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Single-atom modified graphene cocatalyst for enhanced photocatalytic CO_(2)reduction on halide perovskite
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作者 Hui Fu Jin Tian +5 位作者 Qianqian Zhang Zhaoke Zheng Hefeng Cheng Yuanyuan Liu Baibiao Huang Peng Wang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期143-151,共9页
Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2)reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.Howev... Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2)reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.However,photoreduction of CO_(2)by MHP remains a challenge because of the slow charge separation and transfer.Herein,a cobalt single-atom modified nitrogen-doped graphene(Co-NG)cocatalyst is prepared for enhanced photocatalytic CO_(2)reduction of bismuth-based MHP Cs_(3)Bi_(2)Br_(9).The optimal Cs_(3)Bi_(2)Br_(9)/Co-NG composite exhibits the CO production rate of 123.16μmol g-1 h-1,which is 17.3 times higher than that of Cs_(3)Bi_(2)Br_(9).Moreover,the Cs_(3)Bi_(2)Br_(9)/Co-NG composite photocatalyst exhibits nearly 100%CO selectivity as well as impressive long-term stability.Charge carrier dynamic characterizations such as Kelvin probe force microscopy(KPFM),single-particle PL microscope and transient absorption(TA)spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance.The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement.In addition,in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers,demonstrating that the introduction of Co-NG promotes the formation of~(*)COOH intermediate,providing sufficient evidence for the highly selective generation of CO.This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO_(2)reduction and is expected to shed light on other photocatalytic applications. 展开更多
关键词 Bismuth-based perovskite Photocatalysis CO_(2)reduction Single-atom cocatalyst Charge separation
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Higher-order mode analysis for SOLEIL-type superconducting cavity
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作者 Xiyuan Chai Qin Li +3 位作者 Yunpeng Xu Yungai Tang Mingsheng Tan Cong-Feng Wu 《中国科学技术大学学报》 CAS CSCD 北大核心 2024年第7期56-65,55,I0003,共12页
A 499.8 MHz SOLEIL-type superconducting cavity was simulated and designed for the first time in this paper.The higher-order mode(HOM)properties of the cavity were investigated.Two kinds of coaxial HOM couplers were de... A 499.8 MHz SOLEIL-type superconducting cavity was simulated and designed for the first time in this paper.The higher-order mode(HOM)properties of the cavity were investigated.Two kinds of coaxial HOM couplers were designed.Using 4 L-type and 4 T-type HOM couplers,the longitudinal impedance and the transverse impedances were suppressed to below 3 kΩand 30 kΩ/m,respectivly.The HOM damping requirements of Hefei Advanced Light Facility(HALF)were satisfied.This paper conducted an in-depth study on the radio frequency(RF)design,multipacting optimization,and thermal analysis of these coaxial couplers.Simulation results indicated that under operating acceleration voltage,the optimized couplers does not exhibit multiplicating or thermal breakdown phenomena.The cavity has the potential to reach a higher acceleration gradient. 展开更多
关键词 HOM coupler superconducting cavity RF system multipacting thermal simulation
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Tailoring the microenvironment of Ti sites in Ti-containing materials for synergizing with Au sites to boost propylene epoxidation
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作者 Shudong Shi Zhihua Zhang +3 位作者 Yundao Jing Wei Du Xuezhi Duan Xinggui Zhou 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期133-143,共11页
Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species for... Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species formed on Au sites diffuses to the Ti sites to form the Ti-hydroperoxo intermedi-ates and contributes to the formation of propylene oxide(PO).In principle,thermal treatment will significantly affect the chemical and physical structures of Ti-containing materials.Consequently,the synergy between tailored Ti sites with different surface properties and Au sites is highly ex-pected to enhance the catalytic performance for the reaction.Herein,we systematically studied the intrinsic effects of different microenvironments around Ti sites on the PO adsorption/desorption and conversion,and then effectively improved the catalytic performance by tailoring the number of surface hydroxyl groups.The Ti^(Ⅵ)material with fewer hydroxyls stimulates a remarkable enhance-ment in PO selectivity and H_(2)efficiency compared to the Ti^(Ⅵ)material that possessed more hydrox-yls,offering a 7-fold and 4-fold increase,respectively.As expected,the Ti^(Ⅵ)+Ⅳand Ti^(Ⅳ)materials also exhibit a similar phenomenon to the Ti^(Ⅵ)materials through the same thermal treatment,which strongly supports that the Ti sites microenvironment is an important factor in suppressing PO con-version and enhancing catalytic performance.These insights could provide guidance for the rational preparation and optimization of Ti-containing materials synergizing with Au catalysts for propylene epoxidation. 展开更多
关键词 Propylene epoxidation MICROENVIRONMENT Ti-containing material Au-Ti synergy Hydroxyl group
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Enhancing selectivity in acidic CO_(2)electrolysis:Cation effects and catalyst innovation
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作者 Zichao Huang Tinghui Yang +4 位作者 Yingbing Zhang Chaoqun Guan Wenke Gui Min Kuang Jianping Yang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期61-80,共20页
The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral elec-trolytes,their efficie... The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral elec-trolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2)conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2)electrolysis.It commences with an overview of the latest advancements in acidic CO_(2)electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2)elec-trolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2)electrolysis are suggested. 展开更多
关键词 ACIDIC CO_(2)electrolysis High selectivity Cation effects Catalyst design Competitive HER
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Boosting photocatalytic hydrogen evolution enabled by SiO_(2)-supporting chiral covalent organic frameworks with parallel stacking sequence
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作者 Zheng Lin Wanting Xie +2 位作者 Mengjing Zhu Changchun Wang Jia Guo 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期87-97,共11页
Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilita... Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer,but the precise ordered alignment is limited due to the non-covalentπ-stacking of COF layers,accordingly hindering out-of-plane transfer kinetics.Herein,we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO_(2) microsphere.Compared to the achiral COF analogues,the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration,thereby affording superior photocatalytic performance in hydrogen evolution from water splitting.Taking the simplest ketoenamine-linked chiral COF as a shell of SiO_(2) particle,the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^(-1)h^(-1)along with the apparent quantum efficiency of 14.31%at 475 nm.Furthermore,the composite photocatalysts could be fabricated into a film device,displaying a remarkable photocatalytic performance of 178.0 mmol m^(-2)h^(-1)for hydrogen evolution.Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties. 展开更多
关键词 Covalent organic framework PHOTOCATALYSIS Hydrogen generation Chiral induction Core-shell structure
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In-situ thermal Raman mapping and stress analysis of CNT/CF/epoxy interfaces
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作者 HE Jing-zong CHEN Shi +2 位作者 MA Zheng-kun LU Yong-gen WU Qi-lin 《新型炭材料(中英文)》 SCIE EI CAS CSCD 北大核心 2024年第4期703-714,共12页
A study of the interfacial behavior and internal thermal stress distribution in fiber-reinforced composites is essential to assess their performance and reliability.CNT/carbon fiber(CF)hybrid fibers were constructed u... A study of the interfacial behavior and internal thermal stress distribution in fiber-reinforced composites is essential to assess their performance and reliability.CNT/carbon fiber(CF)hybrid fibers were constructed using electrophoretic deposition.The interfacial properties of CF/epoxy and CNT/CF/epoxy composites were statistically investigated and compared using in-situ thermal Raman mapping by dispersing CNTs as a Raman sensing medium(CNT_(R))in a resin.The associated local thermal stress changes can be simulated by capturing the G'band position distribution of CNT_(R) in the epoxy at different temperatures.It was found that the G'band shifted to lower positions with increasing temperature,reaching a maximum difference of 2.43 cm^(−1) at 100℃.The interfacial bonding between CNT/CF and the matrix and the stress distribution and changes during heat treatment(20-100℃)were investig-ated in detail.This work is important for studying thermal stress in fiber-reinforced composites by in-situ thermal Raman mapping technology. 展开更多
关键词 Thermal Raman mapping Stress distribution Carbon fiber Carbon nanotube Interface
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Characteristic analysis of 1.06μm long-cavity diode lasers based on asymmetric waveguide structures
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作者 ZHAO Ren-Ze GAO Xin +3 位作者 FU Ding-Yang ZHANG Yue SU Peng BO Bao-Xue 《红外与毫米波学报》 SCIE EI CAS CSCD 北大核心 2024年第4期557-562,共6页
In long-cavity edge-emitting diode lasers,longitudinal spatial hole burning(LSHB),two-photon ab⁃sorption(TPA)and free carrier absorption(FCA)are among the key factors that affect the linear increase in out⁃put power a... In long-cavity edge-emitting diode lasers,longitudinal spatial hole burning(LSHB),two-photon ab⁃sorption(TPA)and free carrier absorption(FCA)are among the key factors that affect the linear increase in out⁃put power at high injection currents.In this paper,a simplified numerical analysis model is proposed for 1.06μm long-cavity diode lasers by combining TPA and FCA losses with one-dimensional(1D)rate equations.The ef⁃fects of LSHB,TPA and FCA on the output characteristics are systematically analyzed,and it is proposed that ad⁃justing the front facet reflectivity and the position of the quantum well(QW)in the waveguide layer can improve the front facet output power. 展开更多
关键词 diode lasers longitudinal spatial hole burning free carrier absorption two-photon absorption
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Realizing efficient electrochemical oxidation of 5-hydroxymethylfurfural on a freestanding Ni(OH)_(2)/nickel foam catalyst
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作者 Yunying Huo Cong Guo +6 位作者 Yongle Zhang Jingyi Liu Qiao Zhang Zhiting Liu Guangxing Yang Rengui Li Feng Peng 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期282-291,共10页
With the continuous improvement of solar energy production capacity,how to effectively use the electricity generated by renewable solar energy for electrochemical conversion of biomass is a hot topic.Electrochemical c... With the continuous improvement of solar energy production capacity,how to effectively use the electricity generated by renewable solar energy for electrochemical conversion of biomass is a hot topic.Electrochemical conversion of 5-hydroxymethylfurfural(HMF)to biofuels and value-added oxygenated commodity chemicals provides a promising and alternative pathway to convert re-newable electricity into chemicals.Although nickel-based eletrocatalysts are well-known for HMF oxidation,their relatively low intrinsic activity,poor conductivity and stability still limit the poten-tial applications.Here,we report the fabrication of a freestanding nickel-based electrode,in which Ni(OH)2 species were in-situ constructed on Ni foam(NF)support using a facile ac-id-corrosion-induced strategy.The Ni(OH)2/NF electrocatalyst exhibits stable and efficient electro-chemical HMF oxidation into 2,5-furandicarboxylic acid(FDCA)with HMF conversion close to 100%with high Faraday efficiency.In-situ formation strategy results in a compact interface between Ni(OH)2 and NF,which contributes to good conductivity and stability during electrochemical reac-tions.The superior performance benefits from dynamic cyclic evolution of Ni(OH)2 to NiOOH,which acts as the reactive species for HMF oxidation to FDCA.A scaled-up device based on a continu-ous-flow electrolytic cell was also established,giving stable operation with a high FDCA production rate of 27 mg h^(-1)cm^(−2).This job offers a straightforward,economical,and scalable design strategy to design efficient and durable catalysts for electrochemical conversion of valuable chemicals. 展开更多
关键词 Acid-corrosion-induced 5-HYDROXYMETHYLFURFURAL Electrocatalytic oxidation Ni electrocatalysis
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C-H bond activation of propane on Ga_(2)O_(2)^(2+)in Ga/H-ZSM-5 and its mechanistic implications
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作者 Zhaoqi Zhao Yunzhu Zhong +1 位作者 Xiaoxia Chang Bingjun Xu 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期32-43,共12页
Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+)stabilized by framework Al pairs have been identified a... Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+)stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work.Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+)species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+)species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio.This disparity in Ga_(2)O_(2)^(2+)species stems from their differing capacity in completing the catalytic cycle.Spectroscopic results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+)species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+)species corresponding to GaHHW. 展开更多
关键词 Propane dehydrogenation Ga2O22+ Activation of C-H bond Ga species
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Engineering the coordination structure of Cu for enhanced photocatalytic production of C_(1)chemicals from glucose
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作者 Lulu Sun Shiyang Liu +3 位作者 Taifeng Liu Dongqiang Lei Nengchao Luo Feng Wang 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期234-243,共10页
Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1)chemicals requires the cleavage of robust C−C bonds in sugars wit... Photocatalytic decomposition of sugars is a promising way of providing H_(2),CO,and HCOOH as sus-tainable energy vectors.However,the production of C_(1)chemicals requires the cleavage of robust C−C bonds in sugars with concurrent production of H_(2),which remains challenging.Here,the photo-catalytic activity for glucose decomposition to HCOOH,CO(C_(1)chemicals),and H_(2)on Cu/TiO_(2)was enhanced by nitrogen doping.Owing to nitrogen doping,atomically dispersed and stable Cu sites resistant to light irradiation are formed on Cu/TiO_(2).The electronic interaction between Cu and nitrogen ions originates valence band structure and defect levels composed of N 2p orbit,distinct from undoped Cu/TiO_(2).Therefore,the lifetime of charge carriers is prolonged,resulting in the pro-duction of C_(1)chemicals and H_(2)with productivities 1.7 and 2.1 folds that of Cu/TiO_(2).This work pro-vides a strategy to design coordinatively stable Cu ions for photocatalytic biomass conversion. 展开更多
关键词 Cu photocatalyst Coordination structure BIOMASS C−C bond C_(1)chemicals
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Superposition of dual electric fields in covalent organic frameworks for efficient photocatalytic hydrogen evolution
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作者 Chao Li Shuo Wang +8 位作者 Yuan Liub Xihe Huang Yan Zhuang Shuhong Wu Ying Wang Na Wen Kaifeng Wu Zhengxin Ding Jinlin Long 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第8期164-175,共12页
Covalent organic frameworks(COFs)are promising materials for converting solar energy into green hydrogen.However,limited charge separation and transport in COFs impede their application in the photocatalytic hydrogen ... Covalent organic frameworks(COFs)are promising materials for converting solar energy into green hydrogen.However,limited charge separation and transport in COFs impede their application in the photocatalytic hydrogen evolution reaction(HER).In this study,the intrinsically tunable inter-nal bond electric field(IBEF)at the imine bonds of COFs was manipulated to cooperate with the internal molecular electric field(IMEF)induced by the donor-acceptor(D-A)structure for an effi-cient HER.The aligned orientation of IBEF and IMEF resulted in a remarkable H_(2)evolution rate of 57.3 mmol·g^(-1)·h^(-1)on TNCA,which was approximately 520 times higher than that of TCNA(0.11 mmol·g^(-1)·h^(-1))with the opposing electric field orientation.The superposition of the dual electric fields enables the IBEF to function as an accelerating field for electron transfer,kinetically facilitat-ing the migration of photogenerated electrons from D to A.Furthermore,theoretical calculations indicate that the inhomogeneous charge distribution at the C and N atoms in TNCA not only pro-vides a strong driving force for carrier transfer but also effectively hinders the return of free elec-trons to the valence band,improving the utilization of photoelectrons.This strategy of fabricating dual electric fields in COFs offers a novel approach to designing photocatalysts for clean energy synthesis. 展开更多
关键词 Covalent organic framework Internal molecular electric field Internal bond electric field PHOTOCATALYSIS Hydrogen evolution
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Freestanding oxide membranes:synthesis,tunable physical properties,and functional devices
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作者 Ao Wang Jinfeng Zhang Lingfei Wang 《中国科学技术大学学报》 CAS CSCD 北大核心 2024年第7期2-17,1,I0002,共18页
The study of oxide heteroepitaxy has been hindered by the issues of misfit strain and substrate clamping,which impede both the optimization of performance and the acquisition of a fundamental understanding of oxide sy... The study of oxide heteroepitaxy has been hindered by the issues of misfit strain and substrate clamping,which impede both the optimization of performance and the acquisition of a fundamental understanding of oxide systems.Recently,however,the development of freestanding oxide membranes has provided a plausible solution to these substrate limitations.Single-crystalline functional oxide films can be released from their substrates without incurring significant damage and can subsequently be transferred to any substrate of choice.This paper discusses recent advancements in the fabrication,adjustable physical properties,and various applications of freestanding oxide perovskite films.First,we present the primary strategies employed for the synthesis and transfer of these freestanding perovskite thin films.Second,we explore the main functionalities observed in freestanding perovskite oxide thin films,with special attention to the tunable functionalities and physical properties of these freestanding perovskite membranes under varying strain states.Next,we encapsulate three representative devices based on freestanding oxide films.Overall,this review highlights the potential of freestanding oxide films for the study of novel functionalities and flexible electronics. 展开更多
关键词 freestanding oxide membranes transition metal oxides thin films electronic devices
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Charge-balanced codoping enables exceeding doping limit and ultralow thermal conductivity
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作者 Long Chen Chun Wang +3 位作者 Lin Wang Minghao Wang Yongchun Zhu Changzheng Wu 《中国科学技术大学学报》 CAS CSCD 北大核心 2024年第6期1-7,I0009,共8页
Materials with low thermal conductivity are applied extensively in energy management,and breaking the amorphous limits of thermal conductivity to solids has attracted widespread attention from scientists.Doping is a c... Materials with low thermal conductivity are applied extensively in energy management,and breaking the amorphous limits of thermal conductivity to solids has attracted widespread attention from scientists.Doping is a common strategy for achieving low thermal conductivity that can offer abundant scattering centers in which heavier dopants always result in lower phonon group velocities and lower thermal conductivities.However,the amount of equivalent heavyatom single dopant available is limited.Unfortunately,nonequivalent heavy dopants have finite solubility because of charge imbalance.Here,we propose a charge balance strategy for SnS by substituting Sn2+with Ag^(+)and heavy Bi^(3+),improving the doping limit of Ag from 2%to 3%.Ag and Bi codoping increases the point defect concentration and introduces abundant boundaries simultaneously,scattering the phonons at both the atomic scale and nanoscale.The thermal conductivity of Ag0.03Bi0.03Sn0.94S decreased to 0.535 W·m^(−1)·K^(−1)at room temperature and 0.388 W·m^(−1)·K^(−1)at 275°C,which is below the amorphous limit of 0.450 W·m^(−1)·K^(−1)for SnS.This strategy offers a simple way to enhance the doping limit and achieve ultralow thermal conductivity in solids below the amorphous limit without precise structural modification. 展开更多
关键词 charge-balanced codoping heavy atom point defect grain boundary ultralow thermal conductivity
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Damage effect and mechanisms of cyclophosphamide to human neuroblastoma SH-SY5Y cells
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作者 LI Jiajia WANG Jiao +4 位作者 XIAO Wenyi WEI Donghui ZHANG Yongxiang JIANG Ning ZHOU Wenxia 《中国药理学与毒理学杂志》 CAS 北大核心 2024年第8期561-574,共14页
OBJECTIVE To investigate the damage effect and mechanisms of cyclophosphamide(CTX)and its active metabolite derivative 4-hydroperoxycyclophosphamide(4-HC)to human neuroblas⁃toma SH-SY5Y cells.METHODS SH-SY5Y cells wer... OBJECTIVE To investigate the damage effect and mechanisms of cyclophosphamide(CTX)and its active metabolite derivative 4-hydroperoxycyclophosphamide(4-HC)to human neuroblas⁃toma SH-SY5Y cells.METHODS SH-SY5Y cells were treated with CTX[0(cell control),0.01,0.1,1,5,10,20,40 and 80 mmol·L^(-1)]and 4-HC[0(cell control),0.01,0.1,1,5,10,20,40 and 80μmol·L^(-1)]for 48 h.Cell confluence and morphology were observed by the IncuCyte ZOOM system.Cell viability was assessed by CCK-8 assay.Lactate dehydrogenase(LDH)release was measured by LDH assay kit.SH-SY5Y cells were treated with CTX(0,1,5,10 and 20 mmol·L^(-1))and 4-HC(0,1,5,10 and 20μmol·L^(-1))for 48 h before cell proliferation was analyzed by 5-ethynyl-2′-deoxyuridine(EdU)staining assay.Immunofluorescence was employed to assess the levels of the DNA double-strand break markerγ-H2AX and to evaluate changes in mitochondrial membrane potential.SH-SY5Y cells were treated with CTX(0,1,5 and 10 mmol·L^(-1))and 4-HC(0,1,5 and 10μmol·L^(-1))for 48 h,and the alterations in glycolysis and oxidative phosphorylation levels were analyzed using the Seahorse XFe96 Analyzer.RESULTS Compared with the cell control group,cell confluence and cell viability were significantly reduced in the CTX and 4-HC groups(P<0.01),and the half-maximal inhibitory concentrations(IC50)for CTX and 4-HC were 4.44 mmol·L^(-1) and 4.78μmol·L^(-1),respectively.The release rate of LDH was signif⁃icantly increased while the percentage of EdU+cells was significantly reduced in the CTX and 4-HC groups(P<0.01).The percentage ofγ-H2AX+cells was significantly increased and mitochondrial membrane potential significantly decreased in the CTX and 4-HC group(P<0.05).Treatment with CTX and 4-HC resulted in reduced levels of maximum glycolytic capacity,glycolytic reserve,maximal respi⁃ration,and ATP production(P<0.05).CONCLUSION CTX and 4-HC exert significant cytotoxic effects on SH-SY5Y cells by disrupting cell membrane structure,impeding cell proliferation,and reducing cell viability.The mechanisms underlying these effects may involve intracellular DNA damage,disturbance of energy metabolism and mitochondrial dysfunction. 展开更多
关键词 CYCLOPHOSPHAMIDE 4-hydroperoxycyclophosphamide NEUROTOXICITY energy metabolism
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Single atom doping induced charge-specific distribution of Cu1-TiO_(2)for selective aniline oxidation via a new mechanism
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作者 Jiaheng Qin Wantong Zhao +6 位作者 Jie Song Nan Luo Zheng-Lan Ma Baojun Wang Jiantai Ma Riguang Zhang Yu Long 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第9期98-111,共14页
Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile... Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile,identifying the active site also represents a significant obstacle,primarily due to the intricate electronic environment of single atom site doped metal oxide.Herein,a single atom Cu doped TiO_(2)catalyst(Cu_(1)-TiO_(2))is prepared via a simple“colloid-acid treatment”strategy,which switches aniline oxidation selectivity of TiO_(2)from azoxybenzene to nitrosobenzene,without using additives or changing solvent,while other metal or nonmetal doped TiO_(2)did not possess.Comprehensive mechanistic investigations and DFT calculations unveil that Ti-O active site is responsible for triggering the aniline to form a new PhNOH intermediate,two PhNOH condense to azoxybenzene over TiO_(2)catalyst.As for Cu_(1)-TiO_(2),the charge-specific distribution between the isolated Cu and TiO_(2)generates unique Cu_(1)-O-Ti hybridization structure with nine catalytic active sites,eight of them make PhNOH take place spontaneous dissociation to produce nitrosobenzene.This work not only unveils a new mechanistic pathway featuring the PhNOH intermediate in aniline oxidation for the first time but also presents a novel approach for constructing single-atom doped metal oxides and exploring their intricate active sites. 展开更多
关键词 Single atom doped metal oxide Aniline oxidation Selectivity New mechanism Active site
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Machine learning molecular dynamics simulations of liquid methanol
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作者 Jie Qian Junfan Xia Bin Jiang 《中国科学技术大学学报》 CAS CSCD 北大核心 2024年第6期12-21,I0009,I0010,共12页
As the simplest hydrogen-bonded alcohol,liquid methanol has attracted intensive experimental and theoretical interest.However,theoretical investigations on this system have primarily relied on empirical intermolecular... As the simplest hydrogen-bonded alcohol,liquid methanol has attracted intensive experimental and theoretical interest.However,theoretical investigations on this system have primarily relied on empirical intermolecular force fields or ab initio molecular dynamics with semilocal density functionals.Inspired by recent studies on bulk water using increasingly accurate machine learning force fields,we report a new machine learning force field for liquid methanol with a hybrid functional revPBE0 plus dispersion correction.Molecular dynamics simulations on this machine learning force field are orders of magnitude faster than ab initio molecular dynamics simulations,yielding the radial distribution functions,selfdiffusion coefficients,and hydrogen bond network properties with very small statistical errors.The resulting structural and dynamical properties are compared well with the experimental data,demonstrating the superior accuracy of this machine learning force field.This work represents a successful step toward a first-principles description of this benchmark system and showcases the general applicability of the machine learning force field in studying liquid systems. 展开更多
关键词 liquid methanol molecular dynamics machine learning hydrogen bond force field
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Formation of mesophase microbeads from bulk mesophase pitch induced by fullerene
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作者 CHEN Wen-sheng LIU Lan-tao +5 位作者 WANG Zheng DUAN Chun-feng ZHANG Xing-wei MA Zhao-kun CHEN Xiao-hong SONG Huai-he 《新型炭材料(中英文)》 SCIE EI CAS CSCD 北大核心 2024年第4期645-654,共10页
A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liqu... A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liquid-phase carbonization of isotropic pitch to the emergence of carbon microbeads in the matrix and finally their growth to form a 100%anisotropic bulk meso-phase,but rather a reverse transformation.The effects of C_(60) loading and reaction temperature on the morphological transformation of mesophase were investigated by polarizing optical and scanning electron microscopies.The physical changes in the NMP induced by C_(60) were characterized by thermogravimetric analysis,Fourier transform infrared spectroscopy,X-ray diffractometry and Raman spectroscopy.The results show that the coalesced NMP can be converted to a spherical type at 300-320℃ with the addition of 5%C_(60),and the size of the mesophase microbeads increases with increasing temperature.Furthermore,a model is established to ex-plain the unique induction effect of C_(60) in the transformation process.This work makes the morphological transformation of MP con-trollable,and provides a new idea for the understanding and research of mesophase pitch. 展开更多
关键词 Reversible transformation Fullerene induction mechanism Mesophase texture π-electron-induced effect Mesophase microbeads
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Numerical Analysis of Explosion Characteristics of Vent Gas From 18650 LiFePO_(4) Batteries With Different States of Charge
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作者 Shi-Lin Wang Xu Gong +5 位作者 Li-Na Liu Yi-Tong Li Chen-Yu Zhang Le-Jun Xu Xu-Ning Feng Huai-Bin Wang 《电化学(中英文)》 CAS 北大核心 2024年第8期28-35,共8页
The combustion and explosion characteristics of lithium-ion battery vent gas is a key factor in determining the fire hazard of lithium-ion batteries.Investigating the combustion and explosion hazards of lithium-ion ba... The combustion and explosion characteristics of lithium-ion battery vent gas is a key factor in determining the fire hazard of lithium-ion batteries.Investigating the combustion and explosion hazards of lithium-ion batteries vent gas can provide guidance for rescue and protection in explosion accidents in energy storage stations and new energy vehicles,thereby promoting the application and development of lithium-ion batteries.Based on this understanding and combined with previous research on gas production from lithium-ion batteries,this article conducted a study on the combustion and explosion risks of vent gas from thermal runaway of 18650 LFP batteries with different states of charge(SOCs).The explosion limit of mixed gases affected by carbon dioxide inert gas is calculated through the“elimination”method,and the Chemkin-Pro software is used to numerically simulate the laminar flame speed and adiabatic flame temperature of the battery vent gas.And the concentration of free radicals and sensitivity coefficients of major elementary reactions in the system are analyzed to comprehensively evaluate the combustion explosion hazard of battery vent gas.The study found that the 100%SOC battery has the lowest explosion limit of the vent gas.The inhibitory elementary reaction sensitivity coefficient in the reaction system is lower and the concentration of free radicals is higher.Therefore,it has the maximum laminar flame speed and adiabatic flame temperature.The combustion and explosion hazard of battery vent gas increases with the increase of SOC,and the risk of explosion is the greatest and most harmful when SOC reaches 100%.However,the related hazards decrease to varying degrees with overcharging of the battery.This article provides a feasible method for analyzing the combustion mechanism of vent gas from lithium-ion batteries,revealing the impact of SOC on the hazardousness of battery vent gas.It provides references for the safety of storage and transportation of lithium-ion batteries,safety protection of energy storage stations,and the selection of related fire extinguishing agents. 展开更多
关键词 Combustion and explosion characteristics Explosion limit Laminar flame speed Adiabatic flame temperature Sensitivity analysis
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Large and nonlinear electric field response in a two-dimensional ferroelectric Rashba material
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作者 Li Sheng Xiaomin Fu +2 位作者 Chao Jia Xingxing Li Qunxiang Li 《中国科学技术大学学报》 CAS CSCD 北大核心 2024年第6期8-11,21,I0009,共6页
The achievement of electrical spin control is highly desirable.One promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its... The achievement of electrical spin control is highly desirable.One promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its Rashba constant to external electric fields holds great potential for short channel lengths in spin field-effect transistors,which is crucial for preserving spin coherence and enhancing integration density.Hence,two-dimensional(2D)Rashba semiconductors with large Rashba constants and significant electric field responses are highly desirable.Herein,by employing first-principles calculations,we design a thermodynamically stable 2D Rashba semiconductor,YSbTe_(3),which possesses an indirect band gap of 1.04 eV,a large Rashba constant of 1.54 eV·Åand a strong electric field response of up to 4.80 e·Å^(2).In particular,the Rashba constant dependence on the electric field shows an unusual nonlinear relationship.At the same time,YSbTe_(3)has been identified as a 2D ferroelectric material with a moderate polarization switching energy barrier(~0.33 eV per formula).By changing the electric polarization direction,the Rashba spin texture of YSbTe_(3)can be reversed.These out-standing properties make the ferroelectric Rashba semiconductor YSbTe_(3)quite promising for spintronic applications. 展开更多
关键词 computational chemistry Rashba effect FERROELECTRICS SPINTRONICS
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Controlling Reactivity of Palladium Amides for Selective Carbonylation towards Urea and Oxamide Derivatives
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作者 WANG Jin-hui CAO Yan-wei HE Lin 《分子催化(中英文)》 CAS CSCD 北大核心 2024年第4期297-308,共12页
Carbonylation reactions,crucial for carbonyl group incorporation,struggle with the inherent complexity of achieving selective mono-or double-carbonylation on single substrates,often due to competing reaction pathways.... Carbonylation reactions,crucial for carbonyl group incorporation,struggle with the inherent complexity of achieving selective mono-or double-carbonylation on single substrates,often due to competing reaction pathways.Herein,our study introduces a strategy employing palladium amides,harnessing their unique reactivity control,to direct the selective carbonylation of amines for the targeted synthesis of urea and oxamide derivatives.The palladium amide structure was elucidated using single-crystal X-ray diffraction.Controlled experiments and cyclic voltammetry studies further elucidate that the oxidation of palladium amide or its insertion into a carbonyl group diverges into distinct pathways.By employing sodium percarbonate as an eco-friendly oxidant and base,we have successfully constructed a switchable carbonylation system co-catalyzed by palladium and iodide under room temperature.The utilizing strategy in this study not only facilitates effective control over reaction selectivity but also mitigates the risk of explosions,a critical safety concern in traditional carbonylation methods. 展开更多
关键词 selectivity control palladium catalysis oxidative carbonylation AMINOCARBONYLATION green reagents
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