BACKGROUND RAS,BRAF,and mismatch repair(MMR)/microsatellite instability(MSI)are crucial biomarkers recommended by clinical practice guidelines for colorectal cancer(CRC).However,their characteristics and influencing f...BACKGROUND RAS,BRAF,and mismatch repair(MMR)/microsatellite instability(MSI)are crucial biomarkers recommended by clinical practice guidelines for colorectal cancer(CRC).However,their characteristics and influencing factors in Chinese patients have not been thoroughly described.AIM To analyze the clinicopathological features of KRAS,NRAS,BRAF,and PIK3CA mutations and the DNA MMR status in CRC.METHODS We enrolled 2271 Chinese CRC patients at the China-Japan Friendship Hospital.MMR proteins were tested using immunohistochemical analysis,and the KRAS/NRAS/BRAF/PIK3CA mutations were determined using quantitative polymerase chain reaction.Microsatellite status was determined using an MSI detection kit.Statistical analyses were conducted using SPSS software and logistic regression.RESULTS The KRAS,NRAS,BRAF,and PIK3CA mutations were detected in 44.6%,3.4%,3.7%,and 3.9% of CRC patients,respectively.KRAS mutations were more likely to occur in patients with moderate-to-high differentiation.BRAF mutations were more likely to occur in patients with right-sided CRC,poorly differentiated,or no perineural invasion.Deficient MMR(dMMR)was detected in 7.9% of all patients and 16.8% of those with mucinous adenocarcinomas.KRAS,NRAS,BRAF,and PIK3CA mutations were detected in 29.6%,1.1%,8.1%,and 22.3% of patients with dMMR,respectively.The dMMR was more likely to occur in patients with a family history of CRC,aged<50 years,right-sided CRC,poorly differentiated histology,no perineural invasion,and with carcinoma in situ,stage I,or stage II tumors.CONCLUSION This study analyzed the molecular profiles of KRAS,NRAS,BRAF,PIK3CA,and MMR/MSI in CRC,identifying key influencing factors,with implications for clinical management of CRC.展开更多
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a pro...In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.展开更多
Accumulative alternating back extrusion was a potential fine-grain modification method.In this paper,it was an innovative attempt to develop high-performance magnesium alloy sheet by this process.Under the condition o...Accumulative alternating back extrusion was a potential fine-grain modification method.In this paper,it was an innovative attempt to develop high-performance magnesium alloy sheet by this process.Under the condition of 350 K,commercial AZ31 magnesium alloy was made into billet by accumulative alternating back extrusion,and then extruded into fine-grain magnesium alloy sheet.Through a systematic study of its microstructure and mechanical properties,the results showed that the initial state had an important influence on the evolution of the structure during extrusion.After accumulative alternating back extrusion to produce the billet,the grain size of the sheet obtained by extrusion was significantly refined,which was related to the accumulation of deformation and grain refinement during the alternating loading process.Grain refinement caused the proportion of dynamic recrystallization inside the sheet with 2 cycles of accumulative alternating back extrusion to drop to 27%.With the increase of extrusion cycles from 2 to 4,the high density of dislocations led to an increase in the proportion of dynamic recrystallization and finer grains.The texture changed from strong basal texture to weak bimodal texture.The results of uniaxial tensile test show that due to grain refinement and texture change,the yield strength was significantly reduced,and the plasticity was significantly improved.It was verified that accumulative alternating back extrusion was meaningful for subsequent processing,and it also provided scientific guidance for the development of fine-grained magnesium alloy sheet.展开更多
Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable an...Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable and carbon–neutral societies. Much effort has been devoted to catalytic transformations of lignocellulosic biomass, the most abundant and nonedible form of biomass.展开更多
Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity ...Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity and superior lifespan.Herein,hexagonal Cs_(0.3)V_(2)O_(5)cathode is fabricated and investigated in zinc-ion batteries.Compared with the traditional vanadium oxides,the introduction of Cs changes the periodic atomic arrangements,which not only stabilizes the open framework structure but also facilitates the Zn^(2+)diffusion with a lower migration energy barrier.Consequently,high specific capacity of 543.8 mA h g^(-1)at 0.1 A g^(-1)is achieved,which surpasses most of reported cathode materials in zinc-ion batteries.The excellent cycle life is achieved over 1000 cycles with about 87.8%capacity retention at 2 A g^(-1).Furthermore,the morphological evolution and energy storage mechanisms are also revealed via a series of techniques.This work opens up a phase engineering strategy to fabricate the hexagonal vanadium oxide and elucidate the application of phase-dependent cathodes in zinc-ion batteries.展开更多
Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications.This paper reports a novel zero-dimensional perovskite,Rb_(4)CdCl_(6):Sn^(2+),Mn^(2+),which demons...Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications.This paper reports a novel zero-dimensional perovskite,Rb_(4)CdCl_(6):Sn^(2+),Mn^(2+),which demonstrates exceptional white-light properties including adjustable correlated color temperature,high color rendering index of up to 85,and near-unity photoluminescence quantum yield of 99%.Using a co-doping strategy involving Sn^(2+)and Mn^(2+),cyan-orange dual-band emission with complementary spectral ranges is activated by the self-trapped excitons and d-d transitions of the Sn^(2+)and Mn^(2+)centers in the Rb_(4)CdCl_(6)host,respectively.Intriguingly,although Mn^(2+)ions doped in Rb_(4)CdCl_(6)are difficult to excite,efficient Mn^(2+)emission can be realized through an ultra-high-efficient energy transfer between Sn^(2+)and Mn^(2+)via the formation of adjacent exchange-coupled Sn–Mn pairs.Benefiting from this efficient Dexter energy transfer process,the dual emission shares the same optimal excitation wavelengths of the Sn^(2+)centers and suppresses the non-radiative vibration relaxation significantly.Moreover,the relative intensities of the dual-emission components can be modulated flexibly by adjusting the fraction of the Sn^(2+)ions to the Sn–Mn pairs.This co-doping approach involving short-range energy transfer represents a promising avenue for achieving high-quality white light within a single material.展开更多
Lithium-selenium(Li-Se)batteries are deemed as an emerging high energy density electrochemical energy storage system owing to their high specific capacity and volume capacity.Prior to their practicality,a series of cr...Lithium-selenium(Li-Se)batteries are deemed as an emerging high energy density electrochemical energy storage system owing to their high specific capacity and volume capacity.Prior to their practicality,a series of critical challenges from the Se cathode side need to be overcome including low reactivity of bulk Se,shuttle effect of intermediates,sluggish redox kinetics of polyselenides,and volume change etc.In this review,recent progress on design strategies of functional Se cathodes are comprehensively summarized and discussed.Following the significance and key challenges,various efficient functionalized strategies for Se cathodes are presented,encompassing covalent bonding,nanostructure construction,heteroatom doping,component hybridization,and solid solution formation.Specially,the universality of these functional strategies are successfully extended into Na-Se batteries,K-Se batteries,and Mg-Se batteries.At last,a brief summary is made and some perspectives are offered with the goal of guiding future research advances and further exploration of these strategies.展开更多
Selective oxidation of biomass and its derivatives to dicarboxylic acids represents a promising route for biomass valorization.However,the co-presence of multiple functional groups in biomass molecules makes the selec...Selective oxidation of biomass and its derivatives to dicarboxylic acids represents a promising route for biomass valorization.However,the co-presence of multiple functional groups in biomass molecules makes the selective oxidation of particular functional a challenging task.Here,we demonstrate an efficient electrocatalytic system consisting of nickel oxide(NiO)and a nitroxyl radical,i.e.,2,2,6,6-tetrame thylpiperidine-1-oxyl(TEMPO)or 4-acetamido-TEMPO(ACT),for the selective oxidation of key bioplatform molecules including glucose,xylose and 5-hydroxymethylfurfural(HMF)into corresponding dicarboxylic acids,i.e.,glucaric acid,xylaric acid,and 2,5-furandicarboxylic acid(FDCA).NiO is clarified as the active catalyst for the oxidation of aldehyde in bio-platform molecules to carboxylic acid,while TEMPO or ACT is responsible for the oxidation of primary alcohol to aldehyde.The combination of NiO and TEMPO or ACT significantly accelerated the tandem oxidation of aldehyde and hydroxyl groups in glucose,xylose and HMF,thus achieving excellent yields(83%-99%)of dicarboxylic acids.Moreover,the combination catalyst enables the selective oxidation of glucose and xylose with high concentrations(e.g.,20 wt%),which offers a promising strategy for biomass valorization.展开更多
As a near-net-shape technology,the twin-roll strip casting(TRC)process can be considered to apply to the fabrication of TiAl alloy sheets.However,the control of the grain distribution is very important in strip castin...As a near-net-shape technology,the twin-roll strip casting(TRC)process can be considered to apply to the fabrication of TiAl alloy sheets.However,the control of the grain distribution is very important in strip casting because the mechanical properties of strips are directly determined by the solidification microstructure.A three-dimensional(3D)cellular automation finite-element(CAFE)model based on ProCAST software was established to simulate the solidification microstructure of Ti-43Al alloy.Then,the influence of casting temperature and the maximum nucleation density(nmax)on the solidification microstructure was investigated in detail.The simulation results provide a good explanation and prediction for the solidification microstructure in the molten pool before leaving the kissing point.Experimental and simulated microstructure show the common texture<001>orientation in the columnar grains zone.Finally,the microstructure evolution of the Ti-43Al alloy was analyzed and the solidification phase transformation path during the TSC process was determined,i.e.,L→L+β→β→β+α→α+γ+β/B2 phase under a faster cooling rate and L→L+β→β→β+α→γ+lamellar(α_(2)+γ)+β/B2 phase under a slower cooling rate.展开更多
The interactive alternating forward extrusion(AFE) method can realize the change of texture type and the weakening of texture strength.Taking AZ31 magnesium alloy as an example, the texture evolution of interactive AF...The interactive alternating forward extrusion(AFE) method can realize the change of texture type and the weakening of texture strength.Taking AZ31 magnesium alloy as an example, the texture evolution of interactive AFE was studied. The results show that all kinds of dynamic recrystallization(DRX) behaviors can weaken the texture to vary degrees. The weakening effect of twinning-induced recrystallization(TDRX)behavior was particularly significant. During the interactive AFE process, the c-axis of most grains rotated under the external force, and tended to be 90° angle with the ED direction, forming a stable fiber texture. In addition, with the increase of loading passes, the starting of {0001} <11–20> basal slip system became more and more difficult. The(10–10) texture formed by {10–10} <11–20> prismatic slip system after sixth passes was the main texture type. With the increase of forming temperature, the starting ability of {10–10} <11–20>prismatic slip systems increased, and the(10–10) texture formed by prismatic slip system above 623 K dominated.展开更多
Deep-ultraviolet(DUV)disinfection technology provides an expeditious and efficient way to suppress the transmission of coronavirus disease 2019(COVID-19).However,the influences of viral variants(Delta and Omicron)and ...Deep-ultraviolet(DUV)disinfection technology provides an expeditious and efficient way to suppress the transmission of coronavirus disease 2019(COVID-19).However,the influences of viral variants(Delta and Omicron)and low temperatures on the DUV virucidal efficacy are still unknown.Here,we developed a reliable and uniform planar light source comprised of 275-nm light-emitting diodes(LEDs)to investigate the effects of these two unknown factors and delineated the principle behind different disinfection performances.We found the lethal effect of DUV at the same radiation dose was reduced by the cryogenic environment,and a negative-U large-relaxation model was used to explain the difference in view of the photoelectronic nature.The chances were higher in the cryogenic environment for the capture of excited electrons within active genetic molecules back to the initial photo-ionised positions.Additionally,the variant of Omicron required a significantly higher DUV dose to achieve the same virucidal efficacy,and this was thanks to the genetic and proteinic characteristics of the Omicron.The findings in this study are important for human society using DUV disinfection in cold conditions(e.g.,the food cold chain logistics and the open air in winter),and the relevant DUV disinfection suggestion against COVID-19 is provided.展开更多
Li metal anode holds great promise to realize high-energy battery systems.However,the safety issue and limited lifetime caused by the uncontrollable growth of Li dendrites hinder its commercial application.Herein,an i...Li metal anode holds great promise to realize high-energy battery systems.However,the safety issue and limited lifetime caused by the uncontrollable growth of Li dendrites hinder its commercial application.Herein,an interlayer-bridged 3D lithiophilic rGO-Ag-S-CNT composite is proposed to guide uniform and stable Li plating/stripping.The 3D lithiophilic rGO-Ag-S-CNT host is fabricated by incorporating Ag-modified reduced graphene oxide(rGO)with S-doped carbon nanotube(CNT),where the rGO and CNT are closely connected via robust Ag-S covalent bond.This strong Ag-S bond could enhance the structural stability and electrical connection between rGO and CNT,significantly improving the electrochemical kinetics and uniformity of current distribution.Moreover,density functional theory calculation indicates that the introduction of Ag-S bond could further boost the binding energy between Ag and Li,which promotes homogeneous Li nucleation and growth.Consequently,the rGO-Ag-S-CNT-based anode achieves a lower overpotential(7.3 mV at 0.5 mA cm^(−2)),higher Coulombic efficiency(98.1%at 0.5 mA cm^(−2)),and superior long cycling performance(over 500 cycles at 2 mA cm−2)as compared with the rGO-Ag-CNT-and rGO-CNT-based anodes.This work provides a universal avenue and guidance to build a robust Li metal host via constructing a strong covalent bond,effectively suppressing the Li dendrites growth to prompt the development of Li metal battery.展开更多
Predicting potential facts in the future,Temporal Knowledge Graph(TKG)extrapolation remains challenging because of the deep dependence between the temporal association and semantic patterns of facts.Intuitively,facts(...Predicting potential facts in the future,Temporal Knowledge Graph(TKG)extrapolation remains challenging because of the deep dependence between the temporal association and semantic patterns of facts.Intuitively,facts(events)that happened at different timestamps have different influences on future events,which can be attributed to a hierarchy among not only facts but also relevant entities.Therefore,it is crucial to pay more attention to important entities and events when forecasting the future.However,most existing methods focus on reasoning over temporally evolving facts or mining evolutional patterns from known facts,which may be affected by the diversity and variability of the evolution,and they might fail to attach importance to facts that matter.Hyperbolic geometry was proved to be effective in capturing hierarchical patterns among data,which is considered to be a solution for modelling hierarchical relations among facts.To this end,we propose ReTIN,a novel model integrating real-time influence of historical facts for TKG reasoning based on hyperbolic geometry,which provides low-dimensional embeddings to capture latent hierarchical structures and other rich semantic patterns of the existing TKG.Considering both real-time and global features of TKG boosts the adaptation of ReTIN to the ever-changing dynamics and inherent constraints.Extensive experiments on benchmarks demonstrate the superiority of ReTIN over various baselines.The ablation study further supports the value of exploiting temporal information.展开更多
The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward mult...The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward multi-carbon(C_(2+))products.In this work,local CO_(2) and CO intermediate diffusion through the catalyst layer(CL)was investigated for improving CO_(2)RR toward C_(2+)products.The gas permeability tests and finite element simulation results indicated CL can balance the CO_(2) gas diffusion and residence time of the CO intermediate,leading to a sufficient CO concentration with a suitable CO_(2)/H_(2)O supply for high C_(2+)products.As a result,an excellent selectivity of C_(2+)products~79%at a high current density of 400 mA·cm^(-2) could be obtained on the optimal 500 nm Cu CL(Cu500).This work provides a new insight into the optimization of CO_(2)/H_(2)O supply and local CO concentration by controlling CL for C_(2+)products in CO_(2)RR flow cell.展开更多
The graphic design industry has been developing rapidly in recent years.People have begun to focus on steering the development of graphic design in the direction of localization,integrating more traditional Chinese el...The graphic design industry has been developing rapidly in recent years.People have begun to focus on steering the development of graphic design in the direction of localization,integrating more traditional Chinese elements,raising the level of acceptance toward graphic design content,and disseminating traditional culture on this basis.Ink art plays an important role in the historical and cultural development process.It uses simple color contrast to construct different situations and possesses unique artistic charm and cultural heritage.Incorporating ink elements into graphic design may enhance the graphic design style and provide inspiration.This article focuses on the reasons,advantages,and strategies of using ink art in graphic design imagery,hoping to provide references for graphic design activities.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 51704087)the Natural Science Foundation of Heilongjiang Province, China (No. LH2020E083)。
基金Supported by National High Level Hospital Clinical Research Funding,No.2023-NHLHCRF-YYPPLC-TJ-03.
文摘BACKGROUND RAS,BRAF,and mismatch repair(MMR)/microsatellite instability(MSI)are crucial biomarkers recommended by clinical practice guidelines for colorectal cancer(CRC).However,their characteristics and influencing factors in Chinese patients have not been thoroughly described.AIM To analyze the clinicopathological features of KRAS,NRAS,BRAF,and PIK3CA mutations and the DNA MMR status in CRC.METHODS We enrolled 2271 Chinese CRC patients at the China-Japan Friendship Hospital.MMR proteins were tested using immunohistochemical analysis,and the KRAS/NRAS/BRAF/PIK3CA mutations were determined using quantitative polymerase chain reaction.Microsatellite status was determined using an MSI detection kit.Statistical analyses were conducted using SPSS software and logistic regression.RESULTS The KRAS,NRAS,BRAF,and PIK3CA mutations were detected in 44.6%,3.4%,3.7%,and 3.9% of CRC patients,respectively.KRAS mutations were more likely to occur in patients with moderate-to-high differentiation.BRAF mutations were more likely to occur in patients with right-sided CRC,poorly differentiated,or no perineural invasion.Deficient MMR(dMMR)was detected in 7.9% of all patients and 16.8% of those with mucinous adenocarcinomas.KRAS,NRAS,BRAF,and PIK3CA mutations were detected in 29.6%,1.1%,8.1%,and 22.3% of patients with dMMR,respectively.The dMMR was more likely to occur in patients with a family history of CRC,aged<50 years,right-sided CRC,poorly differentiated histology,no perineural invasion,and with carcinoma in situ,stage I,or stage II tumors.CONCLUSION This study analyzed the molecular profiles of KRAS,NRAS,BRAF,PIK3CA,and MMR/MSI in CRC,identifying key influencing factors,with implications for clinical management of CRC.
基金supported by the Key Laboratory of Micro-systems and Micro-structures Manufacturing of Ministry of Education,Harbin Institute of Technology,China(No.2020KM005)the Natural Science Foundation of Heilongjiang Province,China(No.YQ2020E030)。
文摘In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.
基金This project is supported by National Natural Science Foundation of China(No.51975166)。
文摘Accumulative alternating back extrusion was a potential fine-grain modification method.In this paper,it was an innovative attempt to develop high-performance magnesium alloy sheet by this process.Under the condition of 350 K,commercial AZ31 magnesium alloy was made into billet by accumulative alternating back extrusion,and then extruded into fine-grain magnesium alloy sheet.Through a systematic study of its microstructure and mechanical properties,the results showed that the initial state had an important influence on the evolution of the structure during extrusion.After accumulative alternating back extrusion to produce the billet,the grain size of the sheet obtained by extrusion was significantly refined,which was related to the accumulation of deformation and grain refinement during the alternating loading process.Grain refinement caused the proportion of dynamic recrystallization inside the sheet with 2 cycles of accumulative alternating back extrusion to drop to 27%.With the increase of extrusion cycles from 2 to 4,the high density of dislocations led to an increase in the proportion of dynamic recrystallization and finer grains.The texture changed from strong basal texture to weak bimodal texture.The results of uniaxial tensile test show that due to grain refinement and texture change,the yield strength was significantly reduced,and the plasticity was significantly improved.It was verified that accumulative alternating back extrusion was meaningful for subsequent processing,and it also provided scientific guidance for the development of fine-grained magnesium alloy sheet.
基金support by the National Key R&D Program of China(2018YFB1501602)the National Natural Science Foundation of China(22121001 and 22172127)。
文摘Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable and carbon–neutral societies. Much effort has been devoted to catalytic transformations of lignocellulosic biomass, the most abundant and nonedible form of biomass.
基金financialy supported by the National Natural Science Foundation of China(Nos.22109140,21875221,and 22075223)Distinguished Young Scholars Innovation Team of Zhengzhou University(No.32320275)the Youth Talent Support Program of High-Level Talents Special Support Plan in Henan Province(ZYQR201810148)
文摘Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity and superior lifespan.Herein,hexagonal Cs_(0.3)V_(2)O_(5)cathode is fabricated and investigated in zinc-ion batteries.Compared with the traditional vanadium oxides,the introduction of Cs changes the periodic atomic arrangements,which not only stabilizes the open framework structure but also facilitates the Zn^(2+)diffusion with a lower migration energy barrier.Consequently,high specific capacity of 543.8 mA h g^(-1)at 0.1 A g^(-1)is achieved,which surpasses most of reported cathode materials in zinc-ion batteries.The excellent cycle life is achieved over 1000 cycles with about 87.8%capacity retention at 2 A g^(-1).Furthermore,the morphological evolution and energy storage mechanisms are also revealed via a series of techniques.This work opens up a phase engineering strategy to fabricate the hexagonal vanadium oxide and elucidate the application of phase-dependent cathodes in zinc-ion batteries.
基金support from the National Natural Science Foundation of China(Grant No.61874074)Science and Technology Project of Shenzhen(Grant No.JCYJ20220531100815034)+1 种基金H.L.acknowledges the support from Technology and Innovation Commission of Shenzhen(20200810164814001)Guangdong Basic and Applied Basic Research Foundation(General Program,Grant No.2022A1515012055).
文摘Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications.This paper reports a novel zero-dimensional perovskite,Rb_(4)CdCl_(6):Sn^(2+),Mn^(2+),which demonstrates exceptional white-light properties including adjustable correlated color temperature,high color rendering index of up to 85,and near-unity photoluminescence quantum yield of 99%.Using a co-doping strategy involving Sn^(2+)and Mn^(2+),cyan-orange dual-band emission with complementary spectral ranges is activated by the self-trapped excitons and d-d transitions of the Sn^(2+)and Mn^(2+)centers in the Rb_(4)CdCl_(6)host,respectively.Intriguingly,although Mn^(2+)ions doped in Rb_(4)CdCl_(6)are difficult to excite,efficient Mn^(2+)emission can be realized through an ultra-high-efficient energy transfer between Sn^(2+)and Mn^(2+)via the formation of adjacent exchange-coupled Sn–Mn pairs.Benefiting from this efficient Dexter energy transfer process,the dual emission shares the same optimal excitation wavelengths of the Sn^(2+)centers and suppresses the non-radiative vibration relaxation significantly.Moreover,the relative intensities of the dual-emission components can be modulated flexibly by adjusting the fraction of the Sn^(2+)ions to the Sn–Mn pairs.This co-doping approach involving short-range energy transfer represents a promising avenue for achieving high-quality white light within a single material.
基金the financial support from the National Key Research and Development Program of China(2019YFB2203400)the"111 Project"(B20030)ARC DP210102215。
文摘Lithium-selenium(Li-Se)batteries are deemed as an emerging high energy density electrochemical energy storage system owing to their high specific capacity and volume capacity.Prior to their practicality,a series of critical challenges from the Se cathode side need to be overcome including low reactivity of bulk Se,shuttle effect of intermediates,sluggish redox kinetics of polyselenides,and volume change etc.In this review,recent progress on design strategies of functional Se cathodes are comprehensively summarized and discussed.Following the significance and key challenges,various efficient functionalized strategies for Se cathodes are presented,encompassing covalent bonding,nanostructure construction,heteroatom doping,component hybridization,and solid solution formation.Specially,the universality of these functional strategies are successfully extended into Na-Se batteries,K-Se batteries,and Mg-Se batteries.At last,a brief summary is made and some perspectives are offered with the goal of guiding future research advances and further exploration of these strategies.
基金financial supported by the National Key R&D program of China(2018YFB1501602)the National Natural Science Foundation of China(22121001,22172127 and 91945301)。
文摘Selective oxidation of biomass and its derivatives to dicarboxylic acids represents a promising route for biomass valorization.However,the co-presence of multiple functional groups in biomass molecules makes the selective oxidation of particular functional a challenging task.Here,we demonstrate an efficient electrocatalytic system consisting of nickel oxide(NiO)and a nitroxyl radical,i.e.,2,2,6,6-tetrame thylpiperidine-1-oxyl(TEMPO)or 4-acetamido-TEMPO(ACT),for the selective oxidation of key bioplatform molecules including glucose,xylose and 5-hydroxymethylfurfural(HMF)into corresponding dicarboxylic acids,i.e.,glucaric acid,xylaric acid,and 2,5-furandicarboxylic acid(FDCA).NiO is clarified as the active catalyst for the oxidation of aldehyde in bio-platform molecules to carboxylic acid,while TEMPO or ACT is responsible for the oxidation of primary alcohol to aldehyde.The combination of NiO and TEMPO or ACT significantly accelerated the tandem oxidation of aldehyde and hydroxyl groups in glucose,xylose and HMF,thus achieving excellent yields(83%-99%)of dicarboxylic acids.Moreover,the combination catalyst enables the selective oxidation of glucose and xylose with high concentrations(e.g.,20 wt%),which offers a promising strategy for biomass valorization.
基金supported by the National Natural Science Foundation of China(52071065)National Key Research and Development Program of China(2016YFB0301201)the Fundamental Research Funds for the Central Universities(N160713001).
文摘As a near-net-shape technology,the twin-roll strip casting(TRC)process can be considered to apply to the fabrication of TiAl alloy sheets.However,the control of the grain distribution is very important in strip casting because the mechanical properties of strips are directly determined by the solidification microstructure.A three-dimensional(3D)cellular automation finite-element(CAFE)model based on ProCAST software was established to simulate the solidification microstructure of Ti-43Al alloy.Then,the influence of casting temperature and the maximum nucleation density(nmax)on the solidification microstructure was investigated in detail.The simulation results provide a good explanation and prediction for the solidification microstructure in the molten pool before leaving the kissing point.Experimental and simulated microstructure show the common texture<001>orientation in the columnar grains zone.Finally,the microstructure evolution of the Ti-43Al alloy was analyzed and the solidification phase transformation path during the TSC process was determined,i.e.,L→L+β→β→β+α→α+γ+β/B2 phase under a faster cooling rate and L→L+β→β→β+α→γ+lamellar(α_(2)+γ)+β/B2 phase under a slower cooling rate.
基金supported by National Natural Science Foundation of China (no. 51975166)。
文摘The interactive alternating forward extrusion(AFE) method can realize the change of texture type and the weakening of texture strength.Taking AZ31 magnesium alloy as an example, the texture evolution of interactive AFE was studied. The results show that all kinds of dynamic recrystallization(DRX) behaviors can weaken the texture to vary degrees. The weakening effect of twinning-induced recrystallization(TDRX)behavior was particularly significant. During the interactive AFE process, the c-axis of most grains rotated under the external force, and tended to be 90° angle with the ED direction, forming a stable fiber texture. In addition, with the increase of loading passes, the starting of {0001} <11–20> basal slip system became more and more difficult. The(10–10) texture formed by {10–10} <11–20> prismatic slip system after sixth passes was the main texture type. With the increase of forming temperature, the starting ability of {10–10} <11–20>prismatic slip systems increased, and the(10–10) texture formed by prismatic slip system above 623 K dominated.
基金supported by the National Key R&D Program of China(2022YFB3605002)the Key Scientific and Technological Program of Xiamen(3502Z20211002).
文摘Deep-ultraviolet(DUV)disinfection technology provides an expeditious and efficient way to suppress the transmission of coronavirus disease 2019(COVID-19).However,the influences of viral variants(Delta and Omicron)and low temperatures on the DUV virucidal efficacy are still unknown.Here,we developed a reliable and uniform planar light source comprised of 275-nm light-emitting diodes(LEDs)to investigate the effects of these two unknown factors and delineated the principle behind different disinfection performances.We found the lethal effect of DUV at the same radiation dose was reduced by the cryogenic environment,and a negative-U large-relaxation model was used to explain the difference in view of the photoelectronic nature.The chances were higher in the cryogenic environment for the capture of excited electrons within active genetic molecules back to the initial photo-ionised positions.Additionally,the variant of Omicron required a significantly higher DUV dose to achieve the same virucidal efficacy,and this was thanks to the genetic and proteinic characteristics of the Omicron.The findings in this study are important for human society using DUV disinfection in cold conditions(e.g.,the food cold chain logistics and the open air in winter),and the relevant DUV disinfection suggestion against COVID-19 is provided.
基金This work is supported by Singapore Ministry of Education academic research grant Tier 2 (MOE2019-T2-1-181).
文摘Li metal anode holds great promise to realize high-energy battery systems.However,the safety issue and limited lifetime caused by the uncontrollable growth of Li dendrites hinder its commercial application.Herein,an interlayer-bridged 3D lithiophilic rGO-Ag-S-CNT composite is proposed to guide uniform and stable Li plating/stripping.The 3D lithiophilic rGO-Ag-S-CNT host is fabricated by incorporating Ag-modified reduced graphene oxide(rGO)with S-doped carbon nanotube(CNT),where the rGO and CNT are closely connected via robust Ag-S covalent bond.This strong Ag-S bond could enhance the structural stability and electrical connection between rGO and CNT,significantly improving the electrochemical kinetics and uniformity of current distribution.Moreover,density functional theory calculation indicates that the introduction of Ag-S bond could further boost the binding energy between Ag and Li,which promotes homogeneous Li nucleation and growth.Consequently,the rGO-Ag-S-CNT-based anode achieves a lower overpotential(7.3 mV at 0.5 mA cm^(−2)),higher Coulombic efficiency(98.1%at 0.5 mA cm^(−2)),and superior long cycling performance(over 500 cycles at 2 mA cm−2)as compared with the rGO-Ag-CNT-and rGO-CNT-based anodes.This work provides a universal avenue and guidance to build a robust Li metal host via constructing a strong covalent bond,effectively suppressing the Li dendrites growth to prompt the development of Li metal battery.
基金Major Key Project of Pengcheng Laboratory,Grant/Award Number:PCL2022A03。
文摘Predicting potential facts in the future,Temporal Knowledge Graph(TKG)extrapolation remains challenging because of the deep dependence between the temporal association and semantic patterns of facts.Intuitively,facts(events)that happened at different timestamps have different influences on future events,which can be attributed to a hierarchy among not only facts but also relevant entities.Therefore,it is crucial to pay more attention to important entities and events when forecasting the future.However,most existing methods focus on reasoning over temporally evolving facts or mining evolutional patterns from known facts,which may be affected by the diversity and variability of the evolution,and they might fail to attach importance to facts that matter.Hyperbolic geometry was proved to be effective in capturing hierarchical patterns among data,which is considered to be a solution for modelling hierarchical relations among facts.To this end,we propose ReTIN,a novel model integrating real-time influence of historical facts for TKG reasoning based on hyperbolic geometry,which provides low-dimensional embeddings to capture latent hierarchical structures and other rich semantic patterns of the existing TKG.Considering both real-time and global features of TKG boosts the adaptation of ReTIN to the ever-changing dynamics and inherent constraints.Extensive experiments on benchmarks demonstrate the superiority of ReTIN over various baselines.The ablation study further supports the value of exploiting temporal information.
基金The authors gratefully thank the National Natural Science Foundation of China(No.22002189)Central South University Research Programme of Advanced Interdisciplinary Studies(No.2023QYJC012)+1 种基金Central South University Innovation-Driven Research Program(No.2023CXQD042)the Fundamental Research Funds for the Central Universities of Central South University(No.2023ZZTS0962).
文摘The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward multi-carbon(C_(2+))products.In this work,local CO_(2) and CO intermediate diffusion through the catalyst layer(CL)was investigated for improving CO_(2)RR toward C_(2+)products.The gas permeability tests and finite element simulation results indicated CL can balance the CO_(2) gas diffusion and residence time of the CO intermediate,leading to a sufficient CO concentration with a suitable CO_(2)/H_(2)O supply for high C_(2+)products.As a result,an excellent selectivity of C_(2+)products~79%at a high current density of 400 mA·cm^(-2) could be obtained on the optimal 500 nm Cu CL(Cu500).This work provides a new insight into the optimization of CO_(2)/H_(2)O supply and local CO concentration by controlling CL for C_(2+)products in CO_(2)RR flow cell.
文摘The graphic design industry has been developing rapidly in recent years.People have begun to focus on steering the development of graphic design in the direction of localization,integrating more traditional Chinese elements,raising the level of acceptance toward graphic design content,and disseminating traditional culture on this basis.Ink art plays an important role in the historical and cultural development process.It uses simple color contrast to construct different situations and possesses unique artistic charm and cultural heritage.Incorporating ink elements into graphic design may enhance the graphic design style and provide inspiration.This article focuses on the reasons,advantages,and strategies of using ink art in graphic design imagery,hoping to provide references for graphic design activities.