Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via lo...Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.展开更多
This research aims to study the bio-adsorption process of two dyes,Cibacron Green H3G(CG-H3G)and Terasil Red(TR),in a single system and to bring them closer to the industrial textile discharge by a binary mixture of t...This research aims to study the bio-adsorption process of two dyes,Cibacron Green H3G(CG-H3G)and Terasil Red(TR),in a single system and to bring them closer to the industrial textile discharge by a binary mixture of two dyes(TR+CG-H3G).The Cockle Shell(CS)was used as a natural bio-adsorbent.The characterizations of CS were investigated by Fourier transform infrared(FTIR),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy-dispersive X-ray spectroscopy(EDX)and Brunauer–Emmett–Teller(BET).The adsorption potential of Cockle Shells was tested in two cases(single and binary system)and determined by:contact time(0–60 min),bio-adsorption dose(3–15 g/L),initial concentration(10–300 mg/L),temperature(22–61°C)and pH solution(2–12).The study of bio-adsorption(equilibrium and kinetics)was conducted at 22°C.The kinetic studies demon-strated that a pseudo-second-order adsorption mechanism had a good correlation coefficient(R2≥0.999).The Langmuir isotherm modeling provided a well-defined description of TR and CG-H3G bio-adsorption on cockle shells,exhibiting maximum capacities of 29.41 and 3.69 mg/g respectively at 22°C.The thermodynamic study shows that the reaction between the TR,CG-H3G dyes molecules and the bio-adsorbent is exothermic,spontaneous in the range of 22–31°C with the aleatory character decrease at the solid-liquid interface.The study of selectivity in single and binary systems has been performed under optimal operating conditions using the industrial textile rejection pH(pH=6.04).CG-H3G dye is found to have a higher selectivity than TR in single(0–60 min)and binary systems with a range of 6–45 min,as shown by the selectivity measurement.It was discovered that CS has the capability to remove both CG-H3G and TR dyes in both simple and binary systems,making it a superior bio-adsorbent.展开更多
The potential of 2-amino-1-propanol(AP)as a novel depressant in selectively floating ilmenite from titanaugite under weakly acidic conditions was investigated.Micro-flotation results show that AP significantly reduces...The potential of 2-amino-1-propanol(AP)as a novel depressant in selectively floating ilmenite from titanaugite under weakly acidic conditions was investigated.Micro-flotation results show that AP significantly reduces the recovery of titanaugite while having no evident impact on ilmenite flotation.Subsequent bench-scale flotation tests further confirm a remarkable improvement in separation efficiency upon the introduction of AP.Contact angle and adsorption tests reveal a stronger affinity of AP towards the titanaugite surface in comparison to ilmenite.Zeta potential measurements and X-ray photoelectron spectroscopy(XPS)analyses exhibit favorable adsorption characteristics of AP on titanaugite,resulting from a synergy of electrostatic attraction and chemical interaction.In contrast,electrostatic repulsion hinders any significant interaction between AP and the ilmenite surface.These findings highlight the potential of AP as a highly efficient depressant for ilmenite flotation,paving the way for reduced reliance on sulfuric acid in the industry.展开更多
Radioactive microspheres have demonstrated excellent therapeutic effects and good tolerance in the treatment of unresectable primary and secondary liver malignancies.This is attributed to precise embolization and pote...Radioactive microspheres have demonstrated excellent therapeutic effects and good tolerance in the treatment of unresectable primary and secondary liver malignancies.This is attributed to precise embolization and potent anti-tumor effect.However,certain limitations such as unstable loading,perfusion stasis,heterogeneous distribution,ectopic distribution,and insufficient dosage,restrict their clinical application.Herein,a novel personalized Y-90 carbon microsphere with high uniformity,high specific activity and high availability(^(90)Y-HUACM)is presented.It is synthesized through planar molecular complex adsorption and chemical deposition solidification.^(90)Y-HUACM exhibited controllable size,excellent biocompatibility,outstanding in vitro and in vivo stability.The radiolabeling efficiency of Y-90 exceeded 99%and the leaching rate of Y-90 is far below 0.1%.Furthermore,the excellent anti-tumor effect,nuclide loading stability,anti-reflux characteristics,precise embolization,and biosafety of^(90)Y-HUACM were validated in a rabbit VX2liver tumor model.In summary,this new,high-performance,and customizable radioactive microsphere provides a superior choice for selective internal radiation treatment of advanced liver cancer is expected to be rapidly applied in clinical practice.展开更多
Base-catalyzed nucleophilic substitution reactions ofβ-ketonitrile with azodicarboxylates have been developed.A series of disubstituted C—N coupling products were obtained in good to excellent yields under Et_(3)N c...Base-catalyzed nucleophilic substitution reactions ofβ-ketonitrile with azodicarboxylates have been developed.A series of disubstituted C—N coupling products were obtained in good to excellent yields under Et_(3)N catalysis.Monosubstitu-tion C—N bond formation reaction catalyzed by K_(2)CO_(3) also gave novel enol-based target products.This method is simple and mild,with good chemoselectivity,excellent substrate compatibility and tolerance for various functional groups,and achieves gram-scale synthesis.The reaction is a nucleophilic substitution process without the involvement of free radicals.展开更多
ZGH401 alloy was prepared under varying laser power levels and scanning speeds by the orthogonal test method using selective laser melting(SLM).The effect of different energy densities on microstructure and mechanical...ZGH401 alloy was prepared under varying laser power levels and scanning speeds by the orthogonal test method using selective laser melting(SLM).The effect of different energy densities on microstructure and mechanical properties of the formed alloy was investigated.The microstructure of ZGH401 was analyzed by scanning electron microscope,electron back-scattered diffraction,and electron probe microanalysis.The results show that the defects of the as-built ZGH401 are gradually reduced,the relative density is correspondingly enhanced with increasing the energy density,and the ultimate density can reach 99.6%.An increase in laser power leads to a corresponding rise in hardness of ZGH401,while a faster scanning speed reduces the residual stress in asbuilt ZGH401 samples.In addition,better tensile properties are achieved at room temperature due to more grain boundaries perpendicular to the build direction than parallel to the build direction.The precipitated phases are identified as carbides and Laves phases via chemical composition analysis,with fewer carbides observed at the molten pool boundaries than within the molten pools.展开更多
We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of ...We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.展开更多
The elimination of the vertical tail in tailless aircraft results in a significant decrease in heading static stability,causing substantial coupling among the three control channels.In addition,in specific operational...The elimination of the vertical tail in tailless aircraft results in a significant decrease in heading static stability,causing substantial coupling among the three control channels.In addition,in specific operational scenarios,the tailless aircraft is prone to electromagnetic interference,leading to the generation of high-frequency noise and consequently compromising their control performance.To address these issues,a decoupling control method based on a fractional-order error extended state observer(FOEESO)is proposed.A nonlinear model of a tailless aircraft with thrust vectoring capabilities is first developed.The decoupling control design for the three control channels is then implemented using FOEESO,with the asymptotic convergence conditions outlined.The proposed method is evaluated through simulations and compared to coupled control and linear extended state observer(LESO)techniques.Numerical simulations demonstrate that the FOEESO-based control methodology achieves effective decoupling,exhibiting 6.9%and 11.7%reductions in integral absolute error(IAE)relative to LESO under nominal operational conditions and critical fault scenarios,respectively.These improvements thereby highlight FOEESO’s capability to enhance closed-loop stability and tracking precision in tailless aircraft control systems.展开更多
Planar positioning systems are widely utilized in micro and nano applications.The challenges in modeling and control of XYΘflexure-based mechanisms include hysteresis of the piezoelectric actuators,couplings among th...Planar positioning systems are widely utilized in micro and nano applications.The challenges in modeling and control of XYΘflexure-based mechanisms include hysteresis of the piezoelectric actuators,couplings among the input axes,and coupled linear and angular motions of the end effector.This paper presents an inverse hysteresis-coupling hybrid model to account for such hysteresis and couplings.First,a specially designed kinematic chain is adopted to transfer the pose of the end effector into the linear motions at three prismatic joints.Second,an inverse hysteresis-coupling hybrid model is developed to linearize and decouple the system via a multilayer feedforward neural network.A fractional-order PID controller is also integrated to improve the motion accuracy of the overall system.Experimental results demonstrate that the proposed method can accurately control the motion of the end effector with improved accuracy and robustness.展开更多
Dynamical decoupling(DD),usually implemented by sophisticated sequences of instantaneous control pulses,is a well-established quantum control technique for quantum information and quantum sensing.In practice,the pulse...Dynamical decoupling(DD),usually implemented by sophisticated sequences of instantaneous control pulses,is a well-established quantum control technique for quantum information and quantum sensing.In practice,the pulses are inevitably imperfect with many systematic errors that may influence the performances of DD.In particular,Rabi error and detuning are primary systemic errors arising from finite pulse duration,incorrect time control,and frequency instability.Here,we propose a phase-modulated DD with staggered global phases for the basic units of the pulse sequences to suppress these systemic errors.By varying the global phases appended to the pulses in the dynamical decoupling unit alternatively with 0 orπ,our protocol can significantly reduce the influences of Rabi error and detuning.Our protocol is general and can be combined with the most existing DD sequences such as universal DD,knill DD,XY,etc.As an example,we further apply our method to quantum lock-in detection for measuring time-dependent alternating signals.Our study paves the way for a simple and feasible way to realize robust dynamical decoupling sequences,which can be applicable for various quantum sensing scenarios.展开更多
Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving fac...Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving factors at both the generation and treatment stages of SO_(2),more effective targeted mitigation strategies can be developed.We employ the Tapio decoupling model and propose a two-stage method to examine the decoupling issues related to SO_(2).Our findings indicate that:①DEI shows a steady and significant improvement,with SO_(2)emission intensity identified as the primary driver.②for the decoupling of economic growth and SO_(2)generation,energy scale serves as the largest stimulator,while the effect of energy intensity changes from negative to positive,and pollution intensity is first positive and then negative.③For the decoupling of SO_(2)generation and SO_(2)removal,treatment efficiency leads as the largest promoter,followed by treatment intensity.Based on these results,this study recommends that China focuses more on enhancing clean energy utilization and the effectiveness of treatment processes.展开更多
The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively red...The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively reduce C=C or C=O bonds while preserving other functional groups within the molecule.This approach serves as a critical strategy for the directional synthesis of high-value molecules.However,achieving such selectivity remains challenging due to the thermodynamic equilibrium and kinetic competition between C=O and C=C bonds inα,β-unsaturated systems.Consequently,constructing precisely targeted catalytic systems is essential to overcome these limitations,offering both fundamental scientific significance and industrial application potential.Metal-organic frameworks(MOFs)and their derivatives have emerged as innovative platforms for designing such systems,owing to their programmable topology,tunable pore microenvironments,spatially controllable active sites,and modifiable electronic structures.This review systematically summarizes the research progress of MOF-based catalysts for selec-tive hydrogenation ofα,β-unsaturated aldehydes/ketones in the last decade,with emphasis on the design strategy,conformational relationship,and catalytic mechanism,aiming to provide new ideas for the design of targeted catalyt-ic systems for the selective hydrogenation ofα,β-unsaturated aldehydes/ketones.展开更多
The progress from intelligent interactions requires electronic skin(E-skin)to shift from single-functional perception to multisensory capabilities.However,the intuitive and interference-free reading of multiple sensor...The progress from intelligent interactions requires electronic skin(E-skin)to shift from single-functional perception to multisensory capabilities.However,the intuitive and interference-free reading of multiple sensory signals without involving complex algorithms is a critical challenge.Herein,we propose a flexible multisensory E-skin by developing a highly homogeneous dispersion of BaTiO_(3)nanoparticles in polydimethylsiloxane dielectric layer.The E-skin is sensitive to externally applied pressure as well as temperature and can distinguish dual synergetic stimuli by the time decoupling effect.The pressure and temperature perception was achieved in an individual device,which greatly reduced the structural complexity compared with multifunctional integrated devices.The sensitivity of E-skin for pressure detection is as high as 0.0724 kPa^(−1)and the detection range reaches as wide as 15.625-10 MPa.The sensitivity to temperature detection is as high as−1.34℃^(−1)and the detection range reaches 20-200℃.More importantly,by equipping with a multilayer neural network,the evolution from tactile perception to advanced intelligent tactile cognition is demonstrated.展开更多
Against the backdrop of regional coordinated development and China’s“dual carbon”strategic objectives,the Beijing-Tianjin-Hebei(BTH)region faces an urgent need to transition fromits traditional economic growth mode...Against the backdrop of regional coordinated development and China’s“dual carbon”strategic objectives,the Beijing-Tianjin-Hebei(BTH)region faces an urgent need to transition fromits traditional economic growth model,which is heavily reliant on resource consumption.This study investigates the decoupling dynamics among economic growth,energy consumption,and carbon emissions in the BTH region,along with the underlying driving forces,aiming to provide valuable insights for achieving the“dual carbon”targets and fostering high-quality regional development.First,the Tapio decoupling model is employed to analyze the decoupling relationships between economic growth,energy consumption,and carbon emissions in the BTH region from 2000 to 2021.Second,the Logarithmic Mean Divisia Index decomposition method is applied to identify the key driving factors of carbon emission reduction and quantify their respective contributions.Finally,targeted policy recommendations are proposed based on the empirical findings to support regional coordinated development.The results indicate that(1)all three sub-regions within the BTH region have demonstrated consistent improvements in energy utilization efficiency and a gradual decline in carbon emission intensity,although the degree of progress varies across regions;(2)differentiated decoupling states exist between carbon emissions and both economic growth and energy consumption,with Beijing showing significant decoupling,while Tianjin and Hebei Province experience a“rebound”phenomenon following a phase of decoupling;(3)energy consumption intensity and industrial structure optimization have notably positive effects on carbon emission reduction,whereas other factors contribute to varying degrees to the exacerbation of carbon emissions;(4)the impacts of driving factors on carbon emissions exhibit significant spatio-temporal disparities.Based on these findings,the study recommends enhancing fiscal incentives,optimizing industrial structures,improving energy efficiency,and establishing a coordinated regional governance framework to facilitate the BTH region’s low-carbon transition and sustainable development.展开更多
Quantifying material use in infrastructure development and analyzing its relationship with economic growth is essential for enhancing resource efficiency and steering regional resource management toward sustainable de...Quantifying material use in infrastructure development and analyzing its relationship with economic growth is essential for enhancing resource efficiency and steering regional resource management toward sustainable development.This study systematically assessed infrastructure related material use in 30 provinces,autonomous regions,and municipalities in China during 1978-2022.The result indicated that material stock has experienced significant growth,increasing from 16.91×10^(9)t in 1978 to 103.60×10^(9)t in 2022,with an average annual growth rate of 4.20%.However,from 1978 to 2015,material input followed a strong upward trend but saturated after 2015.At the national level,material input peaked in 2015,after which it began to decline.The central region reached its peak earlier in 2013,while the eastern and western regions peaked in 2015.Using a decoupling analysis framework,this study revealed that nationally,the elasticity value between material stock and gross domestic product(GDP)remained near or above 1.0,reflecting continued reliance on stock accumulation.Regionally,the elasticity value between material stock and GDP has increased in the central and western regions during 1978-2022,whereas elasticity value between material stock and GDP in the eastern region showed a slower growth rate but still struggled to achieve absolute decoupling.Moreover,the elasticity value between material input and GDP has declined at the national level,presenting a relative decoupling,with some regions already achieving absolute decoupling.The eastern region was closer to absolute decoupling,while the central and western regions,though still intensive in material input,exhibited faster declines in elasticity.Accelerating the transition from linear to circular economy is an essential step for China to achieve absolute decoupling and long-term sustainability.Finally,this research recommends promoting the adoption of renewable energy,driving industrial upgrading,implementing compact urban design,and extending the lifespan of infrastructure to reduce material dependency and achieve sustainable infrastructure transformation at the national level.展开更多
Compared with natural enzymes, nanozymes have the advantages of high stability and low cost;however,selectivity and sensitivity are key issues that prevent their further development. In this study, we report a cascade...Compared with natural enzymes, nanozymes have the advantages of high stability and low cost;however,selectivity and sensitivity are key issues that prevent their further development. In this study, we report a cascade nanozymatic system with significantly improved selectivity and sensitivity that combines more substrate-specific reactions and sensitive fiuorescence detection. Taking detection of ascorbic acid(AA)as an example, a cascade catalytic reaction system consisting of oxidase-like N-doped carbon nanocages(NC) and peroxidase-like copper oxide(Cu O) improved the reaction selectivity in transforming the substrate into the target product by more than 1200 times against the interference of uric acid. The cascade catalytic reaction system was also applicable for transfer from open reactors into a spatially confined microfiuidic device, increasing the slope of the calibration curves by approximately 1000-fold with a linear detection range of 2.5 nmol/L to 100 nmol/L and a low limit of detection of 0.77 nmol/L. This work offers a new strategy that achieves significant improvements in selectivity and sensitivity.展开更多
The environment-friendly and efficient selective separation of chalcopyrite and molybdenite poses a challenge in mineral pro-cessing.In this study,gum Arabic(GA)was initially proposed as a novel depressant for the sel...The environment-friendly and efficient selective separation of chalcopyrite and molybdenite poses a challenge in mineral pro-cessing.In this study,gum Arabic(GA)was initially proposed as a novel depressant for the selective separation of molybdenite from chalcopyrite during flotation.Microflotation results indicated that the inhibitory capacity of GA was stronger toward molybdenite than chalcopyrite.At pH 8.0 with 20 mg/L GA addition,the recovery rate of chalcopyrite in the concentrate obtained from mixed mineral flota-tion was 67.49%higher than that of molybdenite.Furthermore,the mechanism of GA was systematically investigated by various surface characterization techniques.Contact angle tests indicated that after GA treatment,the hydrophobicity of the molybdenite surface signifi-cantly decreased,but that of the chalcopyrite surface showed no apparent change.Fourier transform-infrared spectroscopy and X-ray photoelectron spectroscopy revealed a weak interaction force between GA and chalcopyrite.By contrast,GA was primarily adsorbed onto the molybdenite surface through chemical chelation,with possible contributions from hydrogen bonding and hydrophobic interactions.Pre-adsorbed GA could prevent butyl xanthate from being adsorbed onto molybdenite.Scanning electron microscopy–energy-dispersive spectrometry further indicated that GA was primarily adsorbed onto the“face”of molybdenite rather than the“edge.”Therefore,GA could be a promising molybdenite depressant for the flotation separation of Cu–Mo.展开更多
The photocatalytic selective oxidation of biomass-derived 5-hydroxymethylfurfural(HMF)offers a sustainable alternative to thermal catalysis.However,the efficiency of this process is significantly limited by inadequate...The photocatalytic selective oxidation of biomass-derived 5-hydroxymethylfurfural(HMF)offers a sustainable alternative to thermal catalysis.However,the efficiency of this process is significantly limited by inadequate light absorption efficiency and the rapid recombination of photogenerated charge carriers in conventional photocatalysts.Herein,we developed a Co_(3)O_(4)/ZnIn_(2)S_(4)(Co_(3)O_(4)/ZIS)photocatalyst,in which Co_(3)O_(4)functions as a multifunctional cocatalyst.This photocatalyst significantly enhances the chemisorption and activation of HMF molecules through interfacial oxygen-hydroxyl interactions.Additionally,the incorporation of narrow-band gap Co_(3)O_(4)broadens the optical absorption range of the composite photocatalyst.Besides,integrating Co_(3)O_(4)with ZnIn_(2)S_(4)leads to a 5.9-fold increase in charge separation efficiency compared to pristine ZnIn_(2)S_(4).The optimized Co_(3)O_(4)/ZIS-3 photocatalyst(3 wt% Co_(3)O_(4)loading)exhibits exceptional selectivity and yield for 2,5-diformylfuran(DFF)under visible light irradiation,achieving 70.4%DFF selectivity with a 5.4-fold enhancement compared to pristine ZnIn_(2)S_(4).Scavenger experiments and electron spin resonance(ESR)spectroscopy indicate that superoxide radicals(O_(2)^(-))and h^(+)are the main active species driving the photocatalytic oxidation of HMF.Molecular simulations reveal that the activation of HMF and the transformation of the intermediate^(*)MF to^(*)DFF are more favorable over the Co_(3)O_(4)/ZIS composite due to lower activation barriers compared to those over ZnIn_(2)S_(4).Through this work,we aim to design highly efficient and affordable photocatalysts for biomass valorization and contribute valuable insights into the mechanisms of photocatalytic oxidation of HMF.展开更多
A control strategy of repetitive control without inductorance decoupling was proposed to address the problem of high total harmonic distortion(THD)rate of the network-side current caused by the reduced stability of th...A control strategy of repetitive control without inductorance decoupling was proposed to address the problem of high total harmonic distortion(THD)rate of the network-side current caused by the reduced stability of the rectifier module of the DC charging pile under weak grid as well as the dead zone and nonlinearity of switching devices during charging.Firstly,the parallel repetitive control was constructed in the inner current loop,and the proportional-integral(PI)+repetitive controller based on parallel structure was designed.For system compensation,a second-order low-pass filter was selected to correct the system,and the network-side current harmonics were actively suppressed without increasing the filtering device,which effectively improves the quality of grid-connected current.Secondly,based on the synthetic vector method,the controller parameters were designed to realize the elimination of main pole by establishing two synchronous rotation coordinate system vector differential equations,so as to realize the inductanceless decoupling to cope with the influence of network-side inductance fluctuation on the stability of the control system under weak grid.By theoretical analysis and simulation,the proposed control strategy was embedded into the self-developed digital signal processor for the rectifier module of DC charging pile,simulated dynamic and steady-state operation experiments were conducted,and comparative analysis was performed to prove the feasibility of the proposed control strategy.展开更多
The hydroformylation of olefins,known as the"oxo reaction",involves the use of syngas(CO/H_(2))to produce aldehyde with an additional carbon atom.However,side reactions such as the isomerization or hydrogena...The hydroformylation of olefins,known as the"oxo reaction",involves the use of syngas(CO/H_(2))to produce aldehyde with an additional carbon atom.However,side reactions such as the isomerization or hydrogenation of olefins often result in unexpected products and other by-products.Recent efforts in developing efficient ligands represent the most effective approach to addressing these challenges.In this study,we described a Bis-OPNN phosphorus ligand facilitated Rh-catalyzed hydroformylation with a high degree of linear selectivity across various olefins.Under mild conditions,a broad range of olefins were efficiently converted into linear aldehydes with high yields and excellent regioselectivity.The protocol also showed impressive functional group tolerance and was successfully applied to modify drugs and natural products,including the total synthesis of(±)-crispine A.Preliminary mechanistic studies revealed that this Bis-OPNN phosphorus ligand anchoring the rhodium catalyst is crucial for controlling the linear selectivity.展开更多
基金the National Nature Science Foundation of China for Excellent Young Scientists Fund(32222058)Fundamental Research Foundation of CAF(CAFYBB2022QB001).
文摘Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.
基金supported by the University Salah Boubnider-Constantine 3 (Algeria).
文摘This research aims to study the bio-adsorption process of two dyes,Cibacron Green H3G(CG-H3G)and Terasil Red(TR),in a single system and to bring them closer to the industrial textile discharge by a binary mixture of two dyes(TR+CG-H3G).The Cockle Shell(CS)was used as a natural bio-adsorbent.The characterizations of CS were investigated by Fourier transform infrared(FTIR),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy-dispersive X-ray spectroscopy(EDX)and Brunauer–Emmett–Teller(BET).The adsorption potential of Cockle Shells was tested in two cases(single and binary system)and determined by:contact time(0–60 min),bio-adsorption dose(3–15 g/L),initial concentration(10–300 mg/L),temperature(22–61°C)and pH solution(2–12).The study of bio-adsorption(equilibrium and kinetics)was conducted at 22°C.The kinetic studies demon-strated that a pseudo-second-order adsorption mechanism had a good correlation coefficient(R2≥0.999).The Langmuir isotherm modeling provided a well-defined description of TR and CG-H3G bio-adsorption on cockle shells,exhibiting maximum capacities of 29.41 and 3.69 mg/g respectively at 22°C.The thermodynamic study shows that the reaction between the TR,CG-H3G dyes molecules and the bio-adsorbent is exothermic,spontaneous in the range of 22–31°C with the aleatory character decrease at the solid-liquid interface.The study of selectivity in single and binary systems has been performed under optimal operating conditions using the industrial textile rejection pH(pH=6.04).CG-H3G dye is found to have a higher selectivity than TR in single(0–60 min)and binary systems with a range of 6–45 min,as shown by the selectivity measurement.It was discovered that CS has the capability to remove both CG-H3G and TR dyes in both simple and binary systems,making it a superior bio-adsorbent.
基金supported by the National Key Research and Development Program of China(No.2019YFC1803501)the National Natural Science Foundation of China(No.52074357)+2 种基金the Natural Science Foundation of Hunan Province,China(No.2022JJ30713)the Vanadium Titanium Union Foundationthe Project of Technology Innovation Center for Comprehensive Utilization of Strategic Mineral Resources,Ministry of Natural Resources,China。
文摘The potential of 2-amino-1-propanol(AP)as a novel depressant in selectively floating ilmenite from titanaugite under weakly acidic conditions was investigated.Micro-flotation results show that AP significantly reduces the recovery of titanaugite while having no evident impact on ilmenite flotation.Subsequent bench-scale flotation tests further confirm a remarkable improvement in separation efficiency upon the introduction of AP.Contact angle and adsorption tests reveal a stronger affinity of AP towards the titanaugite surface in comparison to ilmenite.Zeta potential measurements and X-ray photoelectron spectroscopy(XPS)analyses exhibit favorable adsorption characteristics of AP on titanaugite,resulting from a synergy of electrostatic attraction and chemical interaction.In contrast,electrostatic repulsion hinders any significant interaction between AP and the ilmenite surface.These findings highlight the potential of AP as a highly efficient depressant for ilmenite flotation,paving the way for reduced reliance on sulfuric acid in the industry.
基金supported by the National Major Scientific and Technological Special Project for“Significant New Drugs Development”(No.2018ZX09201018–028)the nuclear energy development projects of China during the 13thFive Year Plan periodthe key research and development project of the Sichuan Provincial Department of Science and Technology(No.18ZDYF1466)。
文摘Radioactive microspheres have demonstrated excellent therapeutic effects and good tolerance in the treatment of unresectable primary and secondary liver malignancies.This is attributed to precise embolization and potent anti-tumor effect.However,certain limitations such as unstable loading,perfusion stasis,heterogeneous distribution,ectopic distribution,and insufficient dosage,restrict their clinical application.Herein,a novel personalized Y-90 carbon microsphere with high uniformity,high specific activity and high availability(^(90)Y-HUACM)is presented.It is synthesized through planar molecular complex adsorption and chemical deposition solidification.^(90)Y-HUACM exhibited controllable size,excellent biocompatibility,outstanding in vitro and in vivo stability.The radiolabeling efficiency of Y-90 exceeded 99%and the leaching rate of Y-90 is far below 0.1%.Furthermore,the excellent anti-tumor effect,nuclide loading stability,anti-reflux characteristics,precise embolization,and biosafety of^(90)Y-HUACM were validated in a rabbit VX2liver tumor model.In summary,this new,high-performance,and customizable radioactive microsphere provides a superior choice for selective internal radiation treatment of advanced liver cancer is expected to be rapidly applied in clinical practice.
文摘Base-catalyzed nucleophilic substitution reactions ofβ-ketonitrile with azodicarboxylates have been developed.A series of disubstituted C—N coupling products were obtained in good to excellent yields under Et_(3)N catalysis.Monosubstitu-tion C—N bond formation reaction catalyzed by K_(2)CO_(3) also gave novel enol-based target products.This method is simple and mild,with good chemoselectivity,excellent substrate compatibility and tolerance for various functional groups,and achieves gram-scale synthesis.The reaction is a nucleophilic substitution process without the involvement of free radicals.
基金National Defense Science and Technology Project Management Center(2021-JCJQ-JJ-0092)。
文摘ZGH401 alloy was prepared under varying laser power levels and scanning speeds by the orthogonal test method using selective laser melting(SLM).The effect of different energy densities on microstructure and mechanical properties of the formed alloy was investigated.The microstructure of ZGH401 was analyzed by scanning electron microscope,electron back-scattered diffraction,and electron probe microanalysis.The results show that the defects of the as-built ZGH401 are gradually reduced,the relative density is correspondingly enhanced with increasing the energy density,and the ultimate density can reach 99.6%.An increase in laser power leads to a corresponding rise in hardness of ZGH401,while a faster scanning speed reduces the residual stress in asbuilt ZGH401 samples.In addition,better tensile properties are achieved at room temperature due to more grain boundaries perpendicular to the build direction than parallel to the build direction.The precipitated phases are identified as carbides and Laves phases via chemical composition analysis,with fewer carbides observed at the molten pool boundaries than within the molten pools.
文摘We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.
文摘The elimination of the vertical tail in tailless aircraft results in a significant decrease in heading static stability,causing substantial coupling among the three control channels.In addition,in specific operational scenarios,the tailless aircraft is prone to electromagnetic interference,leading to the generation of high-frequency noise and consequently compromising their control performance.To address these issues,a decoupling control method based on a fractional-order error extended state observer(FOEESO)is proposed.A nonlinear model of a tailless aircraft with thrust vectoring capabilities is first developed.The decoupling control design for the three control channels is then implemented using FOEESO,with the asymptotic convergence conditions outlined.The proposed method is evaluated through simulations and compared to coupled control and linear extended state observer(LESO)techniques.Numerical simulations demonstrate that the FOEESO-based control methodology achieves effective decoupling,exhibiting 6.9%and 11.7%reductions in integral absolute error(IAE)relative to LESO under nominal operational conditions and critical fault scenarios,respectively.These improvements thereby highlight FOEESO’s capability to enhance closed-loop stability and tracking precision in tailless aircraft control systems.
基金supported in part by the Open Fund of State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment,Guangdong University of Technology(Grant No.JMDZ2021007)in part by the Guangdong International Cooperation Program of Science and Technology(Grant No.2022A0505050078).
文摘Planar positioning systems are widely utilized in micro and nano applications.The challenges in modeling and control of XYΘflexure-based mechanisms include hysteresis of the piezoelectric actuators,couplings among the input axes,and coupled linear and angular motions of the end effector.This paper presents an inverse hysteresis-coupling hybrid model to account for such hysteresis and couplings.First,a specially designed kinematic chain is adopted to transfer the pose of the end effector into the linear motions at three prismatic joints.Second,an inverse hysteresis-coupling hybrid model is developed to linearize and decouple the system via a multilayer feedforward neural network.A fractional-order PID controller is also integrated to improve the motion accuracy of the overall system.Experimental results demonstrate that the proposed method can accurately control the motion of the end effector with improved accuracy and robustness.
基金Project supported by the National Key Research and Development Program of China(Grant No.2022YFA1404104)the National Natural Science Foundation of China(Grant Nos.92476201,12025509,12305022,and 12475029)+1 种基金the Key-Area Research and Development Program of Guangdong Province,China(Grant No.2019B030330001)Guangdong Provincial Quantum Science Strategic Initiative Fund(Grant Nos.GDZX2305006 and GDZX2405002)。
文摘Dynamical decoupling(DD),usually implemented by sophisticated sequences of instantaneous control pulses,is a well-established quantum control technique for quantum information and quantum sensing.In practice,the pulses are inevitably imperfect with many systematic errors that may influence the performances of DD.In particular,Rabi error and detuning are primary systemic errors arising from finite pulse duration,incorrect time control,and frequency instability.Here,we propose a phase-modulated DD with staggered global phases for the basic units of the pulse sequences to suppress these systemic errors.By varying the global phases appended to the pulses in the dynamical decoupling unit alternatively with 0 orπ,our protocol can significantly reduce the influences of Rabi error and detuning.Our protocol is general and can be combined with the most existing DD sequences such as universal DD,knill DD,XY,etc.As an example,we further apply our method to quantum lock-in detection for measuring time-dependent alternating signals.Our study paves the way for a simple and feasible way to realize robust dynamical decoupling sequences,which can be applicable for various quantum sensing scenarios.
基金the National Natural Science Foundation of China[Grant No.52270183].
文摘Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving factors at both the generation and treatment stages of SO_(2),more effective targeted mitigation strategies can be developed.We employ the Tapio decoupling model and propose a two-stage method to examine the decoupling issues related to SO_(2).Our findings indicate that:①DEI shows a steady and significant improvement,with SO_(2)emission intensity identified as the primary driver.②for the decoupling of economic growth and SO_(2)generation,energy scale serves as the largest stimulator,while the effect of energy intensity changes from negative to positive,and pollution intensity is first positive and then negative.③For the decoupling of SO_(2)generation and SO_(2)removal,treatment efficiency leads as the largest promoter,followed by treatment intensity.Based on these results,this study recommends that China focuses more on enhancing clean energy utilization and the effectiveness of treatment processes.
文摘The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively reduce C=C or C=O bonds while preserving other functional groups within the molecule.This approach serves as a critical strategy for the directional synthesis of high-value molecules.However,achieving such selectivity remains challenging due to the thermodynamic equilibrium and kinetic competition between C=O and C=C bonds inα,β-unsaturated systems.Consequently,constructing precisely targeted catalytic systems is essential to overcome these limitations,offering both fundamental scientific significance and industrial application potential.Metal-organic frameworks(MOFs)and their derivatives have emerged as innovative platforms for designing such systems,owing to their programmable topology,tunable pore microenvironments,spatially controllable active sites,and modifiable electronic structures.This review systematically summarizes the research progress of MOF-based catalysts for selec-tive hydrogenation ofα,β-unsaturated aldehydes/ketones in the last decade,with emphasis on the design strategy,conformational relationship,and catalytic mechanism,aiming to provide new ideas for the design of targeted catalyt-ic systems for the selective hydrogenation ofα,β-unsaturated aldehydes/ketones.
基金Ningbo Scientific and Technological Innovation 2025 Major Project,Grant/Award Number:2020Z022German Research Foundation(DFG)grants,Grant/Award Numbers:MA 5144/13-1,MA 5144/28-1+6 种基金the National Natural Science Foundation of China,Grant/Award Numbers:62204246,51931011,51971233,52127803,62174165the External Cooperation Program of Chinese Academy of Sciences,Grant/Award Numbers:174433KYSB20190038,174433KYSB20200013the Instrument Developing Project of the Chinese Academy of Sciences,Grant/Award Number:YJKYYQ20200030K.C.Wong Education Foundation,Grant/Award Number:GJTD-2020-11Chinese Academy of Sciences Youth Innovation Promotion Association,Grant/Award Number:2018334Zhejiang Provincial Key R&D Program,Grant/Award Numbers:2021C01183,2022C01032the National Natural Science Foundation of Zhejiang Province of China,Grant/Award Number:LQ23F040004.
文摘The progress from intelligent interactions requires electronic skin(E-skin)to shift from single-functional perception to multisensory capabilities.However,the intuitive and interference-free reading of multiple sensory signals without involving complex algorithms is a critical challenge.Herein,we propose a flexible multisensory E-skin by developing a highly homogeneous dispersion of BaTiO_(3)nanoparticles in polydimethylsiloxane dielectric layer.The E-skin is sensitive to externally applied pressure as well as temperature and can distinguish dual synergetic stimuli by the time decoupling effect.The pressure and temperature perception was achieved in an individual device,which greatly reduced the structural complexity compared with multifunctional integrated devices.The sensitivity of E-skin for pressure detection is as high as 0.0724 kPa^(−1)and the detection range reaches as wide as 15.625-10 MPa.The sensitivity to temperature detection is as high as−1.34℃^(−1)and the detection range reaches 20-200℃.More importantly,by equipping with a multilayer neural network,the evolution from tactile perception to advanced intelligent tactile cognition is demonstrated.
基金funded by the Science and Technology Project of State Grid Corporation of China(No.52018F240002)the National Natural Science Foundation of China(72403087)the National Natural Science Foundation of China(72173043).
文摘Against the backdrop of regional coordinated development and China’s“dual carbon”strategic objectives,the Beijing-Tianjin-Hebei(BTH)region faces an urgent need to transition fromits traditional economic growth model,which is heavily reliant on resource consumption.This study investigates the decoupling dynamics among economic growth,energy consumption,and carbon emissions in the BTH region,along with the underlying driving forces,aiming to provide valuable insights for achieving the“dual carbon”targets and fostering high-quality regional development.First,the Tapio decoupling model is employed to analyze the decoupling relationships between economic growth,energy consumption,and carbon emissions in the BTH region from 2000 to 2021.Second,the Logarithmic Mean Divisia Index decomposition method is applied to identify the key driving factors of carbon emission reduction and quantify their respective contributions.Finally,targeted policy recommendations are proposed based on the empirical findings to support regional coordinated development.The results indicate that(1)all three sub-regions within the BTH region have demonstrated consistent improvements in energy utilization efficiency and a gradual decline in carbon emission intensity,although the degree of progress varies across regions;(2)differentiated decoupling states exist between carbon emissions and both economic growth and energy consumption,with Beijing showing significant decoupling,while Tianjin and Hebei Province experience a“rebound”phenomenon following a phase of decoupling;(3)energy consumption intensity and industrial structure optimization have notably positive effects on carbon emission reduction,whereas other factors contribute to varying degrees to the exacerbation of carbon emissions;(4)the impacts of driving factors on carbon emissions exhibit significant spatio-temporal disparities.Based on these findings,the study recommends enhancing fiscal incentives,optimizing industrial structures,improving energy efficiency,and establishing a coordinated regional governance framework to facilitate the BTH region’s low-carbon transition and sustainable development.
基金supported by the Shanghai Committee of Science and Technology Fund(22ZR1419300)the Academic Year 2025 Ritsumeikan Asia Pacific University Academic Research Subsidy(Grants-in-Aid Reapplication Type).
文摘Quantifying material use in infrastructure development and analyzing its relationship with economic growth is essential for enhancing resource efficiency and steering regional resource management toward sustainable development.This study systematically assessed infrastructure related material use in 30 provinces,autonomous regions,and municipalities in China during 1978-2022.The result indicated that material stock has experienced significant growth,increasing from 16.91×10^(9)t in 1978 to 103.60×10^(9)t in 2022,with an average annual growth rate of 4.20%.However,from 1978 to 2015,material input followed a strong upward trend but saturated after 2015.At the national level,material input peaked in 2015,after which it began to decline.The central region reached its peak earlier in 2013,while the eastern and western regions peaked in 2015.Using a decoupling analysis framework,this study revealed that nationally,the elasticity value between material stock and gross domestic product(GDP)remained near or above 1.0,reflecting continued reliance on stock accumulation.Regionally,the elasticity value between material stock and GDP has increased in the central and western regions during 1978-2022,whereas elasticity value between material stock and GDP in the eastern region showed a slower growth rate but still struggled to achieve absolute decoupling.Moreover,the elasticity value between material input and GDP has declined at the national level,presenting a relative decoupling,with some regions already achieving absolute decoupling.The eastern region was closer to absolute decoupling,while the central and western regions,though still intensive in material input,exhibited faster declines in elasticity.Accelerating the transition from linear to circular economy is an essential step for China to achieve absolute decoupling and long-term sustainability.Finally,this research recommends promoting the adoption of renewable energy,driving industrial upgrading,implementing compact urban design,and extending the lifespan of infrastructure to reduce material dependency and achieve sustainable infrastructure transformation at the national level.
基金supported by the National Natural Science Foundation of China (Nos. 22174014 and 22074015)。
文摘Compared with natural enzymes, nanozymes have the advantages of high stability and low cost;however,selectivity and sensitivity are key issues that prevent their further development. In this study, we report a cascade nanozymatic system with significantly improved selectivity and sensitivity that combines more substrate-specific reactions and sensitive fiuorescence detection. Taking detection of ascorbic acid(AA)as an example, a cascade catalytic reaction system consisting of oxidase-like N-doped carbon nanocages(NC) and peroxidase-like copper oxide(Cu O) improved the reaction selectivity in transforming the substrate into the target product by more than 1200 times against the interference of uric acid. The cascade catalytic reaction system was also applicable for transfer from open reactors into a spatially confined microfiuidic device, increasing the slope of the calibration curves by approximately 1000-fold with a linear detection range of 2.5 nmol/L to 100 nmol/L and a low limit of detection of 0.77 nmol/L. This work offers a new strategy that achieves significant improvements in selectivity and sensitivity.
基金supported by the National Key Research and Development Program of China(Nos.2022YFC2904502 and 2022YFC2904501)the Major Science and Technology Projects in Yunnan Province,China(No.202202AB080012).
文摘The environment-friendly and efficient selective separation of chalcopyrite and molybdenite poses a challenge in mineral pro-cessing.In this study,gum Arabic(GA)was initially proposed as a novel depressant for the selective separation of molybdenite from chalcopyrite during flotation.Microflotation results indicated that the inhibitory capacity of GA was stronger toward molybdenite than chalcopyrite.At pH 8.0 with 20 mg/L GA addition,the recovery rate of chalcopyrite in the concentrate obtained from mixed mineral flota-tion was 67.49%higher than that of molybdenite.Furthermore,the mechanism of GA was systematically investigated by various surface characterization techniques.Contact angle tests indicated that after GA treatment,the hydrophobicity of the molybdenite surface signifi-cantly decreased,but that of the chalcopyrite surface showed no apparent change.Fourier transform-infrared spectroscopy and X-ray photoelectron spectroscopy revealed a weak interaction force between GA and chalcopyrite.By contrast,GA was primarily adsorbed onto the molybdenite surface through chemical chelation,with possible contributions from hydrogen bonding and hydrophobic interactions.Pre-adsorbed GA could prevent butyl xanthate from being adsorbed onto molybdenite.Scanning electron microscopy–energy-dispersive spectrometry further indicated that GA was primarily adsorbed onto the“face”of molybdenite rather than the“edge.”Therefore,GA could be a promising molybdenite depressant for the flotation separation of Cu–Mo.
基金financially supported by the National Key Research and Development Program of China(No.2022YFB3805400)the National Natural Science Foundation of China(No.22178297,No.22478327)+3 种基金the Science and Technology Innovation Program of Hunan Province(No.2024RC9009)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDC04010100)the Provincial Natural Science Foundation of Hunan(No.2024JJ5371)the Scientific Research Fund of Hunan Provincial Education Department(No.24A0107)。
文摘The photocatalytic selective oxidation of biomass-derived 5-hydroxymethylfurfural(HMF)offers a sustainable alternative to thermal catalysis.However,the efficiency of this process is significantly limited by inadequate light absorption efficiency and the rapid recombination of photogenerated charge carriers in conventional photocatalysts.Herein,we developed a Co_(3)O_(4)/ZnIn_(2)S_(4)(Co_(3)O_(4)/ZIS)photocatalyst,in which Co_(3)O_(4)functions as a multifunctional cocatalyst.This photocatalyst significantly enhances the chemisorption and activation of HMF molecules through interfacial oxygen-hydroxyl interactions.Additionally,the incorporation of narrow-band gap Co_(3)O_(4)broadens the optical absorption range of the composite photocatalyst.Besides,integrating Co_(3)O_(4)with ZnIn_(2)S_(4)leads to a 5.9-fold increase in charge separation efficiency compared to pristine ZnIn_(2)S_(4).The optimized Co_(3)O_(4)/ZIS-3 photocatalyst(3 wt% Co_(3)O_(4)loading)exhibits exceptional selectivity and yield for 2,5-diformylfuran(DFF)under visible light irradiation,achieving 70.4%DFF selectivity with a 5.4-fold enhancement compared to pristine ZnIn_(2)S_(4).Scavenger experiments and electron spin resonance(ESR)spectroscopy indicate that superoxide radicals(O_(2)^(-))and h^(+)are the main active species driving the photocatalytic oxidation of HMF.Molecular simulations reveal that the activation of HMF and the transformation of the intermediate^(*)MF to^(*)DFF are more favorable over the Co_(3)O_(4)/ZIS composite due to lower activation barriers compared to those over ZnIn_(2)S_(4).Through this work,we aim to design highly efficient and affordable photocatalysts for biomass valorization and contribute valuable insights into the mechanisms of photocatalytic oxidation of HMF.
基金supported by National Natural Science Foundation of China(No.61903291)Shaanxi Province Key R&D Program(No.2022GY-134)。
文摘A control strategy of repetitive control without inductorance decoupling was proposed to address the problem of high total harmonic distortion(THD)rate of the network-side current caused by the reduced stability of the rectifier module of the DC charging pile under weak grid as well as the dead zone and nonlinearity of switching devices during charging.Firstly,the parallel repetitive control was constructed in the inner current loop,and the proportional-integral(PI)+repetitive controller based on parallel structure was designed.For system compensation,a second-order low-pass filter was selected to correct the system,and the network-side current harmonics were actively suppressed without increasing the filtering device,which effectively improves the quality of grid-connected current.Secondly,based on the synthetic vector method,the controller parameters were designed to realize the elimination of main pole by establishing two synchronous rotation coordinate system vector differential equations,so as to realize the inductanceless decoupling to cope with the influence of network-side inductance fluctuation on the stability of the control system under weak grid.By theoretical analysis and simulation,the proposed control strategy was embedded into the self-developed digital signal processor for the rectifier module of DC charging pile,simulated dynamic and steady-state operation experiments were conducted,and comparative analysis was performed to prove the feasibility of the proposed control strategy.
基金financial support from the National Key Research and Development Program of China(No.2021YFF0600704).
文摘The hydroformylation of olefins,known as the"oxo reaction",involves the use of syngas(CO/H_(2))to produce aldehyde with an additional carbon atom.However,side reactions such as the isomerization or hydrogenation of olefins often result in unexpected products and other by-products.Recent efforts in developing efficient ligands represent the most effective approach to addressing these challenges.In this study,we described a Bis-OPNN phosphorus ligand facilitated Rh-catalyzed hydroformylation with a high degree of linear selectivity across various olefins.Under mild conditions,a broad range of olefins were efficiently converted into linear aldehydes with high yields and excellent regioselectivity.The protocol also showed impressive functional group tolerance and was successfully applied to modify drugs and natural products,including the total synthesis of(±)-crispine A.Preliminary mechanistic studies revealed that this Bis-OPNN phosphorus ligand anchoring the rhodium catalyst is crucial for controlling the linear selectivity.
