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大面积照明供电布线单相化探讨
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作者 莫湘炯 《灯与照明》 1996年第2期35-36,共2页
大面积照明供电布线单相化探讨莫湘炯(江苏省产品质量监督检验中心所)现今开发住宅小区,多采用密集型高层楼群形式,供电密度增高,而且都是单相,各家用电器间耗电差额范围也较以前为大,几瓦乃至数千瓦不等,因之各家各户用电量参... 大面积照明供电布线单相化探讨莫湘炯(江苏省产品质量监督检验中心所)现今开发住宅小区,多采用密集型高层楼群形式,供电密度增高,而且都是单相,各家用电器间耗电差额范围也较以前为大,几瓦乃至数千瓦不等,因之各家各户用电量参差不一,若仍以传统供电方式,把三相... 展开更多
关键词 建筑 照明供电布线 单相化
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非晶合金Fe_(78)Si_9B_(13)在脉冲电流作用下的单相晶化 被引量:14
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作者 晁月盛 滕功清 +2 位作者 耿岩 刘晓武 赖祖涵 《物理学报》 SCIE EI CAS CSCD 北大核心 1997年第7期1369-1374,共6页
对非晶合金Fe78Si9B13进行了超短脉冲电流处理,实现了晶化时αFe(Si)单相结构析出.可以认为,脉冲电流作用时,电子运动与非晶中空位型结构缺陷间的周期性排斥效应促进了类金属原子从非晶结构单元中析出,使Fe(... 对非晶合金Fe78Si9B13进行了超短脉冲电流处理,实现了晶化时αFe(Si)单相结构析出.可以认为,脉冲电流作用时,电子运动与非晶中空位型结构缺陷间的周期性排斥效应促进了类金属原子从非晶结构单元中析出,使Fe(Si)原子局部富集,导致基体金属相在较低温度下优先成核.而在空位的定向迁移的同时,将伴随B原子的扩散,则B原子局域富集。 展开更多
关键词 非晶态合金 退火 单相 脉冲电流
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Monotonicity of the tail dependence for multivariate t-copula
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作者 石爱菊 林金官 《Journal of Southeast University(English Edition)》 EI CAS 2011年第4期466-470,共5页
This paper considers the upper orthant and extremal tail dependence indices for multivariate t-copula. Where, the multivariate t-copula is defined under a correlation structure. The explicit representations of the tai... This paper considers the upper orthant and extremal tail dependence indices for multivariate t-copula. Where, the multivariate t-copula is defined under a correlation structure. The explicit representations of the tail dependence parameters are deduced since the copula of continuous variables is invariant under strictly increasing transformation about the random variables, which are more simple than those obtained in previous research. Then, the local monotonicity of these indices about the correlation coefficient is discussed, and it is concluded that the upper extremal dependence index increases with the correlation coefficient, but the monotonicity of the upper orthant tail dependence index is complex. Some simulations are performed by the Monte Carlo method to verify the obtained results, which are found to be satisfactory. Meanwhile, it is concluded that the obtained conclusions can be extended to any distribution family in which the generating random variable has a regularly varying distribution. 展开更多
关键词 multivariate t-copula COPULA inverse gamma distribution MONOTONICITY regularly varying function correlation coefficient
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W火焰炉炉内流动特性的试验研究 被引量:2
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作者 姜健 《节能技术》 CAS 2013年第3期223-226,231,共5页
为摸清从国外引进的一台330 MW W火焰锅炉炉内流动特性,依据相似模化的准则,对该锅炉建立了1∶10冷态单相试验台,在试验台上进行了变锅炉配风(即三次风占总二次风的比例R=0%、6%、14%、20%和27%共5个工况)的冷态模化试验,得出了炉内流... 为摸清从国外引进的一台330 MW W火焰锅炉炉内流动特性,依据相似模化的准则,对该锅炉建立了1∶10冷态单相试验台,在试验台上进行了变锅炉配风(即三次风占总二次风的比例R=0%、6%、14%、20%和27%共5个工况)的冷态模化试验,得出了炉内流场特征和拱部下行气流衰减规律。当R=0~6%时炉内流场基本对称,R值加大至14%后炉内流场出现偏斜现象,继续加大R值,则流场偏斜加剧,前、后墙侧下行气流的衰减特性差异变大。 展开更多
关键词 W火焰炉 冷态单相试验 流场 风量分配
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Synthesis and properties of single-crystal Ni-rich cathode materials in Li-ion batteries 被引量:11
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作者 Shi-jie LU Yang LIU +4 位作者 Zhen-jiang HE Yun-jiao LI Jun-chao ZHENG Jing MAO Ke-hua DAI 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2021年第4期1074-1086,共13页
Single-crystal Ni-rich cathode material LiNi0.88Co0.09Al0.03O2(SC) was synthesized by a high-temperature solid-state calcination method. Physicochemical properties of primary and delithiated SC samples were investigat... Single-crystal Ni-rich cathode material LiNi0.88Co0.09Al0.03O2(SC) was synthesized by a high-temperature solid-state calcination method. Physicochemical properties of primary and delithiated SC samples were investigated by X-ray diffractometry, X-ray photoelectron spectroscopy, and transmission electron microscopy. Electrochemical performance was characterized by long-term cycling, cyclic voltammetry, and in-situ impedance spectroscopy. The results indicated that high temperature rendered layered oxides to lose lithium/oxygen in the interior and exterior, and induced cationic disordering. Besides, the solid-phase synthesis process promoted phase transformation for electrode materials, causing the coexisting multi-phase in a single particle. High temperature can foster the growth of single particles, but it caused unstable structure of layered phase. 展开更多
关键词 lithium-ion battery cathode material SINGLE-CRYSTAL electrochemical performance phase transformation
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Zinc single atoms on N-doped carbon: An efficient and stable catalyst for CO2 fixation and conversion 被引量:2
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作者 Xinjiang Cui Xingchao Dai +5 位作者 Annette-Enrica Surkus Kathrin Junge Carsten Kreyenschulte Giovanni Agostini Nils Rockstroh Matthias Beller 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第11期1679-1685,共7页
The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly a... The cycloaddition of epoxides and carbon dioxide represents a straightforward and atom-efficient method for synthesis of cyclic carbonates and utilization of CO2. So far, homogeneous metal complexes have been mainly applied for such transformations. Here, we describe the synthesis of novel heterogeneous Zn-based catalysts, which were conveniently prepared by pyrolysis of an active- carbon-supported phenanthroline-ligated Zn(OAc)2 complex. Detail structural characterizations proved the existence of single zinc sites in the active material. Compared to a Zn-based nanoparticle (Zn-NP) catalyst, the resulting single metal atom catalyst (SAC) displayed improved activity and stability for the cycloaddition of epoxides. By applying the optimal catalyst, a variety of carbonates were successfully obtained in high yields with good functional group tolerance. 展开更多
关键词 Heterogeneous catalysis Single atom catalyst ZINC Carbon dioxide CYCLOADDITION CARBONATE
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Single-atom catalysis: Bridging the homo-and heterogeneous catalysis 被引量:20
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作者 Fang Chen Xunzhu Jiang +2 位作者 Leilei Zhang Rui Lang Botao Qiao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第5期893-898,共6页
Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneo... Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous catalysis.This prediction was first experimentally demonstrated in 2016.In this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H bonds.All of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous catalysts.These pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis. 展开更多
关键词 Single-atom catalysis Heterogenization of homogeneous catalysts Hydroformation HYDROSILYLATION Activation of C–H bonds
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An efficient strategy for photocatalytic hydrogen peroxide production over oxygen-enriched graphitic carbon nitride with sodium phosphate 被引量:2
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作者 Yu Zhang Ling Zhang +4 位作者 Di Zeng Wenjing Wang Juxue Wang Weimin Wang Wenzhong Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第10期2690-2698,共9页
Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxyge... Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its application.In this study,oxygen-rich g-C_(3)N_(4) with abundant nitrogen vacancies(OCN)was synthesized for photocatalytic H_(2)O_(2) production.X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy indicated that oxygen-containing functional groups(–COOH and C–O–C)were obtained.Electron paramagnetic resonance confirmed the successful introduction of nitrogen vacancies.OCN exhibited efficient photocatalytic H_(2)O_(2) production performance of 1965μmol L^(−1) h^(−1) in air under visible-light irradiation.The high H_(2)O_(2) production was attributed to the enhanced adsorption of oxygen,enlarged specific surface area,and promoted carrier separation.An increased H_(2)O_(2) production rate(5781μmol L^(−1) h^(−1))was achieved in a Na_(3)PO_(4) solution.The improved performance was attributed to the changed reactive oxygen species.Specifically,the adsorbed PO_(4)^(3−) on the surface of the OCN promoted the transfer of holes to the catalyst surface.•O_(2)−obtained by O_(2) reduction reacted with adjacent holes to generate 1O_(2),which could efficiently generate H_(2)O_(2) with isopropanol.Additionally,PO_(4)^(3−),as a stabilizer,inhibited the decomposition of H_(2)O_(2). 展开更多
关键词 PHOTOCATALYSIS Hydrogen peroxide production Graphitic carbon nitride Singlet oxygen Sodium phosphate
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Highly efficient Rh(Ⅰ)/tris-H_8-binaphthyl monophosphite catalysts for hydroformylation of dicyclopentadiene to dialdehydes 被引量:4
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作者 Mi Tian Haifeng Li Lailai Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第10期1646-1652,共7页
Novel catalytic systems for the Rh‐catalyzed hydroformylation of dicyclopentadiene have been developed using tris‐H8‐binaphthyl monophosphite as ligands containing different ester substituents at the 2’‐binaphthy... Novel catalytic systems for the Rh‐catalyzed hydroformylation of dicyclopentadiene have been developed using tris‐H8‐binaphthyl monophosphite as ligands containing different ester substituents at the 2’‐binaphthyl position(OCOMe,OCOPh,OCOAdamantyl and OCOPhCl).The catalysts exhibited high activity(S/C=4000,TON=3286)with good to excellent selectivity towards dialdehydes.Remarkably,the Rh(I)complex bearing the ligands with chlorophenyl ester substituents led to 99.9%conversion and 98.7%selectivity for dialdehydes under relatively mild conditions(6 MPa,120°C). 展开更多
关键词 HYDROFORMYLATION DICYCLOPENTADIENE Monophosphite DIALDEHYDE Homogeneous catalysis
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A ROBUST PHASE-ONLY DIRECT DATA DOMAIN ALGORITHM BASED ON GENERALIZED RAYLEIGH QUOTIENT OPTIMIZATION USING HYBRID GENETIC ALGORITHM 被引量:2
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作者 Shao Wei Qian Zuping Yuan Feng 《Journal of Electronics(China)》 2007年第4期560-566,共7页
A robust phase-only Direct Data Domain Least Squares (D3LS) algorithm based on gen- eralized Rayleigh quotient optimization using hybrid Genetic Algorithm (GA) is presented in this letter. The optimization efficiency ... A robust phase-only Direct Data Domain Least Squares (D3LS) algorithm based on gen- eralized Rayleigh quotient optimization using hybrid Genetic Algorithm (GA) is presented in this letter. The optimization efficiency and computational speed are improved via the hybrid GA com- posed of standard GA and Nelder-Mead simplex algorithms. First, the objective function, with a form of generalized Rayleigh quotient, is derived via the standard D3LS algorithm. It is then taken as a fitness function and the unknown phases of all adaptive weights are taken as decision variables. Then, the nonlinear optimization is performed via the hybrid GA to obtain the optimized solution of phase-only adaptive weights. As a phase-only adaptive algorithm, the proposed algorithm is sim- pler than conventional algorithms when it comes to hardware implementation. Moreover, it proc- esses only a single snapshot data as opposed to forming sample covariance matrix and operating matrix inversion. Simulation results show that the proposed algorithm has a good signal recovery and interferences nulling performance, which are superior to that of the phase-only D3LS algorithm based on standard GA. 展开更多
关键词 Generalized Rayleigh quotient Hybrid genetic algorithm Phase-only optimization Direct Data Domain Least Squares (D^3LS) algorithm Nelder-Mead simplex algorithm
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Optimization control strategy for single-phase permanent magnet generator based on voltage ripple
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作者 周寿明 Wu Hongxing +1 位作者 Zhao Gouping Li Liyi 《High Technology Letters》 EI CAS 2013年第4期429-436,共8页
A method of feedforward compensation for electromotive force(EMF) in the single-phase permanent magnet linear generation system and a research in the performance of the single-phase PMLG system are presented.A general... A method of feedforward compensation for electromotive force(EMF) in the single-phase permanent magnet linear generation system and a research in the performance of the single-phase PMLG system are presented.A general mathematical model for the single-phase permanet magnet linear generator(PMLG) system is established and the current loop,voltage loop and the feedforward control are studied based on it for the control system.Then this paper analyses the transfer function of the power system,optimizes current loop and voltage loop parameters by engineering algorithm,and calculates the optimal control parameters.An EMF feedforward compensation method is developed to optimize the control system which improves dynamic performance of the power system but does not affect the steady-state performance.The result of this research verifies the correctness and rationality of the design for the control system. 展开更多
关键词 linear motor generation system single-phase motor feedforward control
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Monodisperse Ni-clusters anchored on carbon nitride for efficient photocatalytic hydrogen evolution 被引量:1
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作者 Liang Jian Huizhen Zhang +6 位作者 Bing Liu Chengsi Pan Yuming Dong Guangli Wang Jun Zhong Yongjie Zheng Yongfa Zhu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第2期536-545,共10页
The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride(CN)by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve... The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride(CN)by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve high-efficiency photocatalytic activity for hydrogen evolution.The Ni-cluster/CN exhibited a photocatalytic hydrogen production rate of 16.5 mmol·h^(-1)·g^(-1) and a total turnover frequency(TOF(H_(2)))value of 461.14 h^(-1).X-ray absorption spectroscopy based on synchrotron radiation indicated that CN had two reaction centers to form stable interface interactions with monodispersed Ni-clusters,in which carbon can act as an electron acceptor,while nitrogen can act as an electron donor.Meanwhile,the hybrid electronic structure of the Ni-cluster/CN system was constructed,which was favorable for photocatalytic activity for hydrogen production.An in-depth understanding of the interfacial interaction between CN and Ni-clusters will have important reference significance on the mechanistic study of development based on the cocatalyst. 展开更多
关键词 Monodisperse Ni-clusters Carbon nitride Interface interaction Photocatalytic hydrogen evolution
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Interfacial engineering of heterogeneous molecular electrocatalysts using ionic liquids towards efficient hydrogen peroxide production 被引量:1
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作者 Zixun Yu Chang Liu +5 位作者 Yeyu Deng Mohan Li Fangxin She Leo Lai Yuan Chen Li Wei 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第5期1238-1246,共9页
Efficient and selective oxygen reduction reaction(ORR)electrocatalysts are critical to realizing decentralized H_(2)O_(2)production and utilization.Here we demonstrate a facile interfacial engineering strategy using a... Efficient and selective oxygen reduction reaction(ORR)electrocatalysts are critical to realizing decentralized H_(2)O_(2)production and utilization.Here we demonstrate a facile interfacial engineering strategy using a hydrophobic ionic liquid(IL,i.e.,[BMIM][NTF2])to boost the performance of a nitrogen coordinated single atom cobalt catalyst(i.e.),cobalt phthalocyanine(CoPc)supported on carbon nanotubes(CNTs).We find a strong correlation between the ORR performance of CoPc/CNT and the thickness of its IL coatings.Detailed characterization revealed that a higher O_(2)solubility(2.12×10^(−3)mol/L)in the IL compared to aqueous electrolytes provides a local O2 enriched surface layer near active catalytic sites,enhancing the ORR thermodynamics.Further,the hydrophobic IL can efficiently repel the as‐synthesized H_(2)O_(2)molecules from the catalyst surface,preventing their fast decomposition to H_(2)O,resulting in improved H_(2)O_(2)selectivity.Compared to CoPc/CNT without IL coatings,the catalyst with an optimal~8 nm IL coating can deliver a nearly 4 times higher mass specific kinetic current density and 12.5%higher H2O2 selectivity up to 92%.In a two‐electrode electrolyzer test,the optimal catalyst exhibits an enhanced productivity of 3.71 molH2O2 gcat^(–1)h^(–1),and robust stability.This IL‐based interfacial engineering strategy may also be extended to many other electrochemical reactions by carefully tailoring the thickness and hydrophobicity of IL coatings. 展开更多
关键词 Hydrogen peroxide Ionic liquid Oxygen reduction reaction Single‐atom catalyst Heterogeneous molecular catalyst
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Mn-corrolazine-based 2D-nanocatalytic material with single Mn atoms for catalytic oxidation of alkane to alcohol 被引量:2
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作者 Chun Zhu Jin-Xia Liang +2 位作者 Yang Meng Jian Lin Zexing Cao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第6期1030-1039,共10页
Heterogenization of organic-macrocyclic metal catalysts is one of the simplest and most efficient methods for effective separation of products and cyclic application of a catalyst.By using an environmentally friendly ... Heterogenization of organic-macrocyclic metal catalysts is one of the simplest and most efficient methods for effective separation of products and cyclic application of a catalyst.By using an environmentally friendly Mn-corrolazine catalyst as the building unit,which can directly oxidize organic substrates under oxygen atmosphere and mild conditions,we theoretically constructed a novel two-dimensional(2D)Mn-corrolazine nanocatalytic material with high catalytic activity.In this material,each Mn atom maintains its electronic configuration in the monomer and can directly activate O2 as the single-atom catalyst(SAC)center to form a radical-like[Mn]-O-O under mild visible-light irradiation conditions.The newly generated[Mn]–O–O can efficiently and selectively oxidize C–H bonds to form alcohol species through H-abstraction and the rebound reaction.Moreover,the catalytic reaction is easily regulated by an external electric field along its intrinsic Mn–O–O reaction axis.The current study provides a theoretical foundation for further experimental studies and practical applications of the Mn-corrolazine-based SAC. 展开更多
关键词 Single-atom catalyst HETEROGENIZATION Two-dimensional nanomaterials First-principles calculations C–H bond activation
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Signatures for Coexistence of Monoclinic and Hexagonal Phases in GaTe Nanoflakes
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作者 Hong-yan Yan Cheng-bing Qin Lian-tuan Xiao 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2022年第6期893-899,I0072,I0073,共9页
The burgeoning two-dimensional(2D)layered materials provide a powerful strategy to realize efficient light-emitting devices.Among them,gallium telluride(Ga Te)nanoflakes,showing strong photoluminescence(PL)emission fr... The burgeoning two-dimensional(2D)layered materials provide a powerful strategy to realize efficient light-emitting devices.Among them,gallium telluride(Ga Te)nanoflakes,showing strong photoluminescence(PL)emission from multilayer to bulk crystal,relax the stringent fabrication requirements of nanodevices.However,detailed knowledge on the optical properties of Ga Te varies as layer thickness is still missing.Here we perform thickness-dependent PL and Raman spectra,as well as temperature-dependent PL spectra of Ga Te nanoflakes.Spectral analysis reveals a spectroscopic signature for the coexistence of both the monoclinic and hexagonal phases in Ga Te nanoflakes.To understand the experimental results,we propose a crystal structure where the hexagonal phase is on the top and bottom of nanoflakes while the monoclinic phase is in the middle of the nanoflakes.On the basis of temperature-dependent PL spectra,the optical gap of the hexagonal phase is determined to be 1.849 eV,which can only survive under temperature higher than 200 K with the increasing phonon population.Furthermore,the strength of exciton-phonon interaction of the hexagonal phase is estimated to be 1.24 me V/K.Our results prove the coexistence of dual crystalline phases in multilayer Ga Te nanoflakes,which may provoke further exploration of phase transformation in Ga Te materials,as well as new applications in 2D light-emitting diodes and heterostructure-based optoelectronics. 展开更多
关键词 GATE Hexagonal phase Monoclinic phase PHOTOLUMINESCENCE
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Reaction kinetics and phase behavior in the chemoselective hydrogenation of 3‐nitrostyrene over Co‐N‐C single‐atom catalyst in compressed CO_(2)
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作者 Dan Zhou Leilei Zhang +5 位作者 Wengang Liu Gang Xu Ji Yang Qike Jiang Aiqin Wang Jianzhong Yin 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第9期1617-1624,共8页
Single‐atom catalysts(SACs)have demonstrated excellent performances in chemoselective hydrogenation reactions.However,the employment of precious metals and/or organic solvents compromises their sustainability.Herein,... Single‐atom catalysts(SACs)have demonstrated excellent performances in chemoselective hydrogenation reactions.However,the employment of precious metals and/or organic solvents compromises their sustainability.Herein,we for the first time report the chemoselective hydrogenation of 3‐nitrostyrene over noble‐metal‐free Co‐N‐C SAC in green solvent—compressed CO2.An interesting inverted V‐curve relation is observed between the catalytic activity and CO2 pressure,where the conversion of 3‐nitrostyrene reaches the maximum of 100%at 5.0 MPa CO2(total pressure of 8.1 MPa).Meanwhile,the selectivities to 3‐vinylaniline at all pressures remain high(>99%).Phase behavior studies reveal that,in sharp contrast with the single phase which is formed at total pressure above 10.8 MPa,bi‐phase composed of CO2/H_(2)gas‐rich phase and CO2‐expanded substrate liquid phase forms at total pressure of 8.1 MPa,which dramatically changes the reaction kinetics of the catalytic system.The reaction order with respect to H_(2)pressure decreases from~0.5 to zero at total pressure of 8.1 MPa,suggesting the dissolved CO2 in 3‐nitrostyrene greatly promotes the dissolution of H_(2)in the substrate,which is responsible for the high catalytic activity at the peak of the inverted V‐curve. 展开更多
关键词 Single‐atom catalyst Co‐N‐C CO2 Phase behavior Chemoselective hydrogenation 3‐Nitrostyrene
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Quaternary phosphonium polymer-supported dual-ionically bound[Rh(CO)I_(3)]^(2-)catalyst for heterogeneous ethanol carbonylation
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作者 Zhou Ren Yang Liu +4 位作者 Yuan Lyu Xiangen Song Changyong Zheng Zheng Jiang Yunjie Ding 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第4期606-617,共12页
A single-Rh-site catalyst(Rh-TPISP)that was ionically-embedded on a P(V)quaternary phosphonium porous polymer was evaluated for heterogeneous ethanol carbonylation.The[Rh(CO)I_(3)]^(2-)unit was proposed to be the acti... A single-Rh-site catalyst(Rh-TPISP)that was ionically-embedded on a P(V)quaternary phosphonium porous polymer was evaluated for heterogeneous ethanol carbonylation.The[Rh(CO)I_(3)]^(2-)unit was proposed to be the active center of Rh-TPISP for the carbonylation reaction based on detailed Rh L3-edge X-ray absorption near edge structure(XANES),X-ray photoelectron spectroscopy(XPS),and Rh extended X-ray absorption fine structure(EXAFS)analyses.As the highlight of this study,Rh-TPISP displayed distinctly higher activity for heterogeneous ethanol carbonylation than the reported catalytic systems in which[Rh(CO)_(2)I_(2)]^(-)is the traditional active center.A TOF of 350 h^(-1)was obtained for the reaction over[Rh(CO)I_(3)]^(2-),with>95%propionyl selectivity at 3.5 MPa and 468 K.No deactivation was detected during a near 1000 h running test.The more electron-rich Rh center was thought to be crucial for explaining the superior activity and selectivity of Rh-TPISP,and the formation of two ionic bonds between[Rh(CO)I_(3)]^(2-)and the cationic P(V)framework([P]^(+))of the polymer was suggested to play a key role in firmly immobilizing the active species to prevent Rh leaching. 展开更多
关键词 Heterogeneous ethanol carbonylation Single-site catalyst Carbonylation active center [Rh(CO)I_(3)]^(2-) Ultrastable dual-ionically bound immobilization Porous ionic polymer
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Boosting photocatalytic hydrogen production by creating isotype heterojunctions and single-atom active sites in highly-crystallized carbon nitride 被引量:6
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作者 Shaohua Shen Jie Chen +9 位作者 Yiqing Wang Chung-Li Dong Fanqi Meng Qinghua Zhang Yiliang Huangfu Zhi Lin Yu-Cheng Huang Yanrui Li Mingtao Li Lin Gu 《Science Bulletin》 SCIE EI CSCD 2022年第5期520-528,M0004,共10页
Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen.A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to... Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen.A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to significantly boost the photocatalytic activity,but is yet to be realized.Herein,we find that cobalt salt added in the ionothermal synthesis can promote the phase transition of heptazine-based crystalline carbon nitride(CCN)to triazine-based poly(triazine imide)(PTI),rendering the creation of singleatom cobalt coordinated isotype CCN/PTI heterojunction.Co-CCN/PTI exhibits an appreciable apparent quantum yield of 20.88%at 425 nm for photocatalytic hydrogen production with a rate achieving3538μmol h^(-1)g^(-1)(λ>420 nm),which is 4.8 times that of CCN and 27.6 times that of PTI.The high photocatalytic activity is attributed to the Type II isotype highly-crystallized CCN/PTI heterojunction for promoting charge carrier migration,and the single-atom Co sites for accelerating surface oxidation reaction. 展开更多
关键词 Photocatalytic hydrogen production Single-atom cobalt Crystalline carbon nitride Poly(triazine imide) Isotype heterojunctions
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Scalable arrays of chemical vapor sensors based on DNA-decorated graphene 被引量:3
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作者 Nicholas J. Kybert Gang Hee Han +3 位作者 Mitchell B. Lerner Eric N. Dattoli Ali Esfandiar A. T. Charlie Johnson 《Nano Research》 SCIE EI CAS CSCD 2014年第1期95-103,共9页
Arrays of chemical vapor sensors based on graphene field effect transistors functionalized with single-stranded DNA have been demonstrated. Standard photolithographic processing was adapted for use on large-area graph... Arrays of chemical vapor sensors based on graphene field effect transistors functionalized with single-stranded DNA have been demonstrated. Standard photolithographic processing was adapted for use on large-area graphene by including a metal protection layer, which protected the graphene from contamination and enabled fabrication of high quality field-effect transistors (GFETs). Processed graphene devices had hole mobilities of 1,640 ± 250 cm2.V-1.s-1 and Dirac voltages of 15 ± 10 V under ambient conditions. Atomic force microscopy was used to verify that the graphene surface remained uncontaminated and therefore suitable for controlled chemical functionalization. Single-stranded DNA was chosen as the functionalization layer due to its affinity to a wide range of target molecules and π-π stacking interaction with graphene, which led to minimal degradation of device characteristics. The resulting sensor arrays showed analyte- and DNA sequence-dependent responses down to parts-per-billion concentrations. DNA/GFET sensors were able to differentiate among chemically similar analytes, including a series of carboxylic acids, and structural isomers of carboxylic acids and pinene. Evidence for the important role of electrostatic chemical gating was provided by the observation of understandable differences in the sensor response to two compounds that differed only by the replacement of a (deprotonating) hydroxyl group by a neutral methyl group. Finally, target analytes were detected without loss of sensitivity in a large background of a chemically similar, volatile compound. These results motivate further development of the DNA/graphene sensor family for use in an electronic olfaction system. 展开更多
关键词 GRAPHENE vapor sensor DNA PHOTOLITHOGRAPHY chemical gating
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Designing noble metal single-atom-loaded two-dimension photocatalyst for N2 and CO2 reduction via anion vacancy engineering 被引量:7
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作者 Peng Zhou Yuguang Chao +3 位作者 Fan Lv Jianping Lai Kai Wang Shaojun Guo 《Science Bulletin》 SCIE EI CAS CSCD 2020年第9期720-725,M0003,共7页
Building highly active and stable noble metal single atom(MSA)catalyst onto photocatalyst materials for nitrogen reduction reaction(NRR)and CO2 reduction reaction(CRR)is a key to future renewable energy conversion and... Building highly active and stable noble metal single atom(MSA)catalyst onto photocatalyst materials for nitrogen reduction reaction(NRR)and CO2 reduction reaction(CRR)is a key to future renewable energy conversion and storage technologies.Here we present a design strategy to optimize the stability and electronic property of noble metal single atoms(MSAs,M=Rh,Pd,Ag,Ir,Pt,Au)catalyst supported on g-C3N4 and 2H-MoS2 photocatalysts towards NRR and CRR.Our results indicate that the MSAs tend to be trapped at the anion-vacancy sites of photocatalyst rather than the pristine photocatalyst surface.This anion vacancy can promise the MSAs with an optimized electron-captured ability in the photoexcitation process,thus decreasing the energy barriers of NRR and CRR on MSAs.Especially,it is revealed that the N-vacancy-stabilized Ir SA on g-C3N4 and the S-vacancy-stabilized RhSA on 2H-MoS2 own the lowest energy barrier in NRR.However,for CRR,the HCOOH is the main product on MSAs supported by gC3N4 and 2H-MoS2.The N-vacancy-stabilized PdSA on g-C3N4 and the S-vacancy-stabilized AuSA on 2H-MoS2 show the lowest energy barrier for HCOOH production in CRR.This finding offers an approach to design specific active MSA centres on photocatalysts by the anion vacancy engineering. 展开更多
关键词 PHOTOCATALYST Noble metal Single atom CRR NRR
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