Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

Dealuminated Hβ zeolite for selective conversion of fructose to furfural and formic acid

The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at433 K for 1 h in the γ-butyrolactone(GBL)-H_(2)O system, as well as the concomitant formation of 83.0% formic acid. The^(13)C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.

Oxygen functionalization-assisted anionic exchange toward unique construction of flower-like transition metal chalcogenide embedded carbon fabric for ultra-long life flexible energy storage and conversion

The metal-organic framework(MOF)derived Ni–Co–C–N composite alloys(NiCCZ)were“embedded”inside the carbon cloth(CC)strands as opposed to the popular idea of growing them upward to realize ultrastable energy storage and conversion application.The NiCCZ was then oxygen functionalized,facilitating the next step of stoichiometric sulfur anion diffusion during hydrothermal sulfurization,generating a flower-like metal hydroxysulfide structure(NiCCZOS)with strong partial implantation inside CC.Thus obtained NiCCZOS shows an excellent capacity when tested as a supercapacitor electrode in a three-electrode configuration.Moreover,when paired with the biomass-derived nitrogen-rich activated carbon,the asymmetric supercapacitor device shows almost 100%capacity retention even after 45,000 charge–discharge cycles with remarkable energy density(59.4 Wh kg^(-1)/263.8μWh cm^(–2))owing to a uniquely designed cathode.Furthermore,the same electrode performed as an excellent bifunctional water-splitting electrocatalyst with an overpotential of 271 mV for oxygen evolution reaction(OER)and 168.4 mV for hydrogen evolution reaction(HER)at 10 mA cm−2 current density along with 30 h of unhinged chronopotentiometric stability performance for both HER and OER.Hence,a unique metal chalcogenide composite electrode/substrate configuration has been proposed as a highly stable electrode material for flexible energy storage and conversion applications.

The impact of demographic dynamics on food consumption and its environmental outcomes:Evidence from China

With increasing population and changing demographics,food consumption has experienced a significant transition in quantity and quality.However,a dearth of knowledge remains regarding its environmental impacts and how it responds to demographic dynamics,particularly in emerging economies like China.Using the two-stage Quadratic Almost Demand System(QUAIDS)model,this study empirically examines the impact of demographic dynamics on food consumption and its environmental outcomes based on the provincial data from 2000 to 2020 in China.Under various scenarios,according to changes in demographics,we extend our analysis to project the long-term trend of food consumption and its environmental impacts,including greenhouse gas(GHG)emissions,water footprint(WF),and land appropriation(LA).The results reveal that an increase in the proportion of senior people significantly decreases the consumption of grain and livestock meat and increases the consumption of poultry,egg,and aquatic products,particularly for urban residents.Moreover,an increase in the proportion of males in the population leads to higher consumption of poultry and aquatic products.Correspondingly,in the current scenario of an increased aging population and sex ratio,it is anticipated that GHG emissions,WF,and LA are likely to decrease by 1.37,2.52,and 3.56%,respectively.More importantly,in the scenario adhering to the standards of nutritional intake according to the Dietary Guidelines for Chinese Residents in 2022,GHG emissions,WF,and LA in urban areas would increase by 12.78,20.94,and 18.32%,respectively.Our findings suggest that changing demographics should be considered when designing policies to mitigate the diet-environment-health trilemma and achieve sustainable food consumption.

A stable implicit nodal integration-based particle finite element method(N-PFEM)for modelling saturated soil dynamics

In this study,we present a novel nodal integration-based particle finite element method(N-PFEM)designed for the dynamic analysis of saturated soils.Our approach incorporates the nodal integration technique into a generalised Hellinger-Reissner(HR)variational principle,creating an implicit PFEM formulation.To mitigate the volumetric locking issue in low-order elements,we employ a node-based strain smoothing technique.By discretising field variables at the centre of smoothing cells,we achieve nodal integration over cells,eliminating the need for sophisticated mapping operations after re-meshing in the PFEM.We express the discretised governing equations as a min-max optimisation problem,which is further reformulated as a standard second-order cone programming(SOCP)problem.Stresses,pore water pressure,and displacements are simultaneously determined using the advanced primal-dual interior point method.Consequently,our numerical model offers improved accuracy for stresses and pore water pressure compared to the displacement-based PFEM formulation.Numerical experiments demonstrate that the N-PFEM efficiently captures both transient and long-term hydro-mechanical behaviour of saturated soils with high accuracy,obviating the need for stabilisation or regularisation techniques commonly employed in other nodal integration-based PFEM approaches.This work holds significant implications for the development of robust and accurate numerical tools for studying saturated soil dynamics.

Two-photon live imaging of direct glia-to-neuron conversion in the mouse cortex

Over the past decade,a growing number of studies have reported transcription factor-based in situ reprogramming that can directly conve rt endogenous glial cells into functional neurons as an alternative approach for n euro regeneration in the adult mammalian central ne rvous system.Howeve r,many questions remain regarding how a terminally differentiated glial cell can transform into a delicate neuron that forms part of the intricate brain circuitry.In addition,concerns have recently been raised around the absence of astrocyte-to-neuron conversion in astrocytic lineage-tra cing mice.In this study,we employed repetitive two-photon imaging to continuously capture the in situ astrocyte-to-neuron conversion process following ecto pic expression of the neural transcription factor NeuroD1 in both prolife rating reactive astrocytes and lineage-tra ced astrocytes in the mouse cortex.Time-lapse imaging over several wee ks revealed the ste p-by-step transition from a typical astrocyte with numero us short,tapered branches to a typical neuro n with a few long neurites and dynamic growth cones that actively explored the local environment.In addition,these lineage-converting cells were able to migrate ra dially or to ngentially to relocate to suitable positions.Furthermore,two-photon Ca2+imaging and patch-clamp recordings confirmed that the newly generated neuro ns exhibited synchronous calcium signals,repetitive action potentials,and spontaneous synaptic responses,suggesting that they had made functional synaptic connections within local neural circuits.In conclusion,we directly visualized the step-by-step lineage conversion process from astrocytes to functional neurons in vivo and unambiguously demonstrated that adult mammalian brains are highly plastic with respect to their potential for neuro regeneration and neural circuit reconstruction.

Semiclassical approach to spin dynamics of a ferromagnetic S = 1 chain

Motivated by recent experimental progress on the quasi-one-dimensional quantum magnet Ni Nb2O6, we study the spin dynamics of an S = 1 ferromagnetic Heisenberg chain with single-ion anisotropy by using a semiclassical molecular dynamics approach. This system undergoes a quantum phase transition from a ferromagnetic to a paramagnetic state under a transverse magnetic field, and the magnetic response reflecting this transition is well described by our semiclassical method.We show that at low temperature the transverse component of the dynamical structure factor depicts clearly the magnon dispersion, and the longitudinal component exhibits two continua associated with single-and two-magnon excitations,respectively. These spin excitation spectra show interesting temperature dependence as effects of magnon interactions. Our findings shed light on the experimental detection of spin excitations in a large class of quasi-one-dimensional magnets.

Ultrafast magneto-optical dynamics in nickel(111)single crystal studied by the integration of ultrafast reflectivity and polarimetry probes

With the integration of ultrafast reflectivity and polarimetry probes,we observed carrier relaxation and spin dynamics induced by ultrafast laser excitation of Ni(111)single crystals.The carrier relaxation time within the linear excitation range reveals that electron-phonon coupling and dissipation of photon energy into the bulk of the crystal take tens of picoseconds.On the other hand,the observed spin dynamics indicate a longer time of about 120 ps.To further understand how the lattice degree of freedom is coupled with these dynamics may require the integration of an ultrafast diffraction probe.

Finite Deformation, Finite Strain Nonlinear Dynamics and Dynamic Bifurcation in TVE Solids with Rheology

This paper presents a mathematical model consisting of conservation and balance laws (CBL) of classical continuum mechanics (CCM) and ordered rate constitutive theories in Lagrangian description derived using entropy inequality and the representation theorem for thermoviscoelastic solids (TVES) with rheology. The CBL and the constitutive theories take into account finite deformation and finite strain deformation physics and are based on contravariant deviatoric second Piola-Kirchhoff stress tensor and its work conjugate covariant Green’s strain tensor and their material derivatives of up to order m and n respectively. All published works on nonlinear dynamics of TVES with rheology are mostly based on phenomenological mathematical models. In rare instances, some aspects of CBL are used but are incorrectly altered to obtain mass, stiffness and damping matrices using space-time decoupled approaches. In the work presented in this paper, we show that this is not possible using CBL of CCM for TVES with rheology. Thus, the mathematical models used currently in the published works are not the correct description of the physics of nonlinear dynamics of TVES with rheology. The mathematical model used in the present work is strictly based on the CBL of CCM and is thermodynamically and mathematically consistent and the space-time coupled finite element methodology used in this work is unconditionally stable and provides solutions with desired accuracy and is ideally suited for nonlinear dynamics of TVES with memory. The work in this paper is the first presentation of a mathematical model strictly based on CBL of CCM and the solution of the mathematical model is obtained using unconditionally stable space-time coupled computational methodology that provides control over the errors in the evolution. Both space-time coupled and space-time decoupled finite element formulations are considered for obtaining solutions of the IVPs described by the mathematical model and are presented in the paper. Factors or the physics influencing dynamic response and dynamic bifurcation for TVES with rheology are identified and are also demonstrated through model problem studies. A simple model problem consisting of a rod (1D) of TVES material with memory fixed at one end and subjected to harmonic excitation at the other end is considered to study nonlinear dynamics of TVES with rheology, frequency response as well as dynamic bifurcation phenomenon.

1.42-fold enhancement of formate selectivity by linker conversion on the Zn-based metal organic framework catalyst

Electro-reduction of carbon dioxide(ERCO_(2)) is considered an effective method to alleviate the greenhouse effect and produce value-added chemicals.Achieving the dominant selectivity of Zn-based catalysts for formate remains a challenge.In this article,the ZnIn-E_(12) catalyst is successfully prepared by solvent assisted ligand exchange(SALE) method to convert organic ligands,achieving a Faradaic efficiency of 72.28% for formate at-1.26 V vs.RHE(V_(RHE)),which is 1.42 times higher than the original catalyst.Evidence shows that the successful conversion of organic ligands can transform the catalyst from the original large size polyhedron to cross-linked network of particles with a diameter of about 30 nm.The increased specific surface area can expose more active sites and facilitate the electrocatalytic conversion of CO_(2) to formate.This work is expected to provide inspiration for the regulation of formate selectivity and catalyst size in Zn-based catalysts.

Hollow Metal-Organic Framework/MXene/Nanocellulose Composite Films for Giga/Terahertz Electromagnetic Shielding and Photothermal Conversion

With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.

Intrinsic polarization conversion and avoided-mode crossing in X-cut lithium niobate microrings

Compared with well-developed free space polarization converters, polarization conversion between TE and TM modes in the waveguide is generally considered to be caused by shape birefringence, like curvature, morphology of waveguide cross section and scattering. Here, we study the polarization conversion mechanism in 1-THz-FSR X-cut lithium niobate microrings with multiple-resonance condition, that is the conversion can be implemented by birefringence of waveguides,which will also introduce an avoided-mode crossing. In the experiment, we find that this mode crossing results in severe suppression of one sideband in local nondegenerate four-wave mixing and disrupts the cascaded four-wave mixing on this side. Simultaneously, we propose one two-dimensional method to simulate the eigenmodes(TE and TM) in X-cut microrings, and the mode crossing point. This work will provide one approach to the design of polarization converters and simulation for monolithic photonics integrated circuits, and may be helpful to the studies of missed temporal dissipative soliton formation in X-cut lithium niobate rings.

Ab initio nonadiabatic molecular dynamics study on spin–orbit coupling induced spin dynamics in ferromagnetic metals

Understanding the photoexcitation induced spin dynamics in ferromagnetic metals is important for the design of photo-controlled ultrafast spintronic device.In this work,by the ab initio nonadiabatic molecular dynamics simulation,we have studied the spin dynamics induced by spin–orbit coupling(SOC)in Co and Fe using both spin-diabatic and spin-adiabatic representations.In Co system,it is found that the Fermi surface(E_(F))is predominantly contributed by the spin-minority states.The SOC induced spin flip will occur for the photo-excited spin-majority electrons as they relax to the E_(F),and the spin-minority electrons tend to relax to the EFwith the same spin through the electron–phonon coupling(EPC).The reduction of spin-majority electrons and the increase of spin-minority electrons lead to demagnetization of Co within100 fs.By contrast,in Fe system,the E_(F) is dominated by the spin-majority states.In this case,the SOC induced spin flip occurs for the photo-excited spin-minority electrons,which leads to a magnetization enhancement.If we move the E_(F) of Fe to higher energy by 0.6eV,the E_(F) will be contributed by the spin-minority states and the demagnetization will be observed again.This work provides a new perspective for understanding the SOC induced spin dynamics mechanism in magnetic metal systems.

Insight into structure evolution of carbon nitrides and its energy conversion as luminescence

A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.

Theoretical and experimental investigation of the resonance responses and chaotic dynamics of a bistable laminated composite shell in the dynamic snap-through mode

The dynamic model of a bistable laminated composite shell simply supported by four corners is further developed to investigate the resonance responses and chaotic behaviors.The existence of the 1:1 resonance relationship between two order vibration modes of the system is verified.The resonance response of this class of bistable structures in the dynamic snap-through mode is investigated,and the four-dimensional(4D)nonlinear modulation equations are derived based on the 1:1 internal resonance relationship by means of the multiple scales method.The Hopf bifurcation and instability interval of the amplitude frequency and force amplitude curves are analyzed.The discussion focuses on investigating the effects of key parameters,e.g.,excitation amplitude,damping coefficient,and detuning parameters,on the resonance responses.The numerical simulations show that the foundation excitation and the degree of coupling between the vibration modes exert a substantial effect on the chaotic dynamics of the system.Furthermore,the significant motions under particular excitation conditions are visualized by bifurcation diagrams,time histories,phase portraits,three-dimensional(3D)phase portraits,and Poincare maps.Finally,the vibration experiment is carried out to study the amplitude frequency responses and bifurcation characteristics for the bistable laminated composite shell,yielding results that are qualitatively consistent with the theoretical results.

Recent advances in core-shell organic framework-based photocatalysts for energy conversion and environmental remediation

Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materials developed as photocatalysts,the core-shell metal/covalent-organic framework(MOF or COF)photocatalysts have garnered significant attention due to their highly porous structure and the adjustability in both structure and functionality.The existing reviews on core-shell organic framework photocatalytic materials have mainly focused on core-shell MOF materials.However,there is still a lack of indepth reviews specifically addressing the photocatalytic performance of core-shell COFs and MOFs@COFs.Simultaneously,there is an urgent need for a comprehensive review encompassing these three types of core-shell structures.Based on this,this review aims to provide a comprehensive understanding and useful guidelines for the exploration of suitable core-shell organic framework photocatalysts towards appropriate photocatalytic energy conversion and environmental governance.Firstly,the classification,synthesis,formation mechanisms,and reasonable regulation of core-shell organic framework were summarized.Then,the photocatalytic applications of these three kinds of core-shell structures in different areas,such as H_(2)evolution,CO_(2)reduction,and pollutants degradation are emphasized.Finally,the main challenges and development prospects of core-shell organic framework photocatalysts were introduced.This review aims to provide insights into the development of a novel generation of efficient and stable core-shell organic framework materials for energy conversion and environmental remediation.

Mitochondrial recruitment in myelin:an anchor for myelin dynamics and plasticity?

Optimal propagation of neuronal electrical impulses depends on the insulation of axons by myelin,produced in the central nervous system by oligodendrocytes.Myelin is an extension of the oligodendrocyte plasma membrane,which wraps around an axon to form a compact multi-layered sheath.Myelin is composed of a substantially higher proportion of lipids compared to other biological membranes and enriched in a small number of specialized proteins.

Community structure and species diversity dynamics of a subtropical evergreen broad-leaved forest in China:2005 to 2020

Here,we characterize the temporal and spatial dynamics of forest community structure and species diversity in a subtropical evergreen broad-leaved forest in China.We found that community structure in this forest changed over a 15-year period.Specifically,renewal and death of common species was large,with the renewal of individuals mainly concentrated within a few populations,especially those of Aidia canthioides and Cryptocarya concinna.The numbers of individual deaths for common species were concentrated in the small and mid-diameter level.The spatial distribution of community species diversity fluctuated in each monitoring period,showing a more dispersed diversity after the 15-year study period,and the coefficient of variation on quadrats increased.In 2010,the death and renewal of the community and the spatial variation of species diversity were different compared to other survey years.Extreme weather may have affected species regeneration and community stability in our subtropical monsoon evergreen broad-leaved forests.Our findings suggest that strengthening the monitoring and management of the forest community will help better understand the long-and short-term causes of dynamic fluctuations of community structure and species diversity,and reveal the factors that drive changes in community structure.

Conformational dynamics as an intrinsic determinant of prion protein misfolding and neurotoxicity

The prion protein(PrP) is the key molecular and pathological mediator of prion diseases,a heterogeneous group of brain disorders with fatal outcomes.Prion diseases are rare but deserve special attention because of their unique familial,sporadic,and transmissible etiologies,all caused by a single agent:misfolded conformations of PrP.

Target layer state estimation in multi-layer complex dynamical networks considering nonlinear node dynamics

In many engineering networks, only a part of target state variables are required to be estimated.On the other hand,multi-layer complex network exists widely in practical situations.In this paper, the state estimation of target state variables in multi-layer complex dynamical networks with nonlinear node dynamics is studied.A suitable functional state observer is constructed with the limited measurement.The parameters of the designed functional observer are obtained from the algebraic method and the stability of the functional observer is proven by the Lyapunov theorem.Some necessary conditions that need to be satisfied for the design of the functional state observer are obtained.Different from previous studies, in the multi-layer complex dynamical network with nonlinear node dynamics, the proposed method can estimate the state of target variables on some layers directly instead of estimating all the individual states.Thus, it can greatly reduce the placement of observers and computational cost.Numerical simulations with the three-layer complex dynamical network composed of three-dimensional nonlinear dynamical nodes are developed to verify the effectiveness of the method.