We propose the new field potential by maintaining both the symmetry of the scalar gauge and the conservation law keeping N?ether’s theorem, while disregarding the symmetry of the vector gauge. The new potential forms...We propose the new field potential by maintaining both the symmetry of the scalar gauge and the conservation law keeping N?ether’s theorem, while disregarding the symmetry of the vector gauge. The new potential forms like the well-type potential where a particle behaves almost freely but is very hard to escape without external energy, which can be interpreted as local confinement and asymptotic freedom. By assuming a 2-dimensional metric tensor in 4-dimensional space-time, we suggest the existence of 3 kinds of particles that resemble QCD with 3 color charges. We also show that the mass term exists but comes to zero and derive the charge and spin values. We can regard the particle with this new potential as a gluon, and the interaction in this well-type potential as a strong interaction for the properties of mass, charge, spin, and its behavior. We suggest the eight-fold way with this new particle, which is similar to the existing method based on SU (3) symmetry. Even though the strong interaction has been analyzed in the standard model and string theory, we build a new consistent model based on the theory of relativity including Riemann geometry, and show the unification of gravitational and strong interactional field.展开更多
The strong force effect on gluon distribution of quark-gluon plasma and its influence on jet energy loss with detailed balance are studied. We solve the possibility equation and obtain the value of non-extensive param...The strong force effect on gluon distribution of quark-gluon plasma and its influence on jet energy loss with detailed balance are studied. We solve the possibility equation and obtain the value of non-extensive parameter q. In the presence of strong interaction, more gluons stay at low-energy state than the free gluon case. The strong interaction effect is found to be important for jet energy loss with detailed balance at intermediate jet energy. The energy gain via absorption increases with the strong interaction. This will affect the nuclear modification factor RAA and the parameter of q at intermediate jet energy.展开更多
Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-gr...Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.展开更多
The unique hierarchical nitrogen-doped carbon nanocages(h NCNC) are used as a new support to homogeneously immobilize spinel Co Fe_2O_4 nanoparticles by a facile solvothermal method. The so-constructed hierarchical Co...The unique hierarchical nitrogen-doped carbon nanocages(h NCNC) are used as a new support to homogeneously immobilize spinel Co Fe_2O_4 nanoparticles by a facile solvothermal method. The so-constructed hierarchical Co Fe_2O_4/h NCNC catalyst exhibits a high oxygen reduction activity with an onset potential of0.966 V and half-wave potential of 0.819 V versus reversible hydrogen electrode, far superior to the corresponding 0.846 and 0.742 V for its counterpart of Co Fe_2O_4/h CNC with undoped hierarchical carbon nanocages(h CNC) as the support, which locates at the top level for spinel-based catalysts to date.Consequently, the Co Fe_2O_4/h NCNC displays the superior performance to the Co Fe_2O_4/h CNC, when used as the cathode catalysts in the home-made Al-air batteries. X-ray photoelectron spectroscopy characterizations reveal the more charge transfer from Co Fe_2O_4 to h NCNC than to h CNC, indicating the stronger interaction between Co Fe_2O_4 and h NCNC due to the nitrogen participation. The enhanced interaction and hierarchical morphology favor the high dispersion and modification of electronic states for the active species as well as the mass transport during the oxygen reduction process, which plays a significant role in boosting the electrocatalytic performances. In addition, we noticed the high sensitivity of O 1 s spectrum to the particle size and chemical environment for spinel oxides, which is used as an indicator to understand the evolution of ORR activities for all the Co Fe_2O_4-related contrast catalysts. Accordingly,the well-defined structure-performance relationship is demonstrated by the combination of experimental characterizations with theoretical calculations. This study provides a promising strategy to develop efficient, inexpensive and durable oxygen reduction electrocatalysts by tuning the interaction between spinel metal oxides and the carbon-based supports.展开更多
In this paper, by using the Lagrangian coordinates, the strongly oblique interactions between solitary waves with the same mode in a stratified fluid ape discussed, which includes the shallow fluid case and deep fluid...In this paper, by using the Lagrangian coordinates, the strongly oblique interactions between solitary waves with the same mode in a stratified fluid ape discussed, which includes the shallow fluid case and deep fluid case. It is found that the interactions are described by the KP equation for the shallow fluid case, the two-dimensional intermediate long wave equation (2D-ILW equation) for the deep fluid case and the two-dimensional BO equation (2D-BO equation) for the infinite deep fluid case.展开更多
High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging sca...High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.展开更多
The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caus...The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.展开更多
Electromagnetically induced transparency (EIT) is investigated in a system of cold, interacting cesium Rydberg atoms. The utilized cesium levels 6S1/2, 6P3/2 and nD5/2 constitute a cascade three-level system, in whi...Electromagnetically induced transparency (EIT) is investigated in a system of cold, interacting cesium Rydberg atoms. The utilized cesium levels 6S1/2, 6P3/2 and nD5/2 constitute a cascade three-level system, in which a coupling laser drives the Rydberg transition, and a probe laser detects the EIT signal on the 6S1/2 to 6/23/2 transition. Rydberg EIT spectra are found to depend on the strong interaction between the Rydberg atoms. Diminished EIT transparency is obtained when the Rabi frequency of the probe laser is increased, whereas the corresponding linewidth remains unchanged. To model the system with a three-level Linclblad equation, we introduce a Rydberg-level dephasing rate γ3 = κ×(P33/Ωp)^2, with a value κ that depends on the ground-state atom density and the Rydberg level, The simulation results are largely consistent with the measurements. The experiments, in which the principal quantum number is varied between 30 and 43, demonstrate that the EIT reduction observed at large Ωp is due to the strong interactions between the Rydberg atoms.展开更多
Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)...Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)effect over FeNi/Al-Ce-O catalysts is revealed via X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(TPR),and energy dispersive X-ray spectroscopy(EDS)elemental mapping.The introduction of Al into Al-Ce-O supports significantly influences the dispersion of surface active components and improves the catalytic performance for DRE over supported FeNi catalysts due to enhancement of the SMSI effect.The catalytic properties,for example,C_(2)H_(6) and CO_(2) conversion,CO selectivity and yield,and turnover frequencies(TOFs),of supported FeNi catalysts first increase and then decrease with increasing Al content,following the same trend as the theoretical effective surface area(TESA)of the corresponding catalysts.The FeNi/Ce-Al_(0.5) catalyst,with 50%Al content,exhibits the best DRE performance under steady-state conditions at 873 K.As observed by with in situ Fourier transform infrared spectroscopy(FTIR)analysis,the introduction of Al not only increases the content of surface Ce3+and oxygen vacancies but also promotes the dispersion of surface active components,which further alters the catalytic properties for DRE over supported FeNi catalysts.展开更多
In this paper we study the interaction of strong and weak singularities for hyperbolic system of conservation laws in multidimensional space. Under the assumption of transversal intersect of the shock front with the b...In this paper we study the interaction of strong and weak singularities for hyperbolic system of conservation laws in multidimensional space. Under the assumption of transversal intersect of the shock front with the bicharacteristics bearing weak singularities we proved a theorem on regularity propagation across the shock front.展开更多
The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research att...The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous catalysis.Notably,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI formation.This emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.展开更多
We study the coexistence of antiferromagnetism and unconventional superconductivity on the Creutz lattice which shows strictly flat bands in the noninteracting regime.The famous renormalized mean-field theory is used ...We study the coexistence of antiferromagnetism and unconventional superconductivity on the Creutz lattice which shows strictly flat bands in the noninteracting regime.The famous renormalized mean-field theory is used to deal with strong electron-electron repulsive Hubbard interaction in the effective low-energy t-J model,the superfluid weight of the unconventional superconducting state has been calculated via the linear response theory.An unconventional superconducting state with both spin-singlet and staggered spin-triplet pairs emerges beyond a critical antiferromagnetic coupling interaction,while antiferromagnetism accompanies this state.The superconducting state with only spin-singlet pairs is dominant with paramagnetic phase.The A phase is analogous to the pseudogap phase,which shows that electrons go to form pairs but do not cause a supercurrent.We also show the superfluid behavior of the unconventional superconducting state and its critical temperature.It is proven directly that the flat band can effectively raise the critical temperature of superconductivity.It is implementable to simulate and control strongly-correlated electrons'behavior on the Creutz lattice in the ultracold atoms experiment or other artificial structures.Our results may help the understanding of the interplay between unconventional superconductivity and magnetism.展开更多
Three Clifford algebras are sufficient to describe all interactions of modern physics: The Clifford algebra of the usual space is enough to describe all aspects of electromagnetism, including the quantum wave of the e...Three Clifford algebras are sufficient to describe all interactions of modern physics: The Clifford algebra of the usual space is enough to describe all aspects of electromagnetism, including the quantum wave of the electron. The Clifford algebra of space-time is enough for electro-weak interactions. To get the gauge group of the standard model, with electro-weak and strong interactions, a third algebra is sufficient, with only two more dimensions of space. The Clifford algebra of space allows us to include also gravitation. We discuss the advantages of our approach.展开更多
For the unification of gravitation with electromagnetism, weak and strong interactions, we use a unique and very simple framework, the Clifford algebra of space . We enlarge our previous wave equation to the general c...For the unification of gravitation with electromagnetism, weak and strong interactions, we use a unique and very simple framework, the Clifford algebra of space . We enlarge our previous wave equation to the general case, including all leptons, quarks and antiparticles of the first generation. The wave equation is a generalization of the Dirac equation with a compulsory non-linear mass term. This equation is form invariant under the group of the invertible elements in the space algebra. The form invariance is fully compatible with the gauge invariance of the standard model. The wave equations of the different particles come by Lagrange equations from a Lagrangian density and this Lagrangian density is the sum of the real parts of the wave equations. Both form invariance and gauge invariance are exact symmetries, not only partial or broken symmetries. Inertia is already present in the part of the gauge group and the inertial chiral potential vector simplifies weak interactions. Relativistic quantum physics is then a naturally yet unified theory, including all interactions.展开更多
The high cost,scarcity,and poor stability of precious-metal-based catalysts have hindered their extensive application in energy conversion and storage.This stimulates the search for earth-abundant alternatives to repl...The high cost,scarcity,and poor stability of precious-metal-based catalysts have hindered their extensive application in energy conversion and storage.This stimulates the search for earth-abundant alternatives to replace noble metal electrocatalysts.Hence,in this study,we investigate a novel and low-cost bifunctional electrocatalyst consisting of ZnCoMnO_(4) anchored on nitrogen-doped graphene oxide(ZnCoMnO_(4)/N-rGO).Benefiting from the strong Co-N interaction in ZnCoMnO_(4) and the coupled conductive N-rGO,the catalysts exhibit high electrocatalytic activity.Moreover,density functional theory calculations support the dominant role of the strong Co-N electronic interaction,which leads to ZnCoMnO_(4)/N-rGO having more favorable binding energies with O2 and H_(2) O,resulting in fast reaction kinetics.The obtained ZnCoMnO_(4)/N-rGO electrocatalyst exhibits superb bifunctional activity,with a half-wave potential of 0.83 V for the oxygen reduction reaction and a low onset potential of 1.57 V for the oxygen evolution reaction in 0.1 M KOH solution.Furthermore,a Zn-air battery driven by the ZnCoMnO_(4)/N-rGO catalyst shows remarkable discharge/charge performance,with a power density of 138.52 mW cm^(-2) and longterm cycling stability for 48 h.This work provides a promising multifunctional electrocatalyst based on non-noble metals for the storage and conversion of renewable energy.展开更多
TWC-equipped exhausts are widely used in gasoline-fueled vehicles to meet stringent emission regulations. The main components in TWCs are precious metals such as palladium (Pd), platinum (Pt), and rhodium (Rh) as the ...TWC-equipped exhausts are widely used in gasoline-fueled vehicles to meet stringent emission regulations. The main components in TWCs are precious metals such as palladium (Pd), platinum (Pt), and rhodium (Rh) as the active component, and inorganic oxides such as γ-alumina (Al 2 O 3 ), ceria (CeO 2 ), zirconia (ZrO 2 ) and ceria-zirconia (CeO 2-ZrO 2 ) are used as the support. Interaction of precious metals and support plays an important role in the thermal stability and catalytic performance of TWCs. The support can improve the dispersion of precious metals and suppress the sintering of precious metals at high temperature. In the same, precious metals can also enhance the redox performance and oxygen storage capacity of support. This paper reviews the reaction phenomenon and mechanism of precious metals (Pt, Pd, Rh) and supports such as Al 2 O 3 , CeO 2-based composite oxides.展开更多
In this study,K_(x)-Mn-Ce catalysts prepared by sol-gel method were investigated for toluene oxidation.Compared with Mn-Ce,the catalytic performance of K_(x)-Mn-Ce was further improved.X-ray diffraction(XRD),high reso...In this study,K_(x)-Mn-Ce catalysts prepared by sol-gel method were investigated for toluene oxidation.Compared with Mn-Ce,the catalytic performance of K_(x)-Mn-Ce was further improved.X-ray diffraction(XRD),high resolution transmission electron microscopy(HRTEM)and Raman analyses demonstrate that K ions enter the lattice of CeO_(2) and disperse uniformly.The results of X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(H_(2)-TPR).and O_(2)-temperature programmed desorption(O_(2)-TPD)analyses indicate that there is a strong interaction between K,Mn and Ce;the charge co mpensation effect would be induced when K ions enter the lattice of CeO_(2),which leads to more oxygen vacancies due to the generation of more Ce^(3+).Toluene-TPD shows that K-doping enhances the activation ability of toluene.Among all catalysts,K0.1-Mn-Ce shows the highest concentration of Mn^(4+),Ce^(3+),Osur,and redox ability,resulting in higher low-temperature catalytic activity.Additionally,the results of stability and water resistance also prove that K0.1-Mn-Ce catalyst possesses excellent stability and water resistance.展开更多
For the high-temperature catalytic reaction,revealing the interface of catalyst–support and its evolution under reactive conditions is of crucial importance for understanding the reaction mechanism.However,much less ...For the high-temperature catalytic reaction,revealing the interface of catalyst–support and its evolution under reactive conditions is of crucial importance for understanding the reaction mechanism.However,much less is known about the atomic-scale interface of the hard-to-reduce silica-metal compared to that of reducible oxide systems.Here we reported the general behaviors of SiO_(2)migration onto various metal(Pt,Co,Rh,Pd,Ru,and Ni)nanocrystals supported on silica.Typically,the Pt/SiO_(2)catalytic system,which boosted the CO_(2)hydrogenation to CO,exhibited the reduction of Si0 at the Pt-SiO2 interface under H2 and further Si diffusion into the near surface of Pt nanoparticles,which was unveiled by in-situ environmental transmission electron microscopy coupled with spectroscopies.This reconstructed interface with Si diffused into Pt increased the sinter resistance of catalyst and thus improved the catalytic stability.The morphology of metal nanoparticles with SiO_(2)overlayer were dynamically evolved under reducing,vacuum,and oxidizing atmospheres,with a thicker SiO_(2)layer under oxidizing condition.The theoretical calculations revealed the mechanism that the Si-Pt surface provided synergistic sites for the activation of CO_(2)/H_(2)to produce CO with lower energy barriers,consequently boosting the high-temperature reverse water-gas shift reaction.These findings deepen the understanding toward the interface structure of inert oxide supported catalysts.展开更多
Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of bot...Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of both metal-air batteries and fuel cells,and precious metals are the dominant catalysts carrying out the ORR in their cathodes.However,how to manipulate the electronic structure of precious metals as active sites to further promote ORR performance and maximize the utilization rate is still under development.Metal oxide serves as suitable and promising support that can strongly interact with precious metals for both activity and durability enhancement.Herein,we present recent research updates on strong precious metal-metal oxide interaction(SPMMOI)utilized in ORR.We start by introducing the background of ORR,the issues to be solved,and its practical applications followed by a thorough discussion of the reaction mechanism and comprehensive evaluation protocols of performance.We then provide a complete understanding of theworking principle of SPMMOI and highlight the related advances.Finally,we summarize the merits of the precious metal-metal oxide systemand propose the research direction aswell as some urgent problems to be addressed in the future.展开更多
The direct conversion of ethanol to 1,1-diethoxyethane(DEE)through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and industry.Based on thermodynamics,the oxidative dehydrogenati...The direct conversion of ethanol to 1,1-diethoxyethane(DEE)through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and industry.Based on thermodynamics,the oxidative dehydrogenation of alcohol to acetaldehyde requires high temperature to activate oxygen to realize the C-H cleavage,while the acetalization of acetaldehyde with ethanol is exothermic reversible reaction favorable at low temperature.The mismatching of the reaction condition for the two consecutive steps makes it a great challenge to achieve both high ethanol conversion and high DEE selectivity.This work reports a highly efficient bi-functional catalysis by Bi/BiCeO_(x)for one-pot oxidative dehydrogenation-acetalization route from ethanol to DEE under 150℃and ambient pressure,affording a selectivity of 98.5%±0.5%to DEE at an ethanol conversion of 87.0%±1.0%.An efficient tandem catalysis has been achieved on the interfacial Bi^(δ)+-Ov-Ce^(III)sites in Bi/BiCeO_(x)established by strong metal-support interaction,in which Biδ+-Ov-sites contribute to the oxidative dehydrogenation of ethanol at mild temperature,and-Ov-CeIII sites to the subsequent acetalization between the generated acetaldehyde and ethanol.展开更多
文摘We propose the new field potential by maintaining both the symmetry of the scalar gauge and the conservation law keeping N?ether’s theorem, while disregarding the symmetry of the vector gauge. The new potential forms like the well-type potential where a particle behaves almost freely but is very hard to escape without external energy, which can be interpreted as local confinement and asymptotic freedom. By assuming a 2-dimensional metric tensor in 4-dimensional space-time, we suggest the existence of 3 kinds of particles that resemble QCD with 3 color charges. We also show that the mass term exists but comes to zero and derive the charge and spin values. We can regard the particle with this new potential as a gluon, and the interaction in this well-type potential as a strong interaction for the properties of mass, charge, spin, and its behavior. We suggest the eight-fold way with this new particle, which is similar to the existing method based on SU (3) symmetry. Even though the strong interaction has been analyzed in the standard model and string theory, we build a new consistent model based on the theory of relativity including Riemann geometry, and show the unification of gravitational and strong interactional field.
基金Supported by the National Natural Science Foundation of China under Grant No 11205024the Doctoral Scientific Fund Project of the Ministry of Education of China under Grant No 2012004112004
文摘The strong force effect on gluon distribution of quark-gluon plasma and its influence on jet energy loss with detailed balance are studied. We solve the possibility equation and obtain the value of non-extensive parameter q. In the presence of strong interaction, more gluons stay at low-energy state than the free gluon case. The strong interaction effect is found to be important for jet energy loss with detailed balance at intermediate jet energy. The energy gain via absorption increases with the strong interaction. This will affect the nuclear modification factor RAA and the parameter of q at intermediate jet energy.
基金supported by the National Natural Science Foundation of China(Grant Nos.22075159,22002066)Shandong Taishan Scholars Project(Grant Nos.ts20190932,tsqn202103058)+1 种基金Open Fund of Hubei Key Laboratory of Processing and Application of Catalytic Materials(Grant No.202203404)Postdoctoral Applied Research Project in Qingdao,and the Youth Innovation Team Project of Shandong Provincial Education Department(Grant No.2019KJC023).
文摘Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.
基金supported by the National Natural Science Foundation of China (21473089, 51232003, 21373108, 21573107, and 51571110)the National Basic Research Program of China (2013CB932902)+2 种基金Changzhou Technology Support Program (CE20130032)Priority Academic Program Development of Jiangsu Higher Education InstitutionsFundamental Research Funds for the Central Universities
文摘The unique hierarchical nitrogen-doped carbon nanocages(h NCNC) are used as a new support to homogeneously immobilize spinel Co Fe_2O_4 nanoparticles by a facile solvothermal method. The so-constructed hierarchical Co Fe_2O_4/h NCNC catalyst exhibits a high oxygen reduction activity with an onset potential of0.966 V and half-wave potential of 0.819 V versus reversible hydrogen electrode, far superior to the corresponding 0.846 and 0.742 V for its counterpart of Co Fe_2O_4/h CNC with undoped hierarchical carbon nanocages(h CNC) as the support, which locates at the top level for spinel-based catalysts to date.Consequently, the Co Fe_2O_4/h NCNC displays the superior performance to the Co Fe_2O_4/h CNC, when used as the cathode catalysts in the home-made Al-air batteries. X-ray photoelectron spectroscopy characterizations reveal the more charge transfer from Co Fe_2O_4 to h NCNC than to h CNC, indicating the stronger interaction between Co Fe_2O_4 and h NCNC due to the nitrogen participation. The enhanced interaction and hierarchical morphology favor the high dispersion and modification of electronic states for the active species as well as the mass transport during the oxygen reduction process, which plays a significant role in boosting the electrocatalytic performances. In addition, we noticed the high sensitivity of O 1 s spectrum to the particle size and chemical environment for spinel oxides, which is used as an indicator to understand the evolution of ORR activities for all the Co Fe_2O_4-related contrast catalysts. Accordingly,the well-defined structure-performance relationship is demonstrated by the combination of experimental characterizations with theoretical calculations. This study provides a promising strategy to develop efficient, inexpensive and durable oxygen reduction electrocatalysts by tuning the interaction between spinel metal oxides and the carbon-based supports.
文摘In this paper, by using the Lagrangian coordinates, the strongly oblique interactions between solitary waves with the same mode in a stratified fluid ape discussed, which includes the shallow fluid case and deep fluid case. It is found that the interactions are described by the KP equation for the shallow fluid case, the two-dimensional intermediate long wave equation (2D-ILW equation) for the deep fluid case and the two-dimensional BO equation (2D-BO equation) for the infinite deep fluid case.
基金project was funded by National Natural Science Foundation of China(Nos.21901154,21671129)the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT17R71)。
文摘High-efficiency electrochemical hydrogen evolution reaction(HER)offers a promising strategy to address energy and environmental crisis.Platinum is the most effective electrocatalyst for the HER.However,challenging scarcity,valuableness,and poor electrochemical stability still hinder its wide application.Here,we designed an outstanding HER electrocatalyst,highly dispersed rhodium(Rh)nanoparticles with an average diameter of only 3 nm supported on boron(B)nanosheets.The HER catalytic activity is even comparable to that of commercial platinum catalysts,with an overpotential of only 66 mV in 0.5 M H_(2)SO_(4) and 101 mV in 1 M KOH to reach the current density of 10 mA cm−2.Meanwhile,the catalyst exhibited impressive electrochemical durability during long-term electrochemical processes in acidic and alkaline media,even the simu-lated seawater environment.Theoretical calculations unraveled that the structure-activity relationship between B(104)crystal plane and Rh(111)crystal plane is beneficial to the release of hydrogen,and surface O plays a vital role in the catalysis process.Our work may gain insights into the development of supported metal catalysts with robust catalytic performance through precise engineering of the strong metal-supported interaction effect.
基金supported by the National Natural Science Foundation of China(21875155,51675275,21703185 and 21473119)Q.B.Z.acknowledges the Leading Project Foundation of Science Department of Fujian Province(2018H0034)Shenzhen Science and Technology Planning Project(JCYJ20170818153427106).
文摘The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.
基金Supported by the National Basic Research Program of China under Grant No 2012CB921603Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China under Grant No IRT13076+2 种基金the State Key Program of the National Natural Science of China under Grant No 11434007the National Natural Science of China under Grant Nos 11274209,61475090,60378039 and 61378013Shanxi Scholarship Council of China(2014-009)
文摘Electromagnetically induced transparency (EIT) is investigated in a system of cold, interacting cesium Rydberg atoms. The utilized cesium levels 6S1/2, 6P3/2 and nD5/2 constitute a cascade three-level system, in which a coupling laser drives the Rydberg transition, and a probe laser detects the EIT signal on the 6S1/2 to 6/23/2 transition. Rydberg EIT spectra are found to depend on the strong interaction between the Rydberg atoms. Diminished EIT transparency is obtained when the Rabi frequency of the probe laser is increased, whereas the corresponding linewidth remains unchanged. To model the system with a three-level Linclblad equation, we introduce a Rydberg-level dephasing rate γ3 = κ×(P33/Ωp)^2, with a value κ that depends on the ground-state atom density and the Rydberg level, The simulation results are largely consistent with the measurements. The experiments, in which the principal quantum number is varied between 30 and 43, demonstrate that the EIT reduction observed at large Ωp is due to the strong interactions between the Rydberg atoms.
基金support from the National Key Research and Development Program of China(2017YFB0702800)the China Petrochemical Corporation(Sinopec Group)the National Natural Science Foundation of China(91434102 and U1663221)。
文摘Dry reforming of ethane(DRE)has received significant attention because of its potential to produce chemical raw materials and reduce carbon emissions.Herein,a composition-induced strong metal-support interaction(SMSI)effect over FeNi/Al-Ce-O catalysts is revealed via X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(TPR),and energy dispersive X-ray spectroscopy(EDS)elemental mapping.The introduction of Al into Al-Ce-O supports significantly influences the dispersion of surface active components and improves the catalytic performance for DRE over supported FeNi catalysts due to enhancement of the SMSI effect.The catalytic properties,for example,C_(2)H_(6) and CO_(2) conversion,CO selectivity and yield,and turnover frequencies(TOFs),of supported FeNi catalysts first increase and then decrease with increasing Al content,following the same trend as the theoretical effective surface area(TESA)of the corresponding catalysts.The FeNi/Ce-Al_(0.5) catalyst,with 50%Al content,exhibits the best DRE performance under steady-state conditions at 873 K.As observed by with in situ Fourier transform infrared spectroscopy(FTIR)analysis,the introduction of Al not only increases the content of surface Ce3+and oxygen vacancies but also promotes the dispersion of surface active components,which further alters the catalytic properties for DRE over supported FeNi catalysts.
文摘In this paper we study the interaction of strong and weak singularities for hyperbolic system of conservation laws in multidimensional space. Under the assumption of transversal intersect of the shock front with the bicharacteristics bearing weak singularities we proved a theorem on regularity propagation across the shock front.
基金the support from the National Natural Science Foundation of China(22376062)the Science and Technology Commission of Shanghai Municipality(22ZR1415700)+1 种基金Shanghai Rising-star Program(20QA1402400)and the Fundamental Research Funds for the Central Universities,Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology。
文摘The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous catalysis.Notably,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI formation.This emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.
基金Project supported by the Natural Science Basic Research Program of Shaanxi(Program Nos.2023KJXX-064 and 2021JQ-748)the National Natural Science Foundation of China(Grant Nos.11804213 and 12174238)Scientific Research Foundation of Shaanxi University of Technology(Grant No.SLGRCQD2006).
文摘We study the coexistence of antiferromagnetism and unconventional superconductivity on the Creutz lattice which shows strictly flat bands in the noninteracting regime.The famous renormalized mean-field theory is used to deal with strong electron-electron repulsive Hubbard interaction in the effective low-energy t-J model,the superfluid weight of the unconventional superconducting state has been calculated via the linear response theory.An unconventional superconducting state with both spin-singlet and staggered spin-triplet pairs emerges beyond a critical antiferromagnetic coupling interaction,while antiferromagnetism accompanies this state.The superconducting state with only spin-singlet pairs is dominant with paramagnetic phase.The A phase is analogous to the pseudogap phase,which shows that electrons go to form pairs but do not cause a supercurrent.We also show the superfluid behavior of the unconventional superconducting state and its critical temperature.It is proven directly that the flat band can effectively raise the critical temperature of superconductivity.It is implementable to simulate and control strongly-correlated electrons'behavior on the Creutz lattice in the ultracold atoms experiment or other artificial structures.Our results may help the understanding of the interplay between unconventional superconductivity and magnetism.
文摘Three Clifford algebras are sufficient to describe all interactions of modern physics: The Clifford algebra of the usual space is enough to describe all aspects of electromagnetism, including the quantum wave of the electron. The Clifford algebra of space-time is enough for electro-weak interactions. To get the gauge group of the standard model, with electro-weak and strong interactions, a third algebra is sufficient, with only two more dimensions of space. The Clifford algebra of space allows us to include also gravitation. We discuss the advantages of our approach.
文摘For the unification of gravitation with electromagnetism, weak and strong interactions, we use a unique and very simple framework, the Clifford algebra of space . We enlarge our previous wave equation to the general case, including all leptons, quarks and antiparticles of the first generation. The wave equation is a generalization of the Dirac equation with a compulsory non-linear mass term. This equation is form invariant under the group of the invertible elements in the space algebra. The form invariance is fully compatible with the gauge invariance of the standard model. The wave equations of the different particles come by Lagrange equations from a Lagrangian density and this Lagrangian density is the sum of the real parts of the wave equations. Both form invariance and gauge invariance are exact symmetries, not only partial or broken symmetries. Inertia is already present in the part of the gauge group and the inertial chiral potential vector simplifies weak interactions. Relativistic quantum physics is then a naturally yet unified theory, including all interactions.
基金financially supported by the National Natural Science Foundation of China for Youths(No.21601067,21701057)the China Postdoctoral Science Foundation(No.2020 M673037)a project funded by the Priority Academic Program Development of the Jiangsu Higher Education Institutions。
文摘The high cost,scarcity,and poor stability of precious-metal-based catalysts have hindered their extensive application in energy conversion and storage.This stimulates the search for earth-abundant alternatives to replace noble metal electrocatalysts.Hence,in this study,we investigate a novel and low-cost bifunctional electrocatalyst consisting of ZnCoMnO_(4) anchored on nitrogen-doped graphene oxide(ZnCoMnO_(4)/N-rGO).Benefiting from the strong Co-N interaction in ZnCoMnO_(4) and the coupled conductive N-rGO,the catalysts exhibit high electrocatalytic activity.Moreover,density functional theory calculations support the dominant role of the strong Co-N electronic interaction,which leads to ZnCoMnO_(4)/N-rGO having more favorable binding energies with O2 and H_(2) O,resulting in fast reaction kinetics.The obtained ZnCoMnO_(4)/N-rGO electrocatalyst exhibits superb bifunctional activity,with a half-wave potential of 0.83 V for the oxygen reduction reaction and a low onset potential of 1.57 V for the oxygen evolution reaction in 0.1 M KOH solution.Furthermore,a Zn-air battery driven by the ZnCoMnO_(4)/N-rGO catalyst shows remarkable discharge/charge performance,with a power density of 138.52 mW cm^(-2) and longterm cycling stability for 48 h.This work provides a promising multifunctional electrocatalyst based on non-noble metals for the storage and conversion of renewable energy.
基金National Science technology Support Plan Projects"(2012BAE06B00)
文摘TWC-equipped exhausts are widely used in gasoline-fueled vehicles to meet stringent emission regulations. The main components in TWCs are precious metals such as palladium (Pd), platinum (Pt), and rhodium (Rh) as the active component, and inorganic oxides such as γ-alumina (Al 2 O 3 ), ceria (CeO 2 ), zirconia (ZrO 2 ) and ceria-zirconia (CeO 2-ZrO 2 ) are used as the support. Interaction of precious metals and support plays an important role in the thermal stability and catalytic performance of TWCs. The support can improve the dispersion of precious metals and suppress the sintering of precious metals at high temperature. In the same, precious metals can also enhance the redox performance and oxygen storage capacity of support. This paper reviews the reaction phenomenon and mechanism of precious metals (Pt, Pd, Rh) and supports such as Al 2 O 3 , CeO 2-based composite oxides.
基金Project supported by the Fundamental Research Funds for the Cornell University(30919011220)the Key Project of Jiangsu Province Programs for Research and Development(BE2019115)+1 种基金Top-notch Academic Programs Project of Jiangsu Higher Education InstitutionsChina-Finland Industrial R&D Program(BZ2018015)。
文摘In this study,K_(x)-Mn-Ce catalysts prepared by sol-gel method were investigated for toluene oxidation.Compared with Mn-Ce,the catalytic performance of K_(x)-Mn-Ce was further improved.X-ray diffraction(XRD),high resolution transmission electron microscopy(HRTEM)and Raman analyses demonstrate that K ions enter the lattice of CeO_(2) and disperse uniformly.The results of X-ray photoelectron spectroscopy(XPS),H_(2)-temperature programmed reduction(H_(2)-TPR).and O_(2)-temperature programmed desorption(O_(2)-TPD)analyses indicate that there is a strong interaction between K,Mn and Ce;the charge co mpensation effect would be induced when K ions enter the lattice of CeO_(2),which leads to more oxygen vacancies due to the generation of more Ce^(3+).Toluene-TPD shows that K-doping enhances the activation ability of toluene.Among all catalysts,K0.1-Mn-Ce shows the highest concentration of Mn^(4+),Ce^(3+),Osur,and redox ability,resulting in higher low-temperature catalytic activity.Additionally,the results of stability and water resistance also prove that K0.1-Mn-Ce catalyst possesses excellent stability and water resistance.
基金supported by the National Natural Science Foundation of China revise to(Nos.22222504,92161124,and 52002165)the National Key Research and Development Program of China(No.2021YFA0717400)+4 种基金the Beijing National Laboratory for Molecular Sciences(No.BNLMS202013)the Guangdong Provincial Natural Science Foundation(No.2021A1515010229)the Shenzhen Basic Research Project(No.JCYJ20210324104808022)the Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)L.W.acknowledges the China Postdoctoral Science Foundation(No.2020M682764).
文摘For the high-temperature catalytic reaction,revealing the interface of catalyst–support and its evolution under reactive conditions is of crucial importance for understanding the reaction mechanism.However,much less is known about the atomic-scale interface of the hard-to-reduce silica-metal compared to that of reducible oxide systems.Here we reported the general behaviors of SiO_(2)migration onto various metal(Pt,Co,Rh,Pd,Ru,and Ni)nanocrystals supported on silica.Typically,the Pt/SiO_(2)catalytic system,which boosted the CO_(2)hydrogenation to CO,exhibited the reduction of Si0 at the Pt-SiO2 interface under H2 and further Si diffusion into the near surface of Pt nanoparticles,which was unveiled by in-situ environmental transmission electron microscopy coupled with spectroscopies.This reconstructed interface with Si diffused into Pt increased the sinter resistance of catalyst and thus improved the catalytic stability.The morphology of metal nanoparticles with SiO_(2)overlayer were dynamically evolved under reducing,vacuum,and oxidizing atmospheres,with a thicker SiO_(2)layer under oxidizing condition.The theoretical calculations revealed the mechanism that the Si-Pt surface provided synergistic sites for the activation of CO_(2)/H_(2)to produce CO with lower energy barriers,consequently boosting the high-temperature reverse water-gas shift reaction.These findings deepen the understanding toward the interface structure of inert oxide supported catalysts.
文摘Oxygen reduction reaction(ORR)is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced toOH−/H2Owhen receiving electrons.This reaction plays a crucial role in shaping the efficiency of both metal-air batteries and fuel cells,and precious metals are the dominant catalysts carrying out the ORR in their cathodes.However,how to manipulate the electronic structure of precious metals as active sites to further promote ORR performance and maximize the utilization rate is still under development.Metal oxide serves as suitable and promising support that can strongly interact with precious metals for both activity and durability enhancement.Herein,we present recent research updates on strong precious metal-metal oxide interaction(SPMMOI)utilized in ORR.We start by introducing the background of ORR,the issues to be solved,and its practical applications followed by a thorough discussion of the reaction mechanism and comprehensive evaluation protocols of performance.We then provide a complete understanding of theworking principle of SPMMOI and highlight the related advances.Finally,we summarize the merits of the precious metal-metal oxide systemand propose the research direction aswell as some urgent problems to be addressed in the future.
基金support from the National Natural Science Foundation of China(Nos.22138001 and 21521005)the National Key R&D Program of China(No.2017YFA0206804)is acknowledged.
文摘The direct conversion of ethanol to 1,1-diethoxyethane(DEE)through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and industry.Based on thermodynamics,the oxidative dehydrogenation of alcohol to acetaldehyde requires high temperature to activate oxygen to realize the C-H cleavage,while the acetalization of acetaldehyde with ethanol is exothermic reversible reaction favorable at low temperature.The mismatching of the reaction condition for the two consecutive steps makes it a great challenge to achieve both high ethanol conversion and high DEE selectivity.This work reports a highly efficient bi-functional catalysis by Bi/BiCeO_(x)for one-pot oxidative dehydrogenation-acetalization route from ethanol to DEE under 150℃and ambient pressure,affording a selectivity of 98.5%±0.5%to DEE at an ethanol conversion of 87.0%±1.0%.An efficient tandem catalysis has been achieved on the interfacial Bi^(δ)+-Ov-Ce^(III)sites in Bi/BiCeO_(x)established by strong metal-support interaction,in which Biδ+-Ov-sites contribute to the oxidative dehydrogenation of ethanol at mild temperature,and-Ov-CeIII sites to the subsequent acetalization between the generated acetaldehyde and ethanol.