Photocatalysis is an important technology for using solar energy to produce hydrogen,convert CO_(2) to synthetic fuels,and decrease persistent pollutant.However,conventional photocatalysts have limitations,including p...Photocatalysis is an important technology for using solar energy to produce hydrogen,convert CO_(2) to synthetic fuels,and decrease persistent pollutant.However,conventional photocatalysts have limitations,including poor spectral absorption,inefficient charge separation,and structural instability under operational stress,which demand innovative durable materials with tailored electronic properties.Nanodiamond(ND)has recently been recognized as a suitable material because of its exceptional chemical stability,superior charge carrier mobility,and possible surface functionalization.While its intrinsic wide bandgap limits its response to visible-light,different methods have been demonstrated to activate its catalytic potential.Here,several emerging strategies for improving the catalytic performance of ND-based photocatalytic systems are summarized,including surface functionalization,plasmonic hybridization,heteroatom doping,and heterostructure design.And the structure-activity relationship and design principle are proposed to improve the light harvesting,charge transport,and redox kinetics for constructing high efficiency ND-based photocatalysts used in the renewable energy and environmental industries.展开更多
CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organ...CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.展开更多
To synergistically recover alumina and alkali from red mud(RM),the structural stability and conversion mechanism of hydroandradite(HA)from hydrogarnet(HG)were investigated via the First-principles,XRF,XRD,PSD and SEM ...To synergistically recover alumina and alkali from red mud(RM),the structural stability and conversion mechanism of hydroandradite(HA)from hydrogarnet(HG)were investigated via the First-principles,XRF,XRD,PSD and SEM methods,and a novel hydrothermal process based on the conversion principle was finally proposed.The crystal structure simulation shows that the HA with varied silicon saturation coefficients is more stable than HG,and the HA with a high iron substitution coefficient is more difficult to be converted from HG.The(110)plane of Fe_(2)O_(3) is easier to combine with HG to form HA,and the binding energy is 81.93 kJ/mol.The effects of raw material ratio,solution concentration and hydrothermal parameters on the conversion from HG to HA were revealed,and the optimal conditions for the alumina recovery were obtained.The recovery efficiencies of alumina and Na_(2)O from the RM are 63.06%and 97.34%,respectively,and the Na_(2)O content in the treated RM is only 0.13%.展开更多
Catalytic CO_(2)-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis.Single-atom catalysts(SACs)with maximized atomic utilization,tai...Catalytic CO_(2)-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis.Single-atom catalysts(SACs)with maximized atomic utilization,tailored electronic configurations and unique metal-support interactions,exhibit superior performance in CO_(2) activation and methanol synthesis.This review systematically compares reaction mechanisms and pathways across thermal,photocatalytic and electrocatalytic systems,emphasizing structure-activity relationships governed by active sites,coordination microenvironments and support functionalities.Through case studies of representative SACs,we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity.A critical analysis of reaction parameters(e.g.,temperature,pressure)reveals condition-dependent catalytic behaviors in thermal system,with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps.While thermal catalysis achieves industrially viable methanol yields,the scalability is constrained by energy-intensive operation and catalyst sintering.Conversely,photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations.To address the challenges,we propose strategic research priorities on precise design of active sites,synergy of multiple technological pathways,development of intelligent catalytic systems and diverse CO_(2) feedstock compatibility.These insights establish a framework for developing next-generation SACs,offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.展开更多
Two-dimensional nanofluidic membranes have garnered considerable interest due to their potential for cost-effective osmotic energy harvesting.One promising approach to enhancing ion conductivity and selectivity is the...Two-dimensional nanofluidic membranes have garnered considerable interest due to their potential for cost-effective osmotic energy harvesting.One promising approach to enhancing ion conductivity and selectivity is the incorporation of vip additives.However,the traditional host-vip configuration can undermine the structural integrity of nanochannels owing to the inconsistent size and shape of these additives.Drawing inspiration from the intricate design of biological protein channels,which utilize small amino acid molecules as vips,we have addressed this issue by incorporating glycine,a common amino acid,into a vermiculite membrane using a simple vacuum-assisted infiltration method.The resulting vermiculite-glycine membrane demonstrates 1.8 times greater ionic conductivity and twice the power density compared to pure vermiculite membranes.Analysis based on glycine content,coupled with spectroscopic examination,reveals that ion conductivity is linked to the distribution of glycine molecules across three specific sites within the membrane.This suggests that glycine molecules—whether confined in voids,adsorbed onto nanochannel surfaces,or intercalated within multilayered vermiculite nanoparticles—enhance nanofluidic ion transport by modulating surface and space charge density,as well as strengthening hydrogen bonding,electrostatic interactions,and steric effects.This work reveals the specific interactions between amino acids and vermiculite,offering a novel path for advancing nanofluidic composite membranes and highlighting critical considerations for the proposed strategy.展开更多
Conventional locking/release mechanisms often face challenges in aircraft wing separation processes,such as excessive impact loads and insufficient synchronization.These may cause structural damage to the airframe or ...Conventional locking/release mechanisms often face challenges in aircraft wing separation processes,such as excessive impact loads and insufficient synchronization.These may cause structural damage to the airframe or attitude instability,seriously compromising mission reliability.To address this engineering challenge,this paper proposes a multi-point low-impact locking/release mechanism based on the mobility model and energy conversion strategy.Through establishing a DOF constraint framework system,this paper systematically analyzes the energy transfer and conversion characteristics during the wing separation process,reveals the generation mechanism of impact loads,and conducts research on low-impact design based on energy conversion strategy.Building on this foundation,a single-point locking/release mechanism employing parallel trapezoidal key shaft structure was designed,which increases frictional contact time and reduces the energy release rate,thereby achieving low-impact characteristics.The mechanism's performance was validated through physical prototype development and systematic functional testing(including unlocking force,synchronization,and impact tests).Experimental results demonstrate:(1)Under 14 kN preload condition,the maximum unlocking force was only 92.54 N,showing a linear relationship with preload that satisfies the"strong-connection/weak-unlock"design requirement;(2)Wing separation was completed within 46 ms,with synchronization time difference among three separation mechanisms stably controlled within 12-14 ms,proving rapid and reliable operation;(3)The unlocking impact acceleration ranged between 26 and 73 g,below the 100 g design limit,confirming the effectiveness of the energy conversion strategy.The proposed low-impact locking/release mechanism design method based on energy conversion strategy resolves the traditional challenges of high impact and synchronization deficiencies.The synergistic optimization mechanism of"structural load reduction and performance improvement"provides a highly reliable technical solution for wing separable mechanisms while offering novel design insights for wing connection/separation systems engineering.展开更多
As a controllable power generation method requiring no energy storage,Ocean Thermal Energy Conversion(OTEC)technology demonstrates characteristics of abundant reserves,low pollution,and round-the-clock stable operatio...As a controllable power generation method requiring no energy storage,Ocean Thermal Energy Conversion(OTEC)technology demonstrates characteristics of abundant reserves,low pollution,and round-the-clock stable operation.The free-standing cold-water pipe(CWP)in the system withstands various complex loads during operation,posing potential failure risks.To reveal the deformation and stress mechanisms of OTEC CWPs,this study first analyzes wave particle velocity and acceleration to determine wave loads at different water depths.Based on the Euler-Bernoulli beam model,a quasi-static load calculation model for OTEC CWPs was established.The governing equations were discretized using the finite difference method,and matrix equations were solved to analyze bending deformation,bending moments,and surface stresses at discrete points along the pipe.Results indicate that water depths within 50 m represent a critical zone where wave particle velocity,acceleration,and wave loads exhibit significant variations in harmonic patterns,while beyond 50 m depth wave loads decrease linearly.Ocean currents and surface wind-driven currents substantially influence the CWP’s lateral displacement.Considering the effect of clump weights,the maximum lateral displacement occurs at 600–800 m below sea level.Utilizing large-wall-thickness high-strength pipes at the top section significantly enhances the structural safety of the CWP system.展开更多
Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O cr...Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.展开更多
Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active ...Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active intermediate for hydrocarbon synthesis.Despite significant progress in methanol-to-hydrocarbon(MTH)conversion,a comprehensive understanding of reaction mechanisms remains essential to enhance catalyst design and industrial applicability.This review critically synthesizes recent advances in mechanistic insights related to methanol conversion and methanol-mediated catalytic processes.Firstly,we systematically outline key reaction pathways involved in initial carbon–carbon(C–C)bond formation through direct and indirect mechanisms,emphasizing significant breakthroughs from spectroscopic analyses and theoretical calculations.Subsequently,we highlight the autocatalytic characteristics and dual-cycle mechanisms underlying MTH processes,critically evaluating the roles of zeolite structures,pore sizes,topology,and acidity in governing product selectivity and catalyst stability.Additionally,we discuss cutting-edge developments in tandem catalytic systems employing methanol as a pivotal intermediate for CO_(x)hydrogenation,emphasizing the transferable mechanistic principles and catalytic insights.Finally,we identify future research directions,including elucidating precise hydrocarbon pool(HCP)intermediates,optimizing zeolite structures through computational-guided design,and developing robust catalytic systems leveraging advanced characterization methods and artificial intelligence.By integrating multidisciplinary approaches from catalytic science,materials engineering,and reaction engineering,this review provides actionable guidance towards rational design and optimization of advanced catalytic systems for efficient methanol conversion processes.展开更多
Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders....Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.展开更多
The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the p...The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the prognosis for ICC remains poor.Owing to the high degree of malignancy and insidious onset of ICC,numerous cases are detected at intermediate or advanced stages of the disease,hence eliminating the chance for surgical intervention.Moreover,because of the highly invasive characteristics of ICC,recurrence and metastasis postresection are prevalent,leading to a 5-year survival rate of only 20%-35%following surgery.In the past decade,different methods of treatment have been investigated,including transarterial chemoembolization,transarterial radioembolization,radiotherapy,systemic therapy,and combination therapies.For certain patients with advanced ICC,conversion treatment may be utilized to facilitate surgical resection and manage disease progression.This review summarizes the definition of downstaging conversion treatment and presents the clinical experience and evidence concerning conversion treatment for advanced ICC.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor m...Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor micro-LED displays.However,the impact of solvent on both the printing process and the morphology of SIJ-printed PNC color conversion microstructures remains underexplored.In this study,we prepared samples of CsPbBr3PNC colloid inks in various solvents and investigated the solvent's impact on SIJ printed PNC microstructures.Our findings reveal that the boiling point of the solvent is crucial to the SIJ printing process of PNC colloid inks.Only does the boiling point of the solvent fall in the optimal range,the regular positioned,micron-scaled,conical PNC microstructures can be successfully printed.Below this optimal range,the ink is unable to be ejected from the nozzle;while above this range,irregular positioned microstructures with nanoscale height and coffee-ring-like morphology are produced.Based on these observations,high-resolution color conversion PNC microstructures were effectively prepared using SIJ printing of PNC colloid ink dispersed in dimethylbenzene solvent.展开更多
Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increase...Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increased applications of plasma technology in the field of multiscale functional materials'preparation,with a number of interesting results.This review will begin by introducing the basic knowledge of plasma,including the definition,typical parameters,and classification of plasma setups.Following this,we will provide a comprehensive review and summary of the applications(phase conversion,doping,deposition,etching,exfoliation,and surface treatment)of plasma in common energy conversion and storage systems,such as electrocatalytic conversion of small molecules,batteries,fuel cells,and supercapacitors.This article summarizes the structure-performance relationships of electrochemical energy conversion and storage materials(ECSMs)that have been prepared or modified by plasma.It also provides an overview of the challenges and perspectives of plasma technology,which could lead to a new approach for designing and modifying electrode materials in ECSMs.展开更多
Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and ca...Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.展开更多
Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity ar...Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity are also tunable,increasing its functional versatility.These make diamond and its related materials,such as its composites,highly promising for various applications in energy fields.This review summarizes recent advances and key achievements in energy storage and conversion,covering electrochemical energy storage(e.g.,batteries and supercapacitors),electrocatalytic energy conversion(e.g.,CO_(2)and nitrogen reduction reactions),and solar energy conversion(e.g.,photo-(electro)chemical CO_(2)and nitrogen reduction reactions,and solar cells).Current challenges and prospects related to the synthesis of diamond materials and the technologies for their energy applications are outlined and discussed.展开更多
文摘Photocatalysis is an important technology for using solar energy to produce hydrogen,convert CO_(2) to synthetic fuels,and decrease persistent pollutant.However,conventional photocatalysts have limitations,including poor spectral absorption,inefficient charge separation,and structural instability under operational stress,which demand innovative durable materials with tailored electronic properties.Nanodiamond(ND)has recently been recognized as a suitable material because of its exceptional chemical stability,superior charge carrier mobility,and possible surface functionalization.While its intrinsic wide bandgap limits its response to visible-light,different methods have been demonstrated to activate its catalytic potential.Here,several emerging strategies for improving the catalytic performance of ND-based photocatalytic systems are summarized,including surface functionalization,plasmonic hybridization,heteroatom doping,and heterostructure design.And the structure-activity relationship and design principle are proposed to improve the light harvesting,charge transport,and redox kinetics for constructing high efficiency ND-based photocatalysts used in the renewable energy and environmental industries.
文摘CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.
基金the financial support from the National Key R&D Program of China(No.2022YFC2904405)the National Natural Science Foundation of China(Nos.22078055,51774079)。
文摘To synergistically recover alumina and alkali from red mud(RM),the structural stability and conversion mechanism of hydroandradite(HA)from hydrogarnet(HG)were investigated via the First-principles,XRF,XRD,PSD and SEM methods,and a novel hydrothermal process based on the conversion principle was finally proposed.The crystal structure simulation shows that the HA with varied silicon saturation coefficients is more stable than HG,and the HA with a high iron substitution coefficient is more difficult to be converted from HG.The(110)plane of Fe_(2)O_(3) is easier to combine with HG to form HA,and the binding energy is 81.93 kJ/mol.The effects of raw material ratio,solution concentration and hydrothermal parameters on the conversion from HG to HA were revealed,and the optimal conditions for the alumina recovery were obtained.The recovery efficiencies of alumina and Na_(2)O from the RM are 63.06%and 97.34%,respectively,and the Na_(2)O content in the treated RM is only 0.13%.
基金supported by the National Natural Science Foundation of China(No.52300170).
文摘Catalytic CO_(2)-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis.Single-atom catalysts(SACs)with maximized atomic utilization,tailored electronic configurations and unique metal-support interactions,exhibit superior performance in CO_(2) activation and methanol synthesis.This review systematically compares reaction mechanisms and pathways across thermal,photocatalytic and electrocatalytic systems,emphasizing structure-activity relationships governed by active sites,coordination microenvironments and support functionalities.Through case studies of representative SACs,we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity.A critical analysis of reaction parameters(e.g.,temperature,pressure)reveals condition-dependent catalytic behaviors in thermal system,with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps.While thermal catalysis achieves industrially viable methanol yields,the scalability is constrained by energy-intensive operation and catalyst sintering.Conversely,photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations.To address the challenges,we propose strategic research priorities on precise design of active sites,synergy of multiple technological pathways,development of intelligent catalytic systems and diverse CO_(2) feedstock compatibility.These insights establish a framework for developing next-generation SACs,offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.
基金supported by the National Natural Science Foundation of China(Grant No.22479097)the Shanghai Science and Technology Committee(Grant Nos.23ZR1433000)the National High-Level Talent Program for Young Scholars,the Start-up Fund(F.S.)from Shanghai Jiao Tong University,China.We also acknowledge the SJTU Instrument Analysis Centre for the measurements.
文摘Two-dimensional nanofluidic membranes have garnered considerable interest due to their potential for cost-effective osmotic energy harvesting.One promising approach to enhancing ion conductivity and selectivity is the incorporation of vip additives.However,the traditional host-vip configuration can undermine the structural integrity of nanochannels owing to the inconsistent size and shape of these additives.Drawing inspiration from the intricate design of biological protein channels,which utilize small amino acid molecules as vips,we have addressed this issue by incorporating glycine,a common amino acid,into a vermiculite membrane using a simple vacuum-assisted infiltration method.The resulting vermiculite-glycine membrane demonstrates 1.8 times greater ionic conductivity and twice the power density compared to pure vermiculite membranes.Analysis based on glycine content,coupled with spectroscopic examination,reveals that ion conductivity is linked to the distribution of glycine molecules across three specific sites within the membrane.This suggests that glycine molecules—whether confined in voids,adsorbed onto nanochannel surfaces,or intercalated within multilayered vermiculite nanoparticles—enhance nanofluidic ion transport by modulating surface and space charge density,as well as strengthening hydrogen bonding,electrostatic interactions,and steric effects.This work reveals the specific interactions between amino acids and vermiculite,offering a novel path for advancing nanofluidic composite membranes and highlighting critical considerations for the proposed strategy.
文摘Conventional locking/release mechanisms often face challenges in aircraft wing separation processes,such as excessive impact loads and insufficient synchronization.These may cause structural damage to the airframe or attitude instability,seriously compromising mission reliability.To address this engineering challenge,this paper proposes a multi-point low-impact locking/release mechanism based on the mobility model and energy conversion strategy.Through establishing a DOF constraint framework system,this paper systematically analyzes the energy transfer and conversion characteristics during the wing separation process,reveals the generation mechanism of impact loads,and conducts research on low-impact design based on energy conversion strategy.Building on this foundation,a single-point locking/release mechanism employing parallel trapezoidal key shaft structure was designed,which increases frictional contact time and reduces the energy release rate,thereby achieving low-impact characteristics.The mechanism's performance was validated through physical prototype development and systematic functional testing(including unlocking force,synchronization,and impact tests).Experimental results demonstrate:(1)Under 14 kN preload condition,the maximum unlocking force was only 92.54 N,showing a linear relationship with preload that satisfies the"strong-connection/weak-unlock"design requirement;(2)Wing separation was completed within 46 ms,with synchronization time difference among three separation mechanisms stably controlled within 12-14 ms,proving rapid and reliable operation;(3)The unlocking impact acceleration ranged between 26 and 73 g,below the 100 g design limit,confirming the effectiveness of the energy conversion strategy.The proposed low-impact locking/release mechanism design method based on energy conversion strategy resolves the traditional challenges of high impact and synchronization deficiencies.The synergistic optimization mechanism of"structural load reduction and performance improvement"provides a highly reliable technical solution for wing separable mechanisms while offering novel design insights for wing connection/separation systems engineering.
基金funded by Nansha District Science and Technology Project(Grant Number.2024ZD008)funded by China Geological Survey(Grant number:No.DD20230066,DD20242659).
文摘As a controllable power generation method requiring no energy storage,Ocean Thermal Energy Conversion(OTEC)technology demonstrates characteristics of abundant reserves,low pollution,and round-the-clock stable operation.The free-standing cold-water pipe(CWP)in the system withstands various complex loads during operation,posing potential failure risks.To reveal the deformation and stress mechanisms of OTEC CWPs,this study first analyzes wave particle velocity and acceleration to determine wave loads at different water depths.Based on the Euler-Bernoulli beam model,a quasi-static load calculation model for OTEC CWPs was established.The governing equations were discretized using the finite difference method,and matrix equations were solved to analyze bending deformation,bending moments,and surface stresses at discrete points along the pipe.Results indicate that water depths within 50 m represent a critical zone where wave particle velocity,acceleration,and wave loads exhibit significant variations in harmonic patterns,while beyond 50 m depth wave loads decrease linearly.Ocean currents and surface wind-driven currents substantially influence the CWP’s lateral displacement.Considering the effect of clump weights,the maximum lateral displacement occurs at 600–800 m below sea level.Utilizing large-wall-thickness high-strength pipes at the top section significantly enhances the structural safety of the CWP system.
基金the financial support from the National Natural Science Foundation of China (Nos.U23A20677,22022610 and 52400137)"Pioneer" and "Leading Goose" R&D Program of Zhejiang (Nos.2022C03146 and 2023C03017)+2 种基金China Postdoctoral Science Foundation (No.2024T170805)Zhejiang Provincial Natural Science Foundation of China (No.LDT23E06015B06)the support of the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University for assistance with the calculations。
文摘Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.
基金the Inner Mongolia Natural Science Foundation(2023ZD05,2025JQ028,2025MS02001)the National Natural Science Foundation of China(22278238,22238004)+3 种基金the National Key Research and Development Program of China(2024YFE0211400)the Major Science and Technology Program of Inner Mongolia Autonomous Region(20212120326)the“Elite Talents Revitalize Inner Mongolia”Initiative–Tier-1 Talent Team(202410)the Ordos Science and Technology Breakthrough(JBGS2024003),and Ordos Laboratory for their financial support.
文摘Methanol,a crucial C1 intermediate,bridges traditional fossil-based chemical processes with emerging sustainable catalytic technologies by serving as both a versatile hydrogenation product from CO/CO_(2)and an active intermediate for hydrocarbon synthesis.Despite significant progress in methanol-to-hydrocarbon(MTH)conversion,a comprehensive understanding of reaction mechanisms remains essential to enhance catalyst design and industrial applicability.This review critically synthesizes recent advances in mechanistic insights related to methanol conversion and methanol-mediated catalytic processes.Firstly,we systematically outline key reaction pathways involved in initial carbon–carbon(C–C)bond formation through direct and indirect mechanisms,emphasizing significant breakthroughs from spectroscopic analyses and theoretical calculations.Subsequently,we highlight the autocatalytic characteristics and dual-cycle mechanisms underlying MTH processes,critically evaluating the roles of zeolite structures,pore sizes,topology,and acidity in governing product selectivity and catalyst stability.Additionally,we discuss cutting-edge developments in tandem catalytic systems employing methanol as a pivotal intermediate for CO_(x)hydrogenation,emphasizing the transferable mechanistic principles and catalytic insights.Finally,we identify future research directions,including elucidating precise hydrocarbon pool(HCP)intermediates,optimizing zeolite structures through computational-guided design,and developing robust catalytic systems leveraging advanced characterization methods and artificial intelligence.By integrating multidisciplinary approaches from catalytic science,materials engineering,and reaction engineering,this review provides actionable guidance towards rational design and optimization of advanced catalytic systems for efficient methanol conversion processes.
基金supported by the Key Project of Guangzhou City,No.202206060002Science and Technology Project of Guangdong Province,No.2018B030332001Guangdong Provincial Pearl River Project,No.2021ZT09Y552 (all to GC)。
文摘Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.
文摘The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the prognosis for ICC remains poor.Owing to the high degree of malignancy and insidious onset of ICC,numerous cases are detected at intermediate or advanced stages of the disease,hence eliminating the chance for surgical intervention.Moreover,because of the highly invasive characteristics of ICC,recurrence and metastasis postresection are prevalent,leading to a 5-year survival rate of only 20%-35%following surgery.In the past decade,different methods of treatment have been investigated,including transarterial chemoembolization,transarterial radioembolization,radiotherapy,systemic therapy,and combination therapies.For certain patients with advanced ICC,conversion treatment may be utilized to facilitate surgical resection and manage disease progression.This review summarizes the definition of downstaging conversion treatment and presents the clinical experience and evidence concerning conversion treatment for advanced ICC.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
基金supported by the National Natural Science Foundation of China(No.62374142)Fundamental Research Funds for the Central Universities(Nos.20720220085 and 20720240064)+2 种基金External Cooperation Program of Fujian(No.2022I0004)Major Science and Technology Project of Xiamen in China(No.3502Z20191015)Xiamen Natural Science Foundation Youth Project(No.3502Z202471002)。
文摘Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor micro-LED displays.However,the impact of solvent on both the printing process and the morphology of SIJ-printed PNC color conversion microstructures remains underexplored.In this study,we prepared samples of CsPbBr3PNC colloid inks in various solvents and investigated the solvent's impact on SIJ printed PNC microstructures.Our findings reveal that the boiling point of the solvent is crucial to the SIJ printing process of PNC colloid inks.Only does the boiling point of the solvent fall in the optimal range,the regular positioned,micron-scaled,conical PNC microstructures can be successfully printed.Below this optimal range,the ink is unable to be ejected from the nozzle;while above this range,irregular positioned microstructures with nanoscale height and coffee-ring-like morphology are produced.Based on these observations,high-resolution color conversion PNC microstructures were effectively prepared using SIJ printing of PNC colloid ink dispersed in dimethylbenzene solvent.
基金National Natural Science Foundation of China,Grant/Award Numbers:52002052,52073252,52372235Science and Technology Department of Zhejiang Province,Grant/Award Number:2023C01231+2 种基金Key Research and Development Project of Science and Technology Department of Sichuan Province,Grant/Award Number:2022YFSY0004the Open Project Program of the State Key Laboratory of New textile Materials and Advanced Processing Technologies,Grant/Award Number:FZ2021009Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),the Ministry of Education,Grant/Award Numbers:KFM202202,KFM202302,KFM202303。
文摘Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increased applications of plasma technology in the field of multiscale functional materials'preparation,with a number of interesting results.This review will begin by introducing the basic knowledge of plasma,including the definition,typical parameters,and classification of plasma setups.Following this,we will provide a comprehensive review and summary of the applications(phase conversion,doping,deposition,etching,exfoliation,and surface treatment)of plasma in common energy conversion and storage systems,such as electrocatalytic conversion of small molecules,batteries,fuel cells,and supercapacitors.This article summarizes the structure-performance relationships of electrochemical energy conversion and storage materials(ECSMs)that have been prepared or modified by plasma.It also provides an overview of the challenges and perspectives of plasma technology,which could lead to a new approach for designing and modifying electrode materials in ECSMs.
基金National Key R&D Program of China (2023YFA1508001 and 2023YFA1508002)National Natural Science Foundation of China (22272120 and U2202251)+1 种基金Hainan Province Science and Technology Special Fund(ZDYF2023SHFZ120)Research Foundation of Marine Science and Technology Collaborative Innovation Center of Hainan University (XTCX2022HYB01)。
文摘Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.
基金西南大学中央高校基本科研业务费项目(SWU-KT22030)重庆市教育委员会科学技术研究项目(KJQN202300205)Deutsche Forschungsgemeinschaft(DFG,German Research Foundation,457444676).
文摘Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity are also tunable,increasing its functional versatility.These make diamond and its related materials,such as its composites,highly promising for various applications in energy fields.This review summarizes recent advances and key achievements in energy storage and conversion,covering electrochemical energy storage(e.g.,batteries and supercapacitors),electrocatalytic energy conversion(e.g.,CO_(2)and nitrogen reduction reactions),and solar energy conversion(e.g.,photo-(electro)chemical CO_(2)and nitrogen reduction reactions,and solar cells).Current challenges and prospects related to the synthesis of diamond materials and the technologies for their energy applications are outlined and discussed.
