborhood rough set model is derived from the strategy of two-layer information granulation.Experimental results show that compared with other neighborhood rough set models,this model can effectively improve the efficiency of attribute reduction and reduce the uncertainty of the system.The strategy provides a new thinking for the exploration of neighborhood rough set models and the study of attribute reduction acceleration problems.展开更多
Attribute reduction,also known as feature selection,for decision information systems is one of the most pivotal issues in machine learning and data mining.Approaches based on the rough set theory and some extensions w...Attribute reduction,also known as feature selection,for decision information systems is one of the most pivotal issues in machine learning and data mining.Approaches based on the rough set theory and some extensions were proved to be efficient for dealing with the problemof attribute reduction.Unfortunately,the intuitionistic fuzzy sets based methods have not received much interest,while these methods are well-known as a very powerful approach to noisy decision tables,i.e.,data tables with the low initial classification accuracy.Therefore,this paper provides a novel incremental attribute reductionmethod to dealmore effectivelywith noisy decision tables,especially for highdimensional ones.In particular,we define a new reduct and then design an original attribute reduction method based on the distance measure between two intuitionistic fuzzy partitions.It should be noted that the intuitionistic fuzzypartitiondistance iswell-knownas aneffectivemeasure todetermine important attributes.More interestingly,an incremental formula is also developed to quickly compute the intuitionistic fuzzy partition distance in case when the decision table increases in the number of objects.This formula is then applied to construct an incremental attribute reduction algorithm for handling such dynamic tables.Besides,some experiments are conducted on real datasets to show that our method is far superior to the fuzzy rough set based methods in terms of the size of reduct and the classification accuracy.展开更多
Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in t...Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in the seismic data,which is a time-intensive task.Many researchers have utilized a robust Grey-level co-occurrence matrix(GLCM)-based texture attributes to map reservoir heterogeneity.However,these attributes take seismic data as input and might not be sensitive to lateral lithology variation.To incorporate the lithology information,we have developed an innovative impedance-based texture approach using GLCM workflow by integrating 3D acoustic impedance volume(a rock propertybased attribute)obtained from a deep convolution network-based impedance inversion.Our proposed workflow is anticipated to be more sensitive toward mapping lateral changes than the conventional amplitude-based texture approach,wherein seismic data is used as input.To evaluate the improvement,we applied the proposed workflow to the full-stack 3D seismic data from the Poseidon field,NW-shelf,Australia.This study demonstrates that a better demarcation of reservoir gas sands with improved lateral continuity is achievable with the presented approach compared to the conventional approach.In addition,we assess the implication of multi-stage faulting on facies distribution for effective reservoir characterization.This study also suggests a well-bounded potential reservoir facies distribution along the parallel fault lines.Thus,the proposed approach provides an efficient strategy by integrating the impedance information with texture attributes to improve the inference on reservoir heterogeneity,which can serve as a promising tool for identifying potential reservoir zones for both production benefits and fluid storage.展开更多
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz...Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.展开更多
Attribute reduction is a hot topic in rough set research. As an extension of rough sets, neighborhood rough sets can effectively solve the problem of information loss after data discretization. However, traditional gr...Attribute reduction is a hot topic in rough set research. As an extension of rough sets, neighborhood rough sets can effectively solve the problem of information loss after data discretization. However, traditional greedy-based neighborhood rough set attribute reduction algorithms have a high computational complexity and long processing time. In this paper, a novel attribute reduction algorithm based on attribute importance is proposed. By using conditional information, the attribute reduction problem in neighborhood rough sets is discussed, and the importance of attributes is measured by conditional information gain. The algorithm iteratively removes the attribute with the lowest importance, thus achieving the goal of attribute reduction. Six groups of UCI datasets are selected, and the proposed algorithm SAR is compared with L<sub>2</sub>-ELM, LapTELM, CTSVM, and TBSVM classifiers. The results demonstrate that SAR can effectively improve the time consumption and accuracy issues in attribute reduction.展开更多
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca...Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.展开更多
Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics t...Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.展开更多
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites...Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.展开更多
Global variance reduction is a bottleneck in Monte Carlo shielding calculations.The global variance reduction problem requires that the statistical error of the entire space is uniform.This study proposed a grid-AIS m...Global variance reduction is a bottleneck in Monte Carlo shielding calculations.The global variance reduction problem requires that the statistical error of the entire space is uniform.This study proposed a grid-AIS method for the global variance reduction problem based on the AIS method,which was implemented in the Monte Carlo program MCShield.The proposed method was validated using the VENUS-Ⅲ international benchmark problem and a self-shielding calculation example.The results from the VENUS-Ⅲ benchmark problem showed that the grid-AIS method achieved a significant reduction in the variance of the statistical errors of the MESH grids,decreasing from 1.08×10^(-2) to 3.84×10^(-3),representing a 64.00% reduction.This demonstrates that the grid-AIS method is effective in addressing global issues.The results of the selfshielding calculation demonstrate that the grid-AIS method produced accurate computational results.Moreover,the grid-AIS method exhibited a computational efficiency approximately one order of magnitude higher than that of the AIS method and approximately two orders of magnitude higher than that of the conventional Monte Carlo method.展开更多
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ...The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.展开更多
Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)...Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.展开更多
The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous me...The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.展开更多
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in...We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.展开更多
The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-b...The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of Zn O electrocatalysts with different N-doping content was assessed in 1.0 M KHCO_(3) electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N:ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FE_(CO))of 92.7%at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped Zn O electrocatalyst(FE_(CO)of 63.4%at-0.78 V_(RHE)).Also,the N:ZnO-1 h electrocatalyst exhibited outstanding durability for 16 h,with a partial current density of-92.1 mA cm^(-2).This improvement of N:ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N:ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping.展开更多
基金Anhui Province Natural Science Research Project of Colleges and Universities(2023AH040321)Excellent Scientific Research and Innovation Team of Anhui Colleges(2022AH010098).
文摘The presence of numerous uncertainties in hybrid decision information systems(HDISs)renders attribute reduction a formidable task.Currently available attribute reduction algorithms,including those based on Pawlak attribute importance,Skowron discernibility matrix,and information entropy,struggle to effectively manages multiple uncertainties simultaneously in HDISs like the precise measurement of disparities between nominal attribute values,and attributes with fuzzy boundaries and abnormal values.In order to address the aforementioned issues,this paper delves into the study of attribute reduction withinHDISs.First of all,a novel metric based on the decision attribute is introduced to solve the problem of accurately measuring the differences between nominal attribute values.The newly introduced distance metric has been christened the supervised distance that can effectively quantify the differences between the nominal attribute values.Then,based on the newly developed metric,a novel fuzzy relationship is defined from the perspective of“feedback on parity of attribute values to attribute sets”.This new fuzzy relationship serves as a valuable tool in addressing the challenges posed by abnormal attribute values.Furthermore,leveraging the newly introduced fuzzy relationship,the fuzzy conditional information entropy is defined as a solution to the challenges posed by fuzzy attributes.It effectively quantifies the uncertainty associated with fuzzy attribute values,thereby providing a robust framework for handling fuzzy information in hybrid information systems.Finally,an algorithm for attribute reduction utilizing the fuzzy conditional information entropy is presented.The experimental results on 12 datasets show that the average reduction rate of our algorithm reaches 84.04%,and the classification accuracy is improved by 3.91%compared to the original dataset,and by an average of 11.25%compared to the other 9 state-of-the-art reduction algorithms.The comprehensive analysis of these research results clearly indicates that our algorithm is highly effective in managing the intricate uncertainties inherent in hybrid data.
基金funded by Vietnam National Foundation for Science and Technology Development(NAFOSTED)under Grant Number 102.05-2021.10.
文摘Attribute reduction through the combined approach of Rough Sets(RS)and algebraic topology is an open research topic with significant potential for applications.Several research works have introduced a strong relationship between RS and topology spaces for the attribute reduction problem.However,the mentioned recent methods followed a strategy to construct a new measure for attribute selection.Meanwhile,the strategy for searching for the reduct is still to select each attribute and gradually add it to the reduct.Consequently,those methods tended to be inefficient for high-dimensional datasets.To overcome these challenges,we use the separability property of Hausdorff topology to quickly identify distinguishable attributes,this approach significantly reduces the time for the attribute filtering stage of the algorithm.In addition,we propose the concept of Hausdorff topological homomorphism to construct candidate reducts,this method significantly reduces the number of candidate reducts for the wrapper stage of the algorithm.These are the two main stages that have the most effect on reducing computing time for the attribute reduction of the proposed algorithm,which we call the Cluster Filter Wrapper algorithm based on Hausdorff Topology.Experimental validation on the UCI Machine Learning Repository Data shows that the proposed method achieves efficiency in both the execution time and the size of the reduct.
文摘Attribute reduction is a research hotspot in rough set theory. Traditional heuristic attribute reduction methods add the most important attribute to the decision attribute set each time, resulting in multiple redundant attribute calculations, high time consumption, and low reduction efficiency. In this paper, based on the idea of sequential three-branch decision classification domain, attributes are treated as objects of three-branch division, and attributes are divided into core attributes, relatively necessary attributes, and unnecessary attributes using attribute importance and thresholds. Core attributes are added to the decision attribute set, unnecessary attributes are rejected from being added, and relatively necessary attributes are repeatedly divided until the reduction result is obtained. Experiments were conducted on 8 groups of UCI datasets, and the results show that, compared to traditional reduction methods, the method proposed in this paper can effectively reduce time consumption while ensuring classification performance.
基金Anhui Provincial University Research Project(Project Number:2023AH051659)Tongling University Talent Research Initiation Fund Project(Project Number:2022tlxyrc31)+1 种基金Tongling University School-Level Scientific Research Project(Project Number:2021tlxytwh05)Tongling University Horizontal Project(Project Number:2023tlxyxdz237)。
文摘For neighborhood rough set attribute reduction algorithms based on dependency degree,a neighborhood computation method incorporating attribute weight values and a neighborhood rough set attribute reduction algorithm using discernment as the heuristic information was proposed.The reduction algorithm comprehensively considers the dependency degree and neighborhood granulation degree of attributes,allowing for a more accurate measurement of the importance degrees of attributes.Example analyses and experimental results demonstrate the feasibility and effectiveness of the algorithm.
文摘This resolution 5 (25−1 factorial) study aimed to ascertain an understanding of the interactions between different geometries on the resulting Radar Cross Section (RCS) of a target. The results of the study are in line with the general understanding of the impact different geometries have on RCS but show that geometries can also influence the variance of measured RCS, and typical attributes that reduce RCS increase the variance of the measured RCS. Notably, an increased angle between the front face of a plate and the direction of the radar signal decreased RCS but increased the variance of the RCS measured.
基金supported by the National Natural Science Foundation of China(Grant Nos.62006099,62076111)the Key Research and Development Program of Zhenjiang-Social Development(Grant No.SH2018005)+1 种基金the Natural Science Foundation of Jiangsu Higher Education(Grant No.17KJB520007)Industry-school Cooperative Education Program of the Ministry of Education(Grant No.202101363034).
文摘It is well-known that attribute reduction is a crucial action of rough set.The significant characteristic of attribute reduction is that it can reduce the dimensions of data with clear semantic explanations.Normally,the learning performance of attributes in derived reduct is much more crucial.Since related measures of rough set dominate the whole process of identifying qualified attributes and deriving reduct,those measures may have a direct impact on the performance of selected attributes in reduct.However,most previous researches about attribute reduction take measures related to either supervised perspective or unsupervised perspective,which are insufficient to identify attributes with superior learning performance,such as stability and accuracy.In order to improve the classification stability and classification accuracy of reduct,in this paper,a novel measure is proposed based on the fusion of supervised and unsupervised perspectives:(1)in terms of supervised perspective,approximation quality is helpful in quantitatively characterizing the relationship between attributes and labels;(2)in terms of unsupervised perspective,conditional entropy is helpful in quantitatively describing the internal structure of data itself.In order to prove the effectiveness of the proposed measure,18 University of CaliforniaIrvine(UCI)datasets and 2 Yale face datasets have been employed in the comparative experiments.Finally,the experimental results show that the proposed measure does well in selecting attributes which can provide distinguished classification stabilities and classification accuracies.
基金supported by the National Natural Science Foundation of China (Nos.62006099,62076111)the Key Laboratory of Oceanographic Big Data Mining&Application of Zhejiang Province (No.OBDMA202104).
文摘Attribute reduction,as one of the essential applications of the rough set,has attracted extensive attention from scholars.Information granulation is a key step of attribute reduction,and its efficiency has a significant impact on the overall efficiency of attribute reduction.The information granulation of the existing neighborhood rough set models is usually a single layer,and the construction of each information granule needs to search all the samples in the universe,which is inefficient.To fill such gap,a new neighborhood rough set model is proposed,which aims to improve the efficiency of attribute reduction by means of two-layer information granulation.The first layer of information granulation constructs a mapping-equivalence relation that divides the universe into multiple mutually independent mapping-equivalence classes.The second layer of information granulation views each mapping-equivalence class as a sub-universe and then performs neighborhood informa-tion granulation.A model named mapping-equivalence neighborhood rough set model is derived from the strategy of two-layer information granulation.Experimental results show that compared with other neighborhood rough set models,this model can effectively improve the efficiency of attribute reduction and reduce the uncertainty of the system.The strategy provides a new thinking for the exploration of neighborhood rough set models and the study of attribute reduction acceleration problems.
基金funded by Hanoi University of Industry under Grant Number 27-2022-RD/HD-DHCN (URL:https://www.haui.edu.vn/).
文摘Attribute reduction,also known as feature selection,for decision information systems is one of the most pivotal issues in machine learning and data mining.Approaches based on the rough set theory and some extensions were proved to be efficient for dealing with the problemof attribute reduction.Unfortunately,the intuitionistic fuzzy sets based methods have not received much interest,while these methods are well-known as a very powerful approach to noisy decision tables,i.e.,data tables with the low initial classification accuracy.Therefore,this paper provides a novel incremental attribute reductionmethod to dealmore effectivelywith noisy decision tables,especially for highdimensional ones.In particular,we define a new reduct and then design an original attribute reduction method based on the distance measure between two intuitionistic fuzzy partitions.It should be noted that the intuitionistic fuzzypartitiondistance iswell-knownas aneffectivemeasure todetermine important attributes.More interestingly,an incremental formula is also developed to quickly compute the intuitionistic fuzzy partition distance in case when the decision table increases in the number of objects.This formula is then applied to construct an incremental attribute reduction algorithm for handling such dynamic tables.Besides,some experiments are conducted on real datasets to show that our method is far superior to the fuzzy rough set based methods in terms of the size of reduct and the classification accuracy.
文摘Reservoir heterogeneities play a crucial role in governing reservoir performance and management.Traditionally,detailed and inter-well heterogeneity analyses are commonly performed by mapping seismic facies change in the seismic data,which is a time-intensive task.Many researchers have utilized a robust Grey-level co-occurrence matrix(GLCM)-based texture attributes to map reservoir heterogeneity.However,these attributes take seismic data as input and might not be sensitive to lateral lithology variation.To incorporate the lithology information,we have developed an innovative impedance-based texture approach using GLCM workflow by integrating 3D acoustic impedance volume(a rock propertybased attribute)obtained from a deep convolution network-based impedance inversion.Our proposed workflow is anticipated to be more sensitive toward mapping lateral changes than the conventional amplitude-based texture approach,wherein seismic data is used as input.To evaluate the improvement,we applied the proposed workflow to the full-stack 3D seismic data from the Poseidon field,NW-shelf,Australia.This study demonstrates that a better demarcation of reservoir gas sands with improved lateral continuity is achievable with the presented approach compared to the conventional approach.In addition,we assess the implication of multi-stage faulting on facies distribution for effective reservoir characterization.This study also suggests a well-bounded potential reservoir facies distribution along the parallel fault lines.Thus,the proposed approach provides an efficient strategy by integrating the impedance information with texture attributes to improve the inference on reservoir heterogeneity,which can serve as a promising tool for identifying potential reservoir zones for both production benefits and fluid storage.
基金supported by the National Natural Science Foundation of China(22234005,21974070)the Natural Science Foundation of Jiangsu Province(BK20222015)。
文摘Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.
文摘Attribute reduction is a hot topic in rough set research. As an extension of rough sets, neighborhood rough sets can effectively solve the problem of information loss after data discretization. However, traditional greedy-based neighborhood rough set attribute reduction algorithms have a high computational complexity and long processing time. In this paper, a novel attribute reduction algorithm based on attribute importance is proposed. By using conditional information, the attribute reduction problem in neighborhood rough sets is discussed, and the importance of attributes is measured by conditional information gain. The algorithm iteratively removes the attribute with the lowest importance, thus achieving the goal of attribute reduction. Six groups of UCI datasets are selected, and the proposed algorithm SAR is compared with L<sub>2</sub>-ELM, LapTELM, CTSVM, and TBSVM classifiers. The results demonstrate that SAR can effectively improve the time consumption and accuracy issues in attribute reduction.
基金supported by the National Natural Science Foundation of China (22178149)Jiangsu Distinguished Professor Program+4 种基金Natural Science Foundation of Jiangsu Province for Outstanding Youth Scientists (BK20211599)Key R and D Project of Zhenjiang City (CQ2022001)Scientific Research Startup Foundation of Jiangsu University (Nos. 202096 and 22JDG020)Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment of Fuzhou University (SKLPEE-KF202310)the Opening Project of Structural Optimization and Application of Functional Molecules Key Laboratory of Sichuan Province (2023GNFZ-01)。
文摘Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.
基金supported by National Natural Science Foundation of China(12372049)Science and Technology Program of China National Accreditation Service for Confor-mity Assessment(2022CNAS15)+1 种基金Sichuan Science and Technology Program(2023JDRC0062)Independent Project of State Key Laboratory of Rail Transit Vehicle System(2023TPL-T06).
文摘Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.
基金the financial support from the Natural Science Foundation of China(Grant No.52172106)Anhui Provincial Natural Science Foundation(Grant Nos.2108085QB60 and 2108085QB61)China Postdoctoral Science Foundation(Grant Nos.2020M682057 and 2023T160651).
文摘Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.
基金supported by the Platform Development Foundation of the China Institute for Radiation Protection(No.YP21030101)the National Natural Science Foundation of China(General Program)(Nos.12175114,U2167209)+1 种基金the National Key R&D Program of China(No.2021YFF0603600)the Tsinghua University Initiative Scientific Research Program(No.20211080081).
文摘Global variance reduction is a bottleneck in Monte Carlo shielding calculations.The global variance reduction problem requires that the statistical error of the entire space is uniform.This study proposed a grid-AIS method for the global variance reduction problem based on the AIS method,which was implemented in the Monte Carlo program MCShield.The proposed method was validated using the VENUS-Ⅲ international benchmark problem and a self-shielding calculation example.The results from the VENUS-Ⅲ benchmark problem showed that the grid-AIS method achieved a significant reduction in the variance of the statistical errors of the MESH grids,decreasing from 1.08×10^(-2) to 3.84×10^(-3),representing a 64.00% reduction.This demonstrates that the grid-AIS method is effective in addressing global issues.The results of the selfshielding calculation demonstrate that the grid-AIS method produced accurate computational results.Moreover,the grid-AIS method exhibited a computational efficiency approximately one order of magnitude higher than that of the AIS method and approximately two orders of magnitude higher than that of the conventional Monte Carlo method.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(NRF,2021R1C1C1013953,2022K1A4A7A04094394,2022K1A4A7A04095890)。
文摘The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.
基金financial support from the National Natural Science Foundation of China(No.22272038)the Science and Technology Planning Project of Guangzhou City(No.2023A03J0026)。
文摘Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.
基金funded by the National Natural Science Foundation of China,China (Nos.52272303 and 52073212)the General Program of Municipal Natural Science Foundation of Tianjin,China (Nos.17JCYBJC22700 and 17JCYBJC17000)the State Scholarship Fund of China Scholarship Council,China (Nos.201709345012 and 201706255009)。
文摘The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.
基金the Natural Science Foundation of China(11922415,12274471)Guangdong Basic and Applied Basic Research Foundation(2022A1515011168,2019A1515011718,2019A1515011337)the Key Research and Development Program of Guangdong Province,China(2019B110209003).
文摘We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) (Grant Nos.2018R1A6A1A03024334,2019R1A2C1007637,2021M3I3A1082880,2021R1I1A1A01044174)the Basic Science Research Capacity Enhancement Project through Korea Basic Science Institute (Grant No.2019R1A6C1010024)。
文摘The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of Zn O electrocatalysts with different N-doping content was assessed in 1.0 M KHCO_(3) electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N:ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FE_(CO))of 92.7%at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped Zn O electrocatalyst(FE_(CO)of 63.4%at-0.78 V_(RHE)).Also,the N:ZnO-1 h electrocatalyst exhibited outstanding durability for 16 h,with a partial current density of-92.1 mA cm^(-2).This improvement of N:ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N:ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping.