Photoheranostics have emerged as a promising tool for cancer theranostics owing to their real-time feedback on treatment and their precise diagnosis.Among them,how to improve the photothermal conversion efficiency(PCE...Photoheranostics have emerged as a promising tool for cancer theranostics owing to their real-time feedback on treatment and their precise diagnosis.Among them,how to improve the photothermal conversion efficiency(PCE)of phototheranostic agents(PTAs)is the key factor for phototheranostic systems.Herein,we provided an efficient method to improve PCE and constructed a biocompatible nano-material ICR-Qu@NH_(2)-Fe_(3)O_(4)@PEG(QNFP)by combing near-infrared second region(NIR-Ⅱ)molecular dye ICR-Qu and amino-modified magnetic nanoparticles and then encapsulated by DSPE-m PEG2000.QNFP exhibited excellent performance for photothermal therapy with a high PCE of 95.6%.Both in vitro and in vivo experiments indicated that QNFP could inhibit the growth of tumors under laser irradiation with low toxicity and realized real-time NIR-Ⅱfiuorescent imaging of tumors.In general,we realized a simple but efficient method to improve the PCE of NIR-Ⅱmolecular dye without reduce its quantum yield,which is an ideal choice for cancer diagnosis and treatment.展开更多
The research on the conversion efficiency of"Green Mountains into Clear Water"(Green)and"Gold and silver Mountains"(Gold)is of great significance to promote the coordination between natural resourc...The research on the conversion efficiency of"Green Mountains into Clear Water"(Green)and"Gold and silver Mountains"(Gold)is of great significance to promote the coordination between natural resource conservation in national park and the local economic and social development.This paper pays attention to the linking role of ecosystem services in different stages of the conversion process between the Green and Gold.Based on the twostage division,this paper constructs the accounting framework for conversion efficiency of Green and Gold.That is,the comprehensive conversion efficiency of Green and Gold is decomposed into the I-stage efficiency of ecological inputs conversion to Green and the II-stage efficiency of ecosystem services conversion to economic output.Furthermore,the Qilian Mountain National Park in China and its surrounding area Zhangye City,is taken as an example.Using a two-stage non-oriented super-efficiency network EBM model and panel data from 2007 to 2018 to empirically analysis the dynamic evolution characteristics of the conversion efficiency of Green and Gold.Based on this,the heterogeneity improvement strategy is proposed.The results show that:(1)the comprehensive efficiency of the Two Mountains conversion in Zhangye City decreased first and then increased.The highest was 1.715 in 2007;the lowest was 1.367 in 2012;since 2012,the development has gradually improved.The main reason for the decrease in the comprehensive efficiency from 2007 to 2012 is the lower conversion efficiency in IIstage.(2)Spatial difference analysis shows that the areas with low the comprehensive efficiency were concentrated in Sunan,Minle,and Shandan Counties along the Qilian Mountains.The comprehensive efficiency was 0.406,0.489 and 0.482 respectively.The key to improving the comprehensive efficiency of Sunan County and Minle County is II-stage,while the focus of improving Shandan County is I-stage.(3)Redundancy analysis found that the main factor affecting the comprehensive efficiency of the Two Mountains conversion is insufficient output.In the future,we should focus on expanding effective pathways for the Two Mountains conversion and innovating institutional mechanisms for realizing ecological value.展开更多
Correction to:Opto-Electronic Science https://www.oejournal.org/oes/article/doi/10.29026/oes.2024.230029 published online 21 March 2024.After the publication of this article1,it was brought to our attention that the i...Correction to:Opto-Electronic Science https://www.oejournal.org/oes/article/doi/10.29026/oes.2024.230029 published online 21 March 2024.After the publication of this article1,it was brought to our attention that the inset image and absorption spectrum in Fig.1(b)contained a mistake,probably leading to misunderstandings.The inset image and the absorption spectrum in Fig.1(b)were not based on the specific batch of PbS colloidal quantum dots(CQDs)used in this work.展开更多
A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamin...A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamino side groups,TT-Ph-C6 demonstrates excellent solubility and its crystal structure exhibits compact packing structures with a three-dimensional molecular stacking network.These structural attributes markedly promote exciton diffusion and charge carrier mobility,particularly advantageous for the fabrication of thick-film devices.TT-Ph-C6-based devices have attained a PCE of 18.01%at a film thickness of 100 nm,and even at a film thickness of 300 nm,the PCE remains at 14.64%,surpassing that of devices based on 2BTh-2F.These remarkable properties position TT-Ph-C6 as a highly promising NFREA material for boosting the efficiency of OSCs.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
Shock waves in the nozzle during supersonic separation under different conditions can disrupt the flow field’s thermodynamic equilibrium.While it contributes to the recovery of pressure energy,it also leads to the di...Shock waves in the nozzle during supersonic separation under different conditions can disrupt the flow field’s thermodynamic equilibrium.While it contributes to the recovery of pressure energy,it also leads to the dissipation of mechanical energy.This study aimed to investigate the effects of changes in back pressure on the shock wave position and its subsequent impact on the refrigeration performance of nozzles.A mathematical model for the supersonic gas in a nozzle was established and evaluated via experiments.The results show that when the back pressure is less than 0.2 MPa,no shock wave is generated in the nozzle,and high refrigeration and liquefaction efficiency can be ensured while effective pressure recovery is achieved.When the back pressure(pb)is increased from 0.3 to 0.6 MPa,the refrigeration efficiency of the nozzle decreases,and the shock wave position(x shock)is advanced from 157 to 118 mm.The maximum Mach number(Ma)that can be reached by the fluid in the nozzle is reduced from 1.97 to 1.27.When the back pressure is increased from 0.2 to 0.6 MPa,the minimum temperature is increased by 55.18 K.When the back pressure is greater than 0.3 MPa,the Mach number upstream of the shock wave is reduced from 1.97 to 1.27,the shock wave intensity is weakened,and the thickness of the boundary layer separation caused by the shock wave is also decreased accordingly.Therefore,to ensure refrigeration efficiency,measures should be taken to control the back pressure within a reasonable range.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
Despite being an excellent candidate for a photocathode,Cu_(2)ZnSnS_4(CZTS)performance is limited by suboptimal bulk and interfacial charge carrier dynamics.In this work,we introduce a facile and versatile CZTS precur...Despite being an excellent candidate for a photocathode,Cu_(2)ZnSnS_4(CZTS)performance is limited by suboptimal bulk and interfacial charge carrier dynamics.In this work,we introduce a facile and versatile CZTS precursor seed layer engineering technique,which significantly enhances crystal growth and mitigates detrimental defects in the postsulfurized CZTS light-absorbing films.This effective optimization of defects and charge carrier dynamics results in a highly efficient CZTS/CdS/TiO_(2)/Pt thin-film photocathode,achieving a record half-cell solar-to-hydrogen(HC-STH)conversion efficiency of 9.91%.Additionally,the photocathode exhibits a highest photocurrent density(J_(ph))of 29.44 m A cm^(-2)(at 0 VRHE)and favorable onset potential(Von)of 0.73 VRHE.Furthermore,our CTZS photocathode demonstrates a remarkable Jph of 16.54 m A cm^(-2)and HC-STH efficiency of 2.56%in natural seawater,followed by an impressive unbiased STH efficiency of 2.20%in a CZTS-BiVO_4 tandem cell.The scalability of this approach is underscored by the successful fabrication of a 4×4 cm^(2)module,highlighting its significant potential for practical,unbiased in situ solar seawater splitting applications.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
Evaluating the effectivenes s of forest restoration projects is crucial for designing adaptive restoration strategies.However,existing studies have primarily focused on ecological outcomes while overlooking cost input...Evaluating the effectivenes s of forest restoration projects is crucial for designing adaptive restoration strategies.However,existing studies have primarily focused on ecological outcomes while overlooking cost inputs.This gap can lead to increased uncertainties in restoration planning.Here we investigated forest dynamics in China's Upper Yangtze River Basin(UYRB)using kernel Normalized Difference Vegetation Index(kNDVI),Leaf Area Index(LAI),Gross Primary Productivity(GPP),Ku-band Vegetation Optical Depth(Ku-VOD)time series and climate data from1982 to 2020.Subsequently,we employed a residual trend analysis integrating temporal effects to determine the relative contributions of climate change and human activities to forest dynamics before and after the implementation of forest restoration engineering in 1998.Additionally,we developed an Afforestation Efficiency Index(AEI)to quantitatively assess the cost efficiency of afforestation projects.Results indicated that forest in the UYRB showed sustained increases during 1982-2020,with most areas experiencing greater growth after 1998 than before.Temporal effects of climatic factors influenced over 42.7%of the forest,and incorporating time-lag and cumulative effects enhanced climate-based explanations of forest variations by 1.61-24.73%.Human activities emerged as the dominant driver of forest dynamics post 1998,whereas climate variables predominated before this period.The cost-effectiveness of forest restoration projects in the UYRB typically ranges from moderate to high,with higher success predominantly observed in the northeastern and eastern counties,while the central,western,and northwestern counties mainly showed relatively low efficiency.These findings stress the need for assessing forest restoration outcomes from both ecological and cost perspectives,and can offer valuable insights for optimizing the layout of forest restoration initiatives in the UYRB.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
The goal of the present work is to demonstrate the potential of Artificial Neural Network(ANN)-driven Genetic Algorithm(GA)methods for energy efficiency and economic performance optimization of energy efficiency measu...The goal of the present work is to demonstrate the potential of Artificial Neural Network(ANN)-driven Genetic Algorithm(GA)methods for energy efficiency and economic performance optimization of energy efficiency measures in a multi-family house building in Greece.The energy efficiency measures include different heating/cooling systems(such as low-temperature and high-temperature heat pumps,natural gas boilers,split units),building envelope components for floor,walls,roof and windows of variable heat transfer coefficients,the installation of solar thermal collectors and PVs.The calculations of the building loads and investment and operating and maintenance costs of the measures are based on the methodology defined in Directive 2010/31/EU,while economic assumptions are based on EN 15459-1 standard.Typically,multi-objective optimization of energy efficiency measures often requires the simulation of very large numbers of cases involving numerous possible combinations,resulting in intense computational load.The results of the study indicate that ANN-driven GA methods can be used as an alternative,valuable tool for reliably predicting the optimal measures which minimize primary energy consumption and life cycle cost of the building with greatly reduced computational requirements.Through GA methods,the computational time needed for obtaining the optimal solutions is reduced by 96.4%-96.8%.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
Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The ch...Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions.In this study,we have tuned orbital hybridization states forming an interface enriched with sp^(2) hybridized carbon(sp^(2)-C),which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation.Benefiting from successfully constructed inorganic-rich SEI,the ICE increased to 91%and sodium storage capacity reached 346 mAh/g.Besides,the capacity retention rate was 90.7%after 700 cycles at 1 A/g higher than pristine electrode(83.8%).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
A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescenc...A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.展开更多
Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting d...Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting density and N rate,and their relationships with grain yield,radiation use efficiency(RUE),and N use efficiency for grain production(NUEg)in rice.A two-year field experiment was conducted with two hybrid varieties under three N levels,0 kg ha^(-1)(N1),90 kg ha^(-1)(N2)and 180 kg ha^(-1)(N3),and two planting densities,22.2 hills m-2(D1)and 33.3 hills m^(-2)(D2).Results showed 3.4%higher yield and 4.4%higher NUEg under N2D2 compared with N3D1.The extinction coefficient for N(K_(N))and light(K_(L))and their ratio(K_(N)/K_(L))at heading stage were significantly influenced by N rate,planting density,and their interaction.K_(N)decreased with the increase of N input or planting density.Compared to N1,K_(N)decreased by 43.5 and 58.8%under N2 and N3,respectively,while K_(N)under D2 decreased by 16.0%compared to D1.Higher K_(L)and K_(N)/K_(L)values occurred under low N rates,with opposite trends under high N rates.Increased planting density led to decreased K_(L)and K_(N)/K_(L)values.N2D2 demonstrated higher K_(L)and K_(N),and thus comparable K_(N)/K_(L),compared to N3D1.Correlation analysis revealed K_(L)negatively correlated with RUE,while K_(N)and K_(N)/K_(L)positively correlated with NUEg.These findings indicate that increasing planting density under reduced N input could maintain rice yield while enhancing resource use efficiency through regulation of canopy light and N distribution.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.U21A20308,22077088)Foundation from Science and Technology Major Project of Tibetan Autonomous Region of China(No.XZ202201ZD0001G)Foundation from Science and Technology Department of Sichuan Province(No.2021ZHCG0025)。
文摘Photoheranostics have emerged as a promising tool for cancer theranostics owing to their real-time feedback on treatment and their precise diagnosis.Among them,how to improve the photothermal conversion efficiency(PCE)of phototheranostic agents(PTAs)is the key factor for phototheranostic systems.Herein,we provided an efficient method to improve PCE and constructed a biocompatible nano-material ICR-Qu@NH_(2)-Fe_(3)O_(4)@PEG(QNFP)by combing near-infrared second region(NIR-Ⅱ)molecular dye ICR-Qu and amino-modified magnetic nanoparticles and then encapsulated by DSPE-m PEG2000.QNFP exhibited excellent performance for photothermal therapy with a high PCE of 95.6%.Both in vitro and in vivo experiments indicated that QNFP could inhibit the growth of tumors under laser irradiation with low toxicity and realized real-time NIR-Ⅱfiuorescent imaging of tumors.In general,we realized a simple but efficient method to improve the PCE of NIR-Ⅱmolecular dye without reduce its quantum yield,which is an ideal choice for cancer diagnosis and treatment.
基金funded by National Natural Science Foundation of China(Grant No.:42461046)the Postdoctoral Science Foundation of China(Grant No.:2020M673641XB).
文摘The research on the conversion efficiency of"Green Mountains into Clear Water"(Green)and"Gold and silver Mountains"(Gold)is of great significance to promote the coordination between natural resource conservation in national park and the local economic and social development.This paper pays attention to the linking role of ecosystem services in different stages of the conversion process between the Green and Gold.Based on the twostage division,this paper constructs the accounting framework for conversion efficiency of Green and Gold.That is,the comprehensive conversion efficiency of Green and Gold is decomposed into the I-stage efficiency of ecological inputs conversion to Green and the II-stage efficiency of ecosystem services conversion to economic output.Furthermore,the Qilian Mountain National Park in China and its surrounding area Zhangye City,is taken as an example.Using a two-stage non-oriented super-efficiency network EBM model and panel data from 2007 to 2018 to empirically analysis the dynamic evolution characteristics of the conversion efficiency of Green and Gold.Based on this,the heterogeneity improvement strategy is proposed.The results show that:(1)the comprehensive efficiency of the Two Mountains conversion in Zhangye City decreased first and then increased.The highest was 1.715 in 2007;the lowest was 1.367 in 2012;since 2012,the development has gradually improved.The main reason for the decrease in the comprehensive efficiency from 2007 to 2012 is the lower conversion efficiency in IIstage.(2)Spatial difference analysis shows that the areas with low the comprehensive efficiency were concentrated in Sunan,Minle,and Shandan Counties along the Qilian Mountains.The comprehensive efficiency was 0.406,0.489 and 0.482 respectively.The key to improving the comprehensive efficiency of Sunan County and Minle County is II-stage,while the focus of improving Shandan County is I-stage.(3)Redundancy analysis found that the main factor affecting the comprehensive efficiency of the Two Mountains conversion is insufficient output.In the future,we should focus on expanding effective pathways for the Two Mountains conversion and innovating institutional mechanisms for realizing ecological value.
文摘Correction to:Opto-Electronic Science https://www.oejournal.org/oes/article/doi/10.29026/oes.2024.230029 published online 21 March 2024.After the publication of this article1,it was brought to our attention that the inset image and absorption spectrum in Fig.1(b)contained a mistake,probably leading to misunderstandings.The inset image and the absorption spectrum in Fig.1(b)were not based on the specific batch of PbS colloidal quantum dots(CQDs)used in this work.
基金Financial support from the National Natural Science Foundation of China(22375024,21975031,21734009,51933001,22109080,and 52173174)the Natural Science Foundation of Shandong Province(No.ZR2022YQ45)+2 种基金the Taishan Scholars Program(Nos.tstp20221121 and tsqnz20221134)The Beijing Natural Science Foundation(No.2244073)supported by State Key Laboratory of Bio-Fibers and Eco-Textiles(Qingdao University)(RZ2200002821)is acknowledged.
文摘A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamino side groups,TT-Ph-C6 demonstrates excellent solubility and its crystal structure exhibits compact packing structures with a three-dimensional molecular stacking network.These structural attributes markedly promote exciton diffusion and charge carrier mobility,particularly advantageous for the fabrication of thick-film devices.TT-Ph-C6-based devices have attained a PCE of 18.01%at a film thickness of 100 nm,and even at a film thickness of 300 nm,the PCE remains at 14.64%,surpassing that of devices based on 2BTh-2F.These remarkable properties position TT-Ph-C6 as a highly promising NFREA material for boosting the efficiency of OSCs.
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.
基金supported by the National Science and Technology Major Project of China(2025ZD1406703)the Open Fund of Key Laboratory of Oil&Gas Equipment,Ministry of Education(Southwest Petroleum University)(Grant No.OGE20230206).
文摘Shock waves in the nozzle during supersonic separation under different conditions can disrupt the flow field’s thermodynamic equilibrium.While it contributes to the recovery of pressure energy,it also leads to the dissipation of mechanical energy.This study aimed to investigate the effects of changes in back pressure on the shock wave position and its subsequent impact on the refrigeration performance of nozzles.A mathematical model for the supersonic gas in a nozzle was established and evaluated via experiments.The results show that when the back pressure is less than 0.2 MPa,no shock wave is generated in the nozzle,and high refrigeration and liquefaction efficiency can be ensured while effective pressure recovery is achieved.When the back pressure(pb)is increased from 0.3 to 0.6 MPa,the refrigeration efficiency of the nozzle decreases,and the shock wave position(x shock)is advanced from 157 to 118 mm.The maximum Mach number(Ma)that can be reached by the fluid in the nozzle is reduced from 1.97 to 1.27.When the back pressure is increased from 0.2 to 0.6 MPa,the minimum temperature is increased by 55.18 K.When the back pressure is greater than 0.3 MPa,the Mach number upstream of the shock wave is reduced from 1.97 to 1.27,the shock wave intensity is weakened,and the thickness of the boundary layer separation caused by the shock wave is also decreased accordingly.Therefore,to ensure refrigeration efficiency,measures should be taken to control the back pressure within a reasonable range.
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 National Natural Science Foundation of China(No.62474114,52472225)Guangdong Basic and Applied Basic Research Foundation(2025A1515012041,2025A1515011515)China+1 种基金Science and Technology plan project of Shenzhen(JCYJ20240813141620027,20231122102326002)ChinaShenzhen University 2035 Program for Excellent Research(Grants 2024B003)。
文摘Despite being an excellent candidate for a photocathode,Cu_(2)ZnSnS_4(CZTS)performance is limited by suboptimal bulk and interfacial charge carrier dynamics.In this work,we introduce a facile and versatile CZTS precursor seed layer engineering technique,which significantly enhances crystal growth and mitigates detrimental defects in the postsulfurized CZTS light-absorbing films.This effective optimization of defects and charge carrier dynamics results in a highly efficient CZTS/CdS/TiO_(2)/Pt thin-film photocathode,achieving a record half-cell solar-to-hydrogen(HC-STH)conversion efficiency of 9.91%.Additionally,the photocathode exhibits a highest photocurrent density(J_(ph))of 29.44 m A cm^(-2)(at 0 VRHE)and favorable onset potential(Von)of 0.73 VRHE.Furthermore,our CTZS photocathode demonstrates a remarkable Jph of 16.54 m A cm^(-2)and HC-STH efficiency of 2.56%in natural seawater,followed by an impressive unbiased STH efficiency of 2.20%in a CZTS-BiVO_4 tandem cell.The scalability of this approach is underscored by the successful fabrication of a 4×4 cm^(2)module,highlighting its significant potential for practical,unbiased in situ solar seawater splitting applications.
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.
基金supported by the National Natural Science Foundation of China(42071238)the Jiuzhaigou Post-Disaster Restoration and Reconstruction Program(5132202020000046)+1 种基金the Second Tibetan Plateau Scientific Expedition and Research Program(STEP)the Ministry of Science and Technology of the People's Republic of China(2019QZKK0402)。
文摘Evaluating the effectivenes s of forest restoration projects is crucial for designing adaptive restoration strategies.However,existing studies have primarily focused on ecological outcomes while overlooking cost inputs.This gap can lead to increased uncertainties in restoration planning.Here we investigated forest dynamics in China's Upper Yangtze River Basin(UYRB)using kernel Normalized Difference Vegetation Index(kNDVI),Leaf Area Index(LAI),Gross Primary Productivity(GPP),Ku-band Vegetation Optical Depth(Ku-VOD)time series and climate data from1982 to 2020.Subsequently,we employed a residual trend analysis integrating temporal effects to determine the relative contributions of climate change and human activities to forest dynamics before and after the implementation of forest restoration engineering in 1998.Additionally,we developed an Afforestation Efficiency Index(AEI)to quantitatively assess the cost efficiency of afforestation projects.Results indicated that forest in the UYRB showed sustained increases during 1982-2020,with most areas experiencing greater growth after 1998 than before.Temporal effects of climatic factors influenced over 42.7%of the forest,and incorporating time-lag and cumulative effects enhanced climate-based explanations of forest variations by 1.61-24.73%.Human activities emerged as the dominant driver of forest dynamics post 1998,whereas climate variables predominated before this period.The cost-effectiveness of forest restoration projects in the UYRB typically ranges from moderate to high,with higher success predominantly observed in the northeastern and eastern counties,while the central,western,and northwestern counties mainly showed relatively low efficiency.These findings stress the need for assessing forest restoration outcomes from both ecological and cost perspectives,and can offer valuable insights for optimizing the layout of forest restoration initiatives in the UYRB.
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.
文摘The goal of the present work is to demonstrate the potential of Artificial Neural Network(ANN)-driven Genetic Algorithm(GA)methods for energy efficiency and economic performance optimization of energy efficiency measures in a multi-family house building in Greece.The energy efficiency measures include different heating/cooling systems(such as low-temperature and high-temperature heat pumps,natural gas boilers,split units),building envelope components for floor,walls,roof and windows of variable heat transfer coefficients,the installation of solar thermal collectors and PVs.The calculations of the building loads and investment and operating and maintenance costs of the measures are based on the methodology defined in Directive 2010/31/EU,while economic assumptions are based on EN 15459-1 standard.Typically,multi-objective optimization of energy efficiency measures often requires the simulation of very large numbers of cases involving numerous possible combinations,resulting in intense computational load.The results of the study indicate that ANN-driven GA methods can be used as an alternative,valuable tool for reliably predicting the optimal measures which minimize primary energy consumption and life cycle cost of the building with greatly reduced computational requirements.Through GA methods,the computational time needed for obtaining the optimal solutions is reduced by 96.4%-96.8%.
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support from the Heilongjiang Province"Double First Class"Discipline Collaborative Innovation Project(No.LJGXCG2023-061).
文摘Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions.In this study,we have tuned orbital hybridization states forming an interface enriched with sp^(2) hybridized carbon(sp^(2)-C),which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation.Benefiting from successfully constructed inorganic-rich SEI,the ICE increased to 91%and sodium storage capacity reached 346 mAh/g.Besides,the capacity retention rate was 90.7%after 700 cycles at 1 A/g higher than pristine electrode(83.8%).
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.
文摘A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.
基金supported by the Hubei Provincial Science and Technology Project,China(2025CSA039)the National Natural Science Foundation of China(32001467)。
文摘Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting density and N rate,and their relationships with grain yield,radiation use efficiency(RUE),and N use efficiency for grain production(NUEg)in rice.A two-year field experiment was conducted with two hybrid varieties under three N levels,0 kg ha^(-1)(N1),90 kg ha^(-1)(N2)and 180 kg ha^(-1)(N3),and two planting densities,22.2 hills m-2(D1)and 33.3 hills m^(-2)(D2).Results showed 3.4%higher yield and 4.4%higher NUEg under N2D2 compared with N3D1.The extinction coefficient for N(K_(N))and light(K_(L))and their ratio(K_(N)/K_(L))at heading stage were significantly influenced by N rate,planting density,and their interaction.K_(N)decreased with the increase of N input or planting density.Compared to N1,K_(N)decreased by 43.5 and 58.8%under N2 and N3,respectively,while K_(N)under D2 decreased by 16.0%compared to D1.Higher K_(L)and K_(N)/K_(L)values occurred under low N rates,with opposite trends under high N rates.Increased planting density led to decreased K_(L)and K_(N)/K_(L)values.N2D2 demonstrated higher K_(L)and K_(N),and thus comparable K_(N)/K_(L),compared to N3D1.Correlation analysis revealed K_(L)negatively correlated with RUE,while K_(N)and K_(N)/K_(L)positively correlated with NUEg.These findings indicate that increasing planting density under reduced N input could maintain rice yield while enhancing resource use efficiency through regulation of canopy light and N distribution.
