The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild conditions.Herein...The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild conditions.Herein,we demonstrate that the descriptorΩparameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst(SAC)for driving electrochemical nitrogen reduction(NRR).Using twodimensional metal(M)-B_(x)P_(y)S_(z)N_m@C_(2)N as prototype SAC models,we reveal that^(*)N_(2)+(H~++e~-)→^(*)N_(2)H acts predominantly as the potential-limiting step(PLS)of NRR on M-B_(2)P_(2)S_(2)@C_(2)N and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N regardless of the distinction in coordination microenvironment.Among the 28 screened M active sites,withΩvalues close to the optimal 4,M-B_(2)P_(2)S_(2)@C_(2)N(M=V(Ω=3.53),Mo(Ω=5.12),and W(Ω=3.92))and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N(M=V(Ω=3.00),Mo(Ω=4.34),and W(Ω=3.32))yield the lowered limiting potential(U_(L))as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR catalysts.More importantly,these SACs are located around the top of volcano-shape plot of U_(L) versusΩ,re-validatingΩas an effective descriptor for accurately predicting the high-activity NRR SACs even with complex coordination.Our study unravels the relationship between active-site structure and NRR performance via the descriptorΩ,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules viaσ-donation andπ^(*)-backdonation mechanism.展开更多
Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused b...Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups,the practical applicability of CNs in photocatalysis is limited.In this study,CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing.The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV,increasing their absorption of visible light.Interestingly,the CNs were distorted after annealing,which can differentiate the spatial positions of electrons and holes,enhancing the visible-light absorption efficiency.As a result,when exposed to visible light,the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times.This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.展开更多
A method is proposed to deal with the uncertain multiple attribute group decision making problems,where 2-dimension uncertain linguistic variables(2DULVs)are used as the reliable way for the experts to express their f...A method is proposed to deal with the uncertain multiple attribute group decision making problems,where 2-dimension uncertain linguistic variables(2DULVs)are used as the reliable way for the experts to express their fuzzy subjective evaluation information.Firstly,in order to measure the 2DULVs more accurately,a new method is proposed to compare two 2DULVs,called a score function,while a new function is defined to measure the distance between two 2DULVs.Secondly,two optimization models are established to determine the weight of experts and attributes based on the new distance formula and a weighted average operator is used to determine the comprehensive evaluation value of each alternative.Then,a score function is used to determine the ranking of the alternatives.Finally,the effectiveness of the proposed method is proved by an illustrated example.展开更多
Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by a...Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by atomic defects and heterostructure effects.A three-dimensional(3D)free-standing integrated electrode was fabricated by numerous nearly-single-crystal TiO_(2-δ)N_δnanowire arrays.Based on the high electronic conductivity network,it exposes numerous active sites as well to facilitate the selective nitrogen adsorption and*H adsorption suppression.The synergistic effects between Ti^(3+)and oxygen vacancy(O_v)boost the intrinsic catalytic activity,in which Ti^(3+)acquired electrons via Ovcan effectively activate the N≡N bond and make it easy to bind with protons.The energy barrier of primary protonation process(*N_(2)+H^(+)+e^(-)→*NNH)can be dramatically decreased.The highest ammonia yield rate(14.33μg h^(-1)mgcat^(-1))emerges at-0.2 V,while the optimal ammonia Faradaic efficiency(9.17%)is acquired at-0.1 V.Density functional theory(DFT)calculation reveals that the Ti^(3+)can be served as the active sites for nitrogen adsorption and activation,while ammonia synthesis is accomplished by the distal pathway.The high electronic conductivity integrated network and synergistic effects can significantly facilitate nitrogen absorption and accelerate electrocatalytic reaction kinetic,which are responsible for the excellent NRR performance at room temperature.展开更多
Using the extension homogeneous balance method,we have obtained some new special types of soliton solutions of the (2+1)-dimensional KdV equation.Starting from the homogeneous balance method,one can obtain a nonlinear...Using the extension homogeneous balance method,we have obtained some new special types of soliton solutions of the (2+1)-dimensional KdV equation.Starting from the homogeneous balance method,one can obtain a nonlinear transformation to simple (2+1)-dimensional KdV equation into a linear partial differential equation and two bilinear partial differential equations.Usually,one can obtain only a kind of soliton-like solutions.In this letter,we find further some special types of the multisoliton solutions from the linear and bilinear partial differential equations.展开更多
A 2-dimension linguistic lattice implication algebra(2DL-LIA)can build a bridge between logical algebra and 2-dimension fuzzy linguistic information.In this paper,the notion of a Boolean element is proposed in a 2DL-L...A 2-dimension linguistic lattice implication algebra(2DL-LIA)can build a bridge between logical algebra and 2-dimension fuzzy linguistic information.In this paper,the notion of a Boolean element is proposed in a 2DL-LIA and some properties of Boolean elements are discussed.Then derivations on 2DL-LIAs are introduced and the related properties of derivations are investigated.Moreover,it proves that the derivations on 2DL-LIAs can be constructed by Boolean elements.展开更多
A new design method interleavers, 2-dimension interleavers, are proposed for interleave division multiple access （IDMA） systems. With a same interleaving rule named I＇, the row indices and column indices of a tradi...A new design method interleavers, 2-dimension interleavers, are proposed for interleave division multiple access （IDMA） systems. With a same interleaving rule named I＇, the row indices and column indices of a traditional block interleaving matrix are scrambled to obtain an interleaver, which is marked as the master interleaver. F is produced by a loworder PN sequence generator. Two ways are provided for generating different interleavers. One is that all interleavers are generated by the circular shifting master interleaver. The other is that different inter leavers are generated by different Ts. Besides, we prove that the minimum distance between two adjacent bits resulted from 2-dimension interleaves is much larger than that of other schemes, such as random interleavers, power interleavers, and shiffting interleaves. The simulation results show that 2-dimension interleavers can achieve much better performance with much less resource consumption than random interleavers in IDMA systems.展开更多
By using the extended homogeneous balance method, the localized coherent structures are studied. A nonlinear transformation was first established, and then the linearization form was obtained based on the extended hom...By using the extended homogeneous balance method, the localized coherent structures are studied. A nonlinear transformation was first established, and then the linearization form was obtained based on the extended homogeneous balance method for the higher order (2 + 1)-dimensional Broer-Kaup equations. Starting from this linearization form equation, a variable separation solution with the entrance of some arbitrary functions and some arbitrary parameters was constructed. The quite rich localized coherent structures were revealed. This method, which can be generalized to other (2 + I) -dimensional nonlinear evolution equation, is simple and powerful.展开更多
In this paper,the bifurcation of solitary,kink,anti-kink,and periodic waves for （2＋1）-dimension nonlinear dispersive long wave equation is studied by using the bifurcation theory of planar dynamical systems.Bifurca...In this paper,the bifurcation of solitary,kink,anti-kink,and periodic waves for （2＋1）-dimension nonlinear dispersive long wave equation is studied by using the bifurcation theory of planar dynamical systems.Bifurcation parameter sets are shown,and under various parameter conditions,all exact explicit formulas of solitary travelling wave solutions and kink travelling wave solutions and periodic travelling wave solutions are listed.展开更多
Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Co...Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.展开更多
With the help of the variable-coefficient generalized projected Ricatti equation expansion method, we present exact solutions for the generalized （2＋1）-dimensional nonlinear SchrSdinger equation with variable coeff...With the help of the variable-coefficient generalized projected Ricatti equation expansion method, we present exact solutions for the generalized （2＋1）-dimensional nonlinear SchrSdinger equation with variable coefficients. These solutions include solitary wave solutions, soliton-like solutions and trigonometric function solutions. Among these solutions, some are found for the first time.展开更多
基金supported by the National Natural Science Foundation of China (21673137)。
文摘The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild conditions.Herein,we demonstrate that the descriptorΩparameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst(SAC)for driving electrochemical nitrogen reduction(NRR).Using twodimensional metal(M)-B_(x)P_(y)S_(z)N_m@C_(2)N as prototype SAC models,we reveal that^(*)N_(2)+(H~++e~-)→^(*)N_(2)H acts predominantly as the potential-limiting step(PLS)of NRR on M-B_(2)P_(2)S_(2)@C_(2)N and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N regardless of the distinction in coordination microenvironment.Among the 28 screened M active sites,withΩvalues close to the optimal 4,M-B_(2)P_(2)S_(2)@C_(2)N(M=V(Ω=3.53),Mo(Ω=5.12),and W(Ω=3.92))and M-B_(1)P_(1)S_(1)N_(3)@C_(2)N(M=V(Ω=3.00),Mo(Ω=4.34),and W(Ω=3.32))yield the lowered limiting potential(U_(L))as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR catalysts.More importantly,these SACs are located around the top of volcano-shape plot of U_(L) versusΩ,re-validatingΩas an effective descriptor for accurately predicting the high-activity NRR SACs even with complex coordination.Our study unravels the relationship between active-site structure and NRR performance via the descriptorΩ,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules viaσ-donation andπ^(*)-backdonation mechanism.
基金supported by the National Natural Science Foundation of China(Nos.12104352 and 12204294)Fundamental Research Funds for the Central Universities(Nos.XJS_(2)12208 and 2020BJ-56)+1 种基金Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K67)the Natural Science Foundation of Shaanxi Province(Nos.2019JCW-17 and 2020JCW-15).
文摘Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups,the practical applicability of CNs in photocatalysis is limited.In this study,CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing.The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV,increasing their absorption of visible light.Interestingly,the CNs were distorted after annealing,which can differentiate the spatial positions of electrons and holes,enhancing the visible-light absorption efficiency.As a result,when exposed to visible light,the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times.This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.
基金This work was supported by the Natural Science Foundation of Liaoning Province(2013020022).
文摘A method is proposed to deal with the uncertain multiple attribute group decision making problems,where 2-dimension uncertain linguistic variables(2DULVs)are used as the reliable way for the experts to express their fuzzy subjective evaluation information.Firstly,in order to measure the 2DULVs more accurately,a new method is proposed to compare two 2DULVs,called a score function,while a new function is defined to measure the distance between two 2DULVs.Secondly,two optimization models are established to determine the weight of experts and attributes based on the new distance formula and a weighted average operator is used to determine the comprehensive evaluation value of each alternative.Then,a score function is used to determine the ranking of the alternatives.Finally,the effectiveness of the proposed method is proved by an illustrated example.
基金financially supported by the Liao Ning Revitalization Talents Program(XLYC2007155)the Fundamental Research Funds for the Central Universities(N2025018,N2025009)。
文摘Owing to the environmental and inherent advantages,nitrogen reduction reaction(NRR)by electrocatalysts attracts global attention.The surface engineering is widely employed to enhance the electrocatalytic activity by atomic defects and heterostructure effects.A three-dimensional(3D)free-standing integrated electrode was fabricated by numerous nearly-single-crystal TiO_(2-δ)N_δnanowire arrays.Based on the high electronic conductivity network,it exposes numerous active sites as well to facilitate the selective nitrogen adsorption and*H adsorption suppression.The synergistic effects between Ti^(3+)and oxygen vacancy(O_v)boost the intrinsic catalytic activity,in which Ti^(3+)acquired electrons via Ovcan effectively activate the N≡N bond and make it easy to bind with protons.The energy barrier of primary protonation process(*N_(2)+H^(+)+e^(-)→*NNH)can be dramatically decreased.The highest ammonia yield rate(14.33μg h^(-1)mgcat^(-1))emerges at-0.2 V,while the optimal ammonia Faradaic efficiency(9.17%)is acquired at-0.1 V.Density functional theory(DFT)calculation reveals that the Ti^(3+)can be served as the active sites for nitrogen adsorption and activation,while ammonia synthesis is accomplished by the distal pathway.The high electronic conductivity integrated network and synergistic effects can significantly facilitate nitrogen absorption and accelerate electrocatalytic reaction kinetic,which are responsible for the excellent NRR performance at room temperature.
文摘Using the extension homogeneous balance method,we have obtained some new special types of soliton solutions of the (2+1)-dimensional KdV equation.Starting from the homogeneous balance method,one can obtain a nonlinear transformation to simple (2+1)-dimensional KdV equation into a linear partial differential equation and two bilinear partial differential equations.Usually,one can obtain only a kind of soliton-like solutions.In this letter,we find further some special types of the multisoliton solutions from the linear and bilinear partial differential equations.
基金Supported by the National Natural Science Foundation of China(11501523,61673320)。
文摘A 2-dimension linguistic lattice implication algebra(2DL-LIA)can build a bridge between logical algebra and 2-dimension fuzzy linguistic information.In this paper,the notion of a Boolean element is proposed in a 2DL-LIA and some properties of Boolean elements are discussed.Then derivations on 2DL-LIAs are introduced and the related properties of derivations are investigated.Moreover,it proves that the derivations on 2DL-LIAs can be constructed by Boolean elements.
基金supported by the National Key Lab. Research Foundation of China under Grant No.2007CB310604
文摘A new design method interleavers, 2-dimension interleavers, are proposed for interleave division multiple access （IDMA） systems. With a same interleaving rule named I＇, the row indices and column indices of a traditional block interleaving matrix are scrambled to obtain an interleaver, which is marked as the master interleaver. F is produced by a loworder PN sequence generator. Two ways are provided for generating different interleavers. One is that all interleavers are generated by the circular shifting master interleaver. The other is that different inter leavers are generated by different Ts. Besides, we prove that the minimum distance between two adjacent bits resulted from 2-dimension interleaves is much larger than that of other schemes, such as random interleavers, power interleavers, and shiffting interleaves. The simulation results show that 2-dimension interleavers can achieve much better performance with much less resource consumption than random interleavers in IDMA systems.
文摘By using the extended homogeneous balance method, the localized coherent structures are studied. A nonlinear transformation was first established, and then the linearization form was obtained based on the extended homogeneous balance method for the higher order (2 + 1)-dimensional Broer-Kaup equations. Starting from this linearization form equation, a variable separation solution with the entrance of some arbitrary functions and some arbitrary parameters was constructed. The quite rich localized coherent structures were revealed. This method, which can be generalized to other (2 + I) -dimensional nonlinear evolution equation, is simple and powerful.
基金Supported by the National Natural Science Foundation of China (10871206)Program for Excellent Talents in Guangxi Higher Education Institutions
文摘In this paper,the bifurcation of solitary,kink,anti-kink,and periodic waves for （2＋1）-dimension nonlinear dispersive long wave equation is studied by using the bifurcation theory of planar dynamical systems.Bifurcation parameter sets are shown,and under various parameter conditions,all exact explicit formulas of solitary travelling wave solutions and kink travelling wave solutions and periodic travelling wave solutions are listed.
基金supported by the National Natural Science Foundation of China(22302115,22072079)the Fundamental Research Program of Shanxi Province(202303021221056).
文摘Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.
基金Supported by the Science Research Foundation of Zhanjiang Normal University(L0803)
文摘With the help of the variable-coefficient generalized projected Ricatti equation expansion method, we present exact solutions for the generalized （2＋1）-dimensional nonlinear SchrSdinger equation with variable coefficients. These solutions include solitary wave solutions, soliton-like solutions and trigonometric function solutions. Among these solutions, some are found for the first time.
