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
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
Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive ...Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive reaction to CO_(2) conversion.Therefore,proper cocatalysts are generally needed to enhance CO_(2) conversion but suppress H_(2) production.In this work,zinc/gallium(Zn/Ga)dual co-catalysts consisting of Zn0 and amorphous ZnGa_(2)O_(4) species were found to selectively produce carbon monoxide(CO)during the photocatalytic conversion of carbon dioxide(CO_(2))using water(H_(2)O)as an electron donor over photocatalysts such as NaTaO_(3),Ga_(2)O_(3),and ZnGa_(2)O_(4),and in the electrochemical reduction of CO_(2) over Zn0 electrodes.It is considered that there are two effects associated with the Zn/Ga dual co-catalysts:(1)a galvanic cell effect between Zn0 and amorphous ZnGa_(2)O_(4),and(2)a Z-scheme effect in NaTaO_(3)/Zn0/amorphous ZnGa_(2)O_(4).The coupling of these two effects favored the active and selective evolution of CO during the photocatalytic conversion of CO_(2) by H_(2)O.In the case of Ga_(2)O_(3) photocatalyst,480.8μmol/h of CO was produced with the presence of Zn/Ga dual cocatalysts.Moreover,the Zn/Ga dual cocatalysts universally worked in the electrochemical reduction of CO_(2).The partial current toward CO_(2) conversion was increased from 2.6 to 6.6 mA/cm,and the selectivity toward CO was promoted to from 46.4%to 74.2%.展开更多
Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible s...Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible structural degradation.To overcome these limitations,we propose a rationally engineered nanoreactor architecture that stabilizes defect-rich MoS_(2)via interlayer incorporation of a carbon monolayer,followed by encapsulation within a nitrogen-doped carbon shell,forming a MoSSe@NC heterostructure.This tailored structure synergistically accelerates both K^(+)diffusion kinetics and electron transfer,enabling unprecedented rate performance(107 mAh g^(-1)at 10 Ag^(-1))and ultralong cyclability(86.5%capacity retention after 1200 cycles at 3 A g^(-1)).Mechanistic insights reveal a distinctive“adsorption-conversion”pathway,where sulfur vacancies on exposed S-Mo-S basal planes act as preferential K^(+)adsorption sites,effectively suppressing parasitic phase transitions during intercalation.In situ X-ray diffraction and transmission electron microscopy corroborate the structural reversibility of the conversion reaction,with the carbon matrix dynamically accommodating strain while preserving electrode integrity.This work not only advances the understanding of defect-driven interfacial chemistry in conversion-type materials but also provides a versatile strategy for designing high-performance anodes in next-generation PIBs through heterostructure engineering.展开更多
Thermoelectric (TE) materials enable precise, noiseless, and moving-part-free waste heat recovery and solid-state refrigeration through the Seebeck and Peltier effects [1–3]. The efficiency of TE materials is typical...Thermoelectric (TE) materials enable precise, noiseless, and moving-part-free waste heat recovery and solid-state refrigeration through the Seebeck and Peltier effects [1–3]. The efficiency of TE materials is typically evaluated by a dimensionless figure of merit (ZT = S2σT/(κe+ κl)), which depends on the delicate interplay among the electrical conductivity (σ), Seebeck coefficient (S), lattice thermal conductivity (κl), and electronic thermal conductivity (κe) [4].展开更多
As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode mate...As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode materials undergo complex ion intercalation and deintercalation processes,accompanied by defect formation and structural evolution.However,the microscopic mechanisms underlying processes such as cation disordering,lattice oxygen loss,and stage structure formation are still not fully understood.To address these challenges,we have developed the Electrode Dynamic Ion Intercalation/Deintercalation Simulator(EDIS),a software platform designed to simulate the dynamic processes of ion intercalation and deintercalation in electrode materials.Leveraging high-precision machine learning potentials,EDIS can efficiently model structural evolution and lithium-ion diffusion behavior under various states of charge and discharge,achieving accuracy approaching that of quantum mechanical methods in relevant chemical spaces.The software supports quantitative analysis of how variations in lithium-ion concentration and distribution affect lithium-ion transport properties,enables evaluation of the impact of structural defects,and allows for tracking of both structural evolution and transport characteristics during continuous cycling.EDIS is versatile and can be extended to sodium-ion batteries and related systems.By enabling in-depth analysis of these microscopic processes,EDIS provides a robust theoretical tool for mechanistic studies and the rational design of high-performance electrode materials for next-generation lithium-ion batteries.展开更多
Transcription factor-mediated cell conversion has been reported in the central nervous system of both rodents and nonhuman primates.In particular,glia-to-neuron conversion has been achieved in the brain and spinal cor...Transcription factor-mediated cell conversion has been reported in the central nervous system of both rodents and nonhuman primates.In particular,glia-to-neuron conversion has been achieved in the brain and spinal cord of animal models for neural regeneration and repair.However,whether glia-to-neuron conversion can be used for brain repair in humans needs to be explored.To investigate the use of glia-to-neuron conversion technology in the human brain,we established a long-term ex vivo culture system using human brain tissue that was surgically removed from epileptic patients to test glia-to-neuron conversion directly.We found that neural transcription factors NeuroD1 and Ascl1 both converted human glial cells into neurons.Immunostaining and electrophysiological recordings showed that the glia-converted neurons demonstrated immature properties during the initial 7-14 days of conversion,and then acquired more mature neuronal properties after 21-27 days of conversion.These ex vivo conversion studies in human brain tissue pave the way toward future clinical trials using a transcription factor-based glia-to-neuron conversion approach to treat neurological disorders.展开更多
Zirconium-based conversion coatings have emerged as an environmentally friendly alternative to traditional phosphate coatings in the automotive industry,offering excellent corrosion resistance and effective protection...Zirconium-based conversion coatings have emerged as an environmentally friendly alternative to traditional phosphate coatings in the automotive industry,offering excellent corrosion resistance and effective protection for metal substrates.However,due to their relatively recent use in industrial applications,process control during zirconium conversion coating remains underdeveloped.In this study,the reaction kinetics of galvanized steel during the zirconium conversion coating were investigated systematically.The findings reveal an optimal coating time,after which the corrosion resistance of galvanized steel decreases.This decline results from the formation of corrosion cavities that cause discontinuities in the protective zirconium layer.These insights provide guidance for optimizing zirconium conversion coating processes in industrial manufacturing.展开更多
Laser-induced graphene(LIG)has emerged as a versatile,sustainable material for advanced energy technologies,offering a scalable,catalyst-free,and programmable method to directly convert carbon-rich substrates into por...Laser-induced graphene(LIG)has emerged as a versatile,sustainable material for advanced energy technologies,offering a scalable,catalyst-free,and programmable method to directly convert carbon-rich substrates into porous,conductive graphene.This single-step laser writing approach enables flexible,patternable electrodes without complex post-processing.With its high conductivity,large surface area,and tunable chemistry,LIG is well-suited for diverse applications including batteries,supercapacitors,dyesensitized solar cells(DSSCs),dual cells,water-splitting electrocatalysis,and triboelectric nanogenerators(TENGs).In energy storage,LIG improves charge transport,buffer volume changes,and provides a robust framework,enhancing capacitance,cycling stability,and rate capability.Its catalytic activity is further boosted through heteroatom doping or transition-metal incorporation,achieving HER/OER performance comparable to noble metals.In DSSCs,LIG functions as a flexible,low-cost alternative to platinum counter electrodes,while in TENGs,its strong triboelectric response and mechanical durability enable integration into self-powered,wearable systems.Despite the immense recent progress in this field,challenges remain regarding the scalability,long-term operational stability,and interfacial engineering of LIGbased composites.Further exploration into multi-laser systems,substrate diversity,and synergistic composite architectures will be crucial to optimizing device performance and reliability.Nevertheless,the green,cost-efficient,rapid,and programmable synthesis of LIG poses it as a cornerstone potential building block material in the development of future sustainable and multifunctional energy systems.Throughout the review we compare fabrication strategies,summarize performance metrics against relevant benchmarks,and identifying common mechanistic advantages conferred by the laser writing process.Remaining challenges-such as scale-up,precursor diversity,long-term environmental stability,and integration into complex device architectures-are outlined alongside prospective research directions.Collectively,this review article provides an in-depth perspective on the multifunctional nature of LIG,underscoring its promise in next-generation energy storage,conversion,harvesting applications,and laying the groundwork for future research directions.展开更多
The promising prospects for all-day building thermal management are driving widespread research into spectrally selective manipulation materials.This article first summarizes the evolution path of metal reversible dep...The promising prospects for all-day building thermal management are driving widespread research into spectrally selective manipulation materials.This article first summarizes the evolution path of metal reversible deposition technology,noting its advantages of cost-effectiveness and scientific rigor.It then highlights the groundbreaking work by Wang et al.(published in ACS Energy Letters,2025,10,3231)on coupling metastructured photothermal conversion electrodes and reversible Cu deposition for all-day energy management.Finally,the commercial viability of Wang et al.'s approach for building energy saving and its potential applicability to other scenarios are elaborated.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
County-to-district conversion(CDC) has restructured the pattern of urban-rural development and influenced the allocation of resources by local governments as well as the urbanization process.However,the impact and mec...County-to-district conversion(CDC) has restructured the pattern of urban-rural development and influenced the allocation of resources by local governments as well as the urbanization process.However,the impact and mechanism of the CDC on China's urban-rural integration development(URID) are not yet clear.Using panel data from 52 county-level cities,districts,and counties in Jiangsu Province of China during 2005–2021,this paper constructed an evaluation system for URID and applied the multi-period difference-in-differences(DID) model to measure the impact of the CDC on URID and identify its primary mechanisms of action.The results demonstrated that the CDC has significantly fostered URID,though with pronounced regional heterogeneity.Specifically,while the CDC facilitated URID in the southern and central Jiangsu Province—regions characterized by high socio-economic development—it exerted a less significant impact in the comparatively underdeveloped northern Jiangsu Province.Mechanistically,the implementation of the CDC promotes equal regional development,enhances rural selfdevelopment capacity,improves environmental quality and living standards,and optimizes urban-rural land allocation and transport networks.Ultimately,this study clarifies the role of the CDC in China,provides insights for achieving URID,and offers a reference for other countries pursuing coordinated urban-rural development.展开更多
Adult neurogenesis is generally considered to be very limited;however,there is increasing evidence that this phenomenon is conserved across species.Traditionally,research has focused on identifying precursor cells,tho...Adult neurogenesis is generally considered to be very limited;however,there is increasing evidence that this phenomenon is conserved across species.Traditionally,research has focused on identifying precursor cells,those that are actively dividing or have the potential to divide.Direct evidence of adult neurogenesis has been found in rats,mice,songbirds,and nonhuman primates.In humans,while the evidence is indirect,it strongly suggests that neurogenesis also occurs during adulthood.In mammals,this active neurogenesis is preserved by radial glial progenitors,which remain in specific niches in the subventricular zone of the lateral ventricles and in the subgranular zone of the hippocampal dentate gyrus(Kumar et al.,2019).展开更多
Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge t...Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge towards efficient DCBs.Here,we introduce a heteroatom-doped sp^(3) /sp^(2) hybridized carbon fiber membrane(cPAN-Gr)as a universal binder-free active electrode that effectively overcomes this trade-off,enabling efficient Li-ion intercalation chemistry for advanced DCBs.By strategically tuning the sp^(3) and sp^(2) carbon hybridization,the interlayer interaction,geometric and electronic structures of c PANGr are simultaneously optimized,which facilitates rapid Li-ion adsorption,smooth interlayer transport,and efficient electron transport by maximizing the synergy between sp^(2) -and sp^(3) -hybridized carbon.This,coupled with a 3D porous network structure,endows the c PAN-Gr with superior Li-ion storage capability and fast reaction kinetics.Therefore,the c PAN-Gr electrode delivers a high reversible capacity of 345 m A h g^(-1),excellent rate capability(50 C),and an ultralong cycle life over 10,000 cycles,outperforming other reported carbon-based electrodes.Moreover,the constructed DCB exhibits a large specific capacity of 135 m A h g^(-1),long-term cyclability over 500 cycles,and a remarkable energy density of 524.4 Wh kg^(-1).The c PAN-Gr electrode can also be expanded to construct a LiFePO_(4)//cPAN-Gr full battery.Combined theoretical and experimental studies reveal the crucial role of an optimized sp^(3) /sp^(2) ratio(79%)with topological defects and pyridine/pyrrolic N sites on the performance enhancement.This work offers new insights into the design of advanced carbon materials for DCBs and beyond.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
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%.
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supported by the National Key R&D Program of China(No.2023YFC3710800)the National Natural Science Foundation of China(No.22376207)+1 种基金the Research Fund of High-Level Training Talents of“333”Project in Jiangsu provinceFunding for school-level research projects of Yancheng Institute of Technology(Nos.xjr2024008 and xjr2023055).
文摘Artificial synthesis is an environment friendly photocatalytic strategy to converse carbon dioxide(CO_(2))into useful chemicals.However,water(H_(2)O)splitting,producing(hydrogen)H_(2) strongly,is always a competitive reaction to CO_(2) conversion.Therefore,proper cocatalysts are generally needed to enhance CO_(2) conversion but suppress H_(2) production.In this work,zinc/gallium(Zn/Ga)dual co-catalysts consisting of Zn0 and amorphous ZnGa_(2)O_(4) species were found to selectively produce carbon monoxide(CO)during the photocatalytic conversion of carbon dioxide(CO_(2))using water(H_(2)O)as an electron donor over photocatalysts such as NaTaO_(3),Ga_(2)O_(3),and ZnGa_(2)O_(4),and in the electrochemical reduction of CO_(2) over Zn0 electrodes.It is considered that there are two effects associated with the Zn/Ga dual co-catalysts:(1)a galvanic cell effect between Zn0 and amorphous ZnGa_(2)O_(4),and(2)a Z-scheme effect in NaTaO_(3)/Zn0/amorphous ZnGa_(2)O_(4).The coupling of these two effects favored the active and selective evolution of CO during the photocatalytic conversion of CO_(2) by H_(2)O.In the case of Ga_(2)O_(3) photocatalyst,480.8μmol/h of CO was produced with the presence of Zn/Ga dual cocatalysts.Moreover,the Zn/Ga dual cocatalysts universally worked in the electrochemical reduction of CO_(2).The partial current toward CO_(2) conversion was increased from 2.6 to 6.6 mA/cm,and the selectivity toward CO was promoted to from 46.4%to 74.2%.
基金financially supported by the supported by Shandong Provincial Natural Science Foundation(ZR2024MB108)Taishan Young Scholar Program(tsqn202312312)Excellent Young Scholars of the Shandong Provincial Natural Science Foundation(Overseas)(2023HWYQ-112)。
文摘Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible structural degradation.To overcome these limitations,we propose a rationally engineered nanoreactor architecture that stabilizes defect-rich MoS_(2)via interlayer incorporation of a carbon monolayer,followed by encapsulation within a nitrogen-doped carbon shell,forming a MoSSe@NC heterostructure.This tailored structure synergistically accelerates both K^(+)diffusion kinetics and electron transfer,enabling unprecedented rate performance(107 mAh g^(-1)at 10 Ag^(-1))and ultralong cyclability(86.5%capacity retention after 1200 cycles at 3 A g^(-1)).Mechanistic insights reveal a distinctive“adsorption-conversion”pathway,where sulfur vacancies on exposed S-Mo-S basal planes act as preferential K^(+)adsorption sites,effectively suppressing parasitic phase transitions during intercalation.In situ X-ray diffraction and transmission electron microscopy corroborate the structural reversibility of the conversion reaction,with the carbon matrix dynamically accommodating strain while preserving electrode integrity.This work not only advances the understanding of defect-driven interfacial chemistry in conversion-type materials but also provides a versatile strategy for designing high-performance anodes in next-generation PIBs through heterostructure engineering.
基金supports from the Department of Education of Liaoning Province (LJ242510147006)
文摘Thermoelectric (TE) materials enable precise, noiseless, and moving-part-free waste heat recovery and solid-state refrigeration through the Seebeck and Peltier effects [1–3]. The efficiency of TE materials is typically evaluated by a dimensionless figure of merit (ZT = S2σT/(κe+ κl)), which depends on the delicate interplay among the electrical conductivity (σ), Seebeck coefficient (S), lattice thermal conductivity (κl), and electronic thermal conductivity (κe) [4].
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB1040300)the National Natural Science Foundation of China(Grant No.52172258)。
文摘As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode materials undergo complex ion intercalation and deintercalation processes,accompanied by defect formation and structural evolution.However,the microscopic mechanisms underlying processes such as cation disordering,lattice oxygen loss,and stage structure formation are still not fully understood.To address these challenges,we have developed the Electrode Dynamic Ion Intercalation/Deintercalation Simulator(EDIS),a software platform designed to simulate the dynamic processes of ion intercalation and deintercalation in electrode materials.Leveraging high-precision machine learning potentials,EDIS can efficiently model structural evolution and lithium-ion diffusion behavior under various states of charge and discharge,achieving accuracy approaching that of quantum mechanical methods in relevant chemical spaces.The software supports quantitative analysis of how variations in lithium-ion concentration and distribution affect lithium-ion transport properties,enables evaluation of the impact of structural defects,and allows for tracking of both structural evolution and transport characteristics during continuous cycling.EDIS is versatile and can be extended to sodium-ion batteries and related systems.By enabling in-depth analysis of these microscopic processes,EDIS provides a robust theoretical tool for mechanistic studies and the rational design of high-performance electrode materials for next-generation lithium-ion batteries.
基金supported by the Key Project of Guangzhou City,No.202206060002(to GC)the Guangdong Province Science and Technology Project of China,No.2018B030332001(to GC)+1 种基金the Natural Science Foundation of Guangdong Province of China,No.2020A1515010854(to QW)the Yi-Liang Liu Endowment Fund from Jinan University Education Development Foundation。
文摘Transcription factor-mediated cell conversion has been reported in the central nervous system of both rodents and nonhuman primates.In particular,glia-to-neuron conversion has been achieved in the brain and spinal cord of animal models for neural regeneration and repair.However,whether glia-to-neuron conversion can be used for brain repair in humans needs to be explored.To investigate the use of glia-to-neuron conversion technology in the human brain,we established a long-term ex vivo culture system using human brain tissue that was surgically removed from epileptic patients to test glia-to-neuron conversion directly.We found that neural transcription factors NeuroD1 and Ascl1 both converted human glial cells into neurons.Immunostaining and electrophysiological recordings showed that the glia-converted neurons demonstrated immature properties during the initial 7-14 days of conversion,and then acquired more mature neuronal properties after 21-27 days of conversion.These ex vivo conversion studies in human brain tissue pave the way toward future clinical trials using a transcription factor-based glia-to-neuron conversion approach to treat neurological disorders.
基金express their sincere gratitude to the Jiangsu Key Laboratory of Advanced Metallic Materials of Southeast University for providing the complete laboratory facilities required for this research project.
文摘Zirconium-based conversion coatings have emerged as an environmentally friendly alternative to traditional phosphate coatings in the automotive industry,offering excellent corrosion resistance and effective protection for metal substrates.However,due to their relatively recent use in industrial applications,process control during zirconium conversion coating remains underdeveloped.In this study,the reaction kinetics of galvanized steel during the zirconium conversion coating were investigated systematically.The findings reveal an optimal coating time,after which the corrosion resistance of galvanized steel decreases.This decline results from the formation of corrosion cavities that cause discontinuities in the protective zirconium layer.These insights provide guidance for optimizing zirconium conversion coating processes in industrial manufacturing.
文摘Laser-induced graphene(LIG)has emerged as a versatile,sustainable material for advanced energy technologies,offering a scalable,catalyst-free,and programmable method to directly convert carbon-rich substrates into porous,conductive graphene.This single-step laser writing approach enables flexible,patternable electrodes without complex post-processing.With its high conductivity,large surface area,and tunable chemistry,LIG is well-suited for diverse applications including batteries,supercapacitors,dyesensitized solar cells(DSSCs),dual cells,water-splitting electrocatalysis,and triboelectric nanogenerators(TENGs).In energy storage,LIG improves charge transport,buffer volume changes,and provides a robust framework,enhancing capacitance,cycling stability,and rate capability.Its catalytic activity is further boosted through heteroatom doping or transition-metal incorporation,achieving HER/OER performance comparable to noble metals.In DSSCs,LIG functions as a flexible,low-cost alternative to platinum counter electrodes,while in TENGs,its strong triboelectric response and mechanical durability enable integration into self-powered,wearable systems.Despite the immense recent progress in this field,challenges remain regarding the scalability,long-term operational stability,and interfacial engineering of LIGbased composites.Further exploration into multi-laser systems,substrate diversity,and synergistic composite architectures will be crucial to optimizing device performance and reliability.Nevertheless,the green,cost-efficient,rapid,and programmable synthesis of LIG poses it as a cornerstone potential building block material in the development of future sustainable and multifunctional energy systems.Throughout the review we compare fabrication strategies,summarize performance metrics against relevant benchmarks,and identifying common mechanistic advantages conferred by the laser writing process.Remaining challenges-such as scale-up,precursor diversity,long-term environmental stability,and integration into complex device architectures-are outlined alongside prospective research directions.Collectively,this review article provides an in-depth perspective on the multifunctional nature of LIG,underscoring its promise in next-generation energy storage,conversion,harvesting applications,and laying the groundwork for future research directions.
基金supported by grants from the National Natural Science Foundation of China(no.62175248,U24A2061)Shanghai Science and Technology Funds(no.23ZR1481900,25ZR1401373)Science Foundation for Youth Scholar of State Key Laboratory of High Performance Ceramics and Superfine Microstructures(no.SKL202202).
文摘The promising prospects for all-day building thermal management are driving widespread research into spectrally selective manipulation materials.This article first summarizes the evolution path of metal reversible deposition technology,noting its advantages of cost-effectiveness and scientific rigor.It then highlights the groundbreaking work by Wang et al.(published in ACS Energy Letters,2025,10,3231)on coupling metastructured photothermal conversion electrodes and reversible Cu deposition for all-day energy management.Finally,the commercial viability of Wang et al.'s approach for building energy saving and its potential applicability to other scenarios are elaborated.
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supported by the National Natural Science Foundation of China (42271252,42230510)。
文摘County-to-district conversion(CDC) has restructured the pattern of urban-rural development and influenced the allocation of resources by local governments as well as the urbanization process.However,the impact and mechanism of the CDC on China's urban-rural integration development(URID) are not yet clear.Using panel data from 52 county-level cities,districts,and counties in Jiangsu Province of China during 2005–2021,this paper constructed an evaluation system for URID and applied the multi-period difference-in-differences(DID) model to measure the impact of the CDC on URID and identify its primary mechanisms of action.The results demonstrated that the CDC has significantly fostered URID,though with pronounced regional heterogeneity.Specifically,while the CDC facilitated URID in the southern and central Jiangsu Province—regions characterized by high socio-economic development—it exerted a less significant impact in the comparatively underdeveloped northern Jiangsu Province.Mechanistically,the implementation of the CDC promotes equal regional development,enhances rural selfdevelopment capacity,improves environmental quality and living standards,and optimizes urban-rural land allocation and transport networks.Ultimately,this study clarifies the role of the CDC in China,provides insights for achieving URID,and offers a reference for other countries pursuing coordinated urban-rural development.
文摘Adult neurogenesis is generally considered to be very limited;however,there is increasing evidence that this phenomenon is conserved across species.Traditionally,research has focused on identifying precursor cells,those that are actively dividing or have the potential to divide.Direct evidence of adult neurogenesis has been found in rats,mice,songbirds,and nonhuman primates.In humans,while the evidence is indirect,it strongly suggests that neurogenesis also occurs during adulthood.In mammals,this active neurogenesis is preserved by radial glial progenitors,which remain in specific niches in the subventricular zone of the lateral ventricles and in the subgranular zone of the hippocampal dentate gyrus(Kumar et al.,2019).
基金financial support from Guangdong Basic and Applied Basic Research Foundation(2020B1515420001and 2023B1515040027)Fundamental Research Funds for the Central Universities,Sun Yat-sen University(23yxqntd002)the Postdoctoral Fellowship Program of CPSF(GZC20242066)。
文摘Dual-carbon batteries(DCBs)have emerged as an appealing candidate for large-scale energy storage,yet the common trade-off between active sites and electronic conduction in carbon materials engenders a main challenge towards efficient DCBs.Here,we introduce a heteroatom-doped sp^(3) /sp^(2) hybridized carbon fiber membrane(cPAN-Gr)as a universal binder-free active electrode that effectively overcomes this trade-off,enabling efficient Li-ion intercalation chemistry for advanced DCBs.By strategically tuning the sp^(3) and sp^(2) carbon hybridization,the interlayer interaction,geometric and electronic structures of c PANGr are simultaneously optimized,which facilitates rapid Li-ion adsorption,smooth interlayer transport,and efficient electron transport by maximizing the synergy between sp^(2) -and sp^(3) -hybridized carbon.This,coupled with a 3D porous network structure,endows the c PAN-Gr with superior Li-ion storage capability and fast reaction kinetics.Therefore,the c PAN-Gr electrode delivers a high reversible capacity of 345 m A h g^(-1),excellent rate capability(50 C),and an ultralong cycle life over 10,000 cycles,outperforming other reported carbon-based electrodes.Moreover,the constructed DCB exhibits a large specific capacity of 135 m A h g^(-1),long-term cyclability over 500 cycles,and a remarkable energy density of 524.4 Wh kg^(-1).The c PAN-Gr electrode can also be expanded to construct a LiFePO_(4)//cPAN-Gr full battery.Combined theoretical and experimental studies reveal the crucial role of an optimized sp^(3) /sp^(2) ratio(79%)with topological defects and pyridine/pyrrolic N sites on the performance enhancement.This work offers new insights into the design of advanced carbon materials for DCBs and beyond.
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.
