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Synergistic rare-earth yttrium single atoms and copper phosphide nanoparticles for high-selectivity ammonia electrosynthesis

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Rare Metals 2024年第11期 5792-5801页

作者： yi-meng cai Yang-Hua Li yi Xiao Quentin Meyer Qian Sun Wan-Jing Lai Shu-Wen Zhao Jun Li Lin-Jie Zhang Han Wang Zhang Lin Jun Luo Li-Li Han School of Materials Science and Engineering Institute for New Energy Materials and Low-Carbon TechnologiesTianjin University of Technology State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences School of Chemistry The University of New South Wales School of Metallurgy and Environment Central South University Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of China

Electrochemical nitrate reduction to NH3holds a great promise for N-upcycling in nature,while its sluggish reaction kinetics involved in both the stepwise deoxygenation and hydrogenation processes necessitates the development of bespoke catalysts with multi-site ***,we report a hybrid catalyst composed of rare-earth（RE） yttrium（Y） single atoms and copper phosphide（Cu3P） nanoparticles loaded on N,P-doped carbon(YSA-Cu3P/CNP) through a chelating and pyrolysis *** to a synergistic contribution of Y single atoms and Cu3P nanoparticles,YSA-Cu3P/CNP achieves an impressive NH3Faradaic efficiency（FE） of 92% at-0.5V（***） and the highest NH3yield rate of11.4 mg·h-1·cm-2at-0.6 V（***） in an alkaline media,which surpass most of the reported *** intricate reaction pathway has been explored by online differential electrochemical mass spectrometry（DEMS）,and the synergistic effect between Y single atoms and Cu3P nanoparticles has been studied by in situ synchrotron X-ray absorption ***,density-functional theory（DFT） calculations unveil that the high-efficiency nitrate reduction on YSA-Cu3P/CNP is attributed to a reduced energy barrier of the rate-determining deoxygenation step coupled with the enhanced stabilization of active hydrogen favorable for the hydrogenation steps,thereby boosting the overall reaction *** addition,a prototype Zn-nitrate battery utilizing YSA-Cu3P/CNP as the cathode is *** work not only elucidates the mechanism behind the enhanced catalytic performance but also paves the way for the future development of highefficiency electrocatalysts through dual-site engineering.

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Shor's algorithm does not factor large integers in the presence of noise

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Science China(Information Sciences) 2024年第7期67卷 305-320页

作者： Jin-yi cai College of Letters and Science University of Wisconsin

We consider Shor's quantum factoring algorithm in the setting of noisy quantum gates. Under a generic model of random noise for(controlled) rotation gates, we prove that the algorithm does not factor integers of the form pq when the noise exceeds a vanishingly small level in terms of n—the number of bits of the integer to be factored, where p and q are from a well-defined set of primes of positive density. We further prove that with probability 1-o(1) over random prime pairs(p, q), Shor's factoring algorithm does not factor numbers of the form pq, with the same level of random noise present.

关键词： random noise Shor’s algorithm rotation gates quantum computing prime factorization

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WEAK APPROXIMATIONS OF STOCHASTIC PARTIAL DIFFERENTIAL EQUATIONS WITH FRACTIONAL NOISE

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Journal of Computational Mathematics 2024年第3期42卷 735-754页

作者： meng cai Siqing Gan Xiaojie Wang School of Mathematics and Statistics HNP-LAMACentral South UniversityChangshaChina

This paper aims to analyze the weak approximation error of a fully discrete scheme for a class of semi-linear parabolic stochastic partial differential equations(SPDEs)driven by additive fractional Brownian motions with the Hurst parameter H∈(1/2,1).The spatial approximation is performed by a spectral Galerkin method and the temporal discretization by an exponential Euler *** far as we know,the weak error analysis for approximations of fractional noise driven SPDEs is absent in the literature.A key difficulty in the analysis is caused by the lack of the associated Kolmogorov *** the present work,a novel and efficient approach is presented to carry out the weak error analysis for the approximations,which does not rely on the associated Kolmogorov equations but relies on the Malliavin *** the best of our knowledge,the rates of weak convergence,shown to be higher than the strong convergence rates,are revealed in the fractional noise driven SPDE setting for the first *** examples corroborate the claimed weak orders of convergence.

关键词： Parabolic SPDEs Fractional Brownian motion Weak convergence rates Spec-tral Galerkin method Exponential Euler method Malliavin calculus

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Effect of Fluoride on the Ion-association of Calcium Phosphate and Crystallization of Hydroxyapatite

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Journal of Wuhan University of Technology(Materials Science) 2024年第4期39卷 831-838页

作者：宋昊月 cai meng 袁萍邹朝勇 School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Using a titration setup to accurately control the reaction conditions and in situ monitor the reaction,we showed that fluoride exhibited negligible effects on the ion association process of calcium and phosphate and the formation of ACP nanospheres in a buffer solution with constant ionic ***,the stability of ACP increased with increasing fluoride concentration,which was ascribed to the inhibitory effect of fluoride on the aggregation of ACP nanospheres and the nucleation of nanocrystals on the surface of ACP ***,fluoride could inhibit the lateral growth of HAP nanosheets and promote the formation of rod-like *** results further improve our understanding of the crystallization pathway of HAP crystals and the regulatory effects of fluoride.

关键词： crystallization amorphous calcium phosphate hydroxyapatite fluoride

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A dual adaptive unscented Kalman filter algorithm for SINS-based integrated navigation system

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Journal of Systems Engineering and Electronics 2024年第3期35卷 732-740页

作者： LYU Xu meng Ziyang LI Chunyu cai Zhenyu HUANG yi LI Xiaoyong YU Xingkai Department of Precision Instrument Tsinghua UniversityBeijing 100084China College of Mechanical and Power Engineering Three Gorges UniversityYichang 443002China Unit 91001 of the PLA Beijing 100161China School of Control and Computer Engineering North China Electric Power UniversityBeijing 100096China

In this study, the problem of measuring noise pollution distribution by the intertial-based integrated navigation system is effectively suppressed. Based on nonlinear inertial navigation error modeling, a nested dual Kalman filter framework structure is developed. It consists of unscented Kalman filter (UKF)master filter and Kalman filter slave filter. This method uses nonlinear UKF for integrated navigation state estimation. At the same time, the exact noise measurement covariance is estimated by the Kalman filter dependency filter. The algorithm based on dual adaptive UKF (Dual-AUKF) has high accuracy and robustness, especially in the case of measurement information interference. Finally, vehicle-mounted and ship-mounted integrated navigation tests are conducted. Compared with traditional UKF and the Sage-Husa adaptive UKF (SH-AUKF), this method has comparable filtering accuracy and better filtering stability. The effectiveness of the proposed algorithm is verified.

关键词： Kalman filter dual-adaptive integrated navigation unscented Kalman filter(UKF) robust

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Tailoring sulfur-doped and nitrogen-defective carbon nitride nanosheets for efficient photo-controlled radical polymerizations

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Science China Chemistry 2024年第7期67卷 2325-2334页

作者： Xue Li meng Kai Xu Yuan Huang Tao cai Key Laboratory of Biomedical Polymers of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China Wuhan University Shenzhen Research Institute Shenzhen 518057China

Despite the challenges that remain,the synergistic adjustment of various microstructures and photochemical parameters of graphitic carbon nitride(g-C_(3)N_(4))in photocatalytic reactions holds promises for improving catalytic efficiency and reducing energy ***,sulfur-doped and nitrogen-defective g-C_(3)N_(4)(n-SC_(3)N_(x))nanosheets were designed and elaborately *** resultant n-SC_(3)N_(x)possessed a precisely defined 2D layer structure with extensive porosity and incremental specific surface *** photoinduced electron transfer-reversible addition-fragmentation chain transfer(PET-RAFT)polymerization of vinyl monomers with low dispersity,excellent temporal control and high chain-end fidelity was achieved under mild blue light irradiation in a nondegassed *** to their ultrathin nanostructures with nitrogen defects and sulfur dopants,n-SC_(3)N_(x)was capable of catalyzing RAFT polymerization in aqueous solutions at significantly accelerated rates,which were nearly 8 times faster compared to bulk g-C_(3)N_(4).The ease of separation and efficient reusability in subsequent polymerizations was enabled by the heterogeneous nature of n-SC_(3)N_(x).The appeal of this approach was illustrated by the fact that utilizing a reusable and metal-free photocatalyst in aqueous environments allowed for the synthesis of polymers with molecular weight up to 300 kg mol^(-1) and a dispersity of 1.32.

关键词： graphitic carbon nitride nitrogen defects sulfur dopants PET-RAFT polymerization recyclability

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Interplay between Microscopic Structures and Macroscopic Viscoelastic Properties of Polyampholyte Gels

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Chinese Journal of Polymer Science 2024年第9期42卷 1360-1367,I0008页

作者： You-cai Xue yi-Ming Yang Di Jia Beijing National Laboratory for Molecular Sciences Laboratory of Polymer Physics and ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China

Polyampholyte gels,which have hierarchical structures,exhibit excellent self-healing properties and have great promise for biomaterials and *** investigated the relationship between microscopic structures and macroscopic viscoelastic properties of polyampholyte gels and found three factors influencing their viscoelastic properties,including the chemical crosslinking bonds,topological entanglements controlled by monomer concentration,and the ionic *** strength plays a major role on the strength of ionic bonds.A crossover point of elastic modulus and loss modulus was observed in the dynamic frequency sweeps at low monomer concentration or low chemical crosslinking density for gels with intermediate strength of ionic *** solid-liquid transition signaled by the crossover point is a typical feature of dynamic associated gels,representing the dynamical association-dissociation of the ionic bonds and full relaxation of the topological entanglements in the gel *** the crossover point disappears when the ionic bonds are too weak or too strong to form“permanent”***,in the non-linear yielding measurement,gels with intermediate strength of the ionic bonds are ductile and yield at very large shear strain due to the self-healing properties and the dynamic association-dissociation of the ionic *** the self-healing properties disappear when the ionic bond strength is too weak or too *** work reveals the mechanism of how the dynamic association-dissociation of ionic bonds influences both the linear and non-linear viscoelastic properties of the polyampholyte gels.

关键词： Polyampholyte gel Ionic bond Topological entanglement Self-healing Hierarchical structure

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N-Heterocyclic carbene-catalyzed enantioselective(dynamic) kinetic resolutions and desymmetrizations

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Science China Chemistry 2024年第2期67卷 482-511页

作者： yi Zhang Hui cai Xiuhai Gan Zhichao Jin National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityHuaxi DistrictGuiyang550025China

N-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically *** content is organized according to the activation modes involved i... 详细信息

关键词： N-heterocyclic carbene kinetic resolution dynamic kinetic resolution desymmetrization organocatalysis

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Zn-air batteries for electric vehicles

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Tungsten 2024年第1期6卷 164-173页

作者： Nai-Qi meng Yu-Xin Fan Jing-Sheng cai State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804China

The increasingly serious environmental challenges have gradually aroused people's interest in electric *** the last decade,governments and automakers have collaborated on the manufacturing of electric vehicles with high ***-edge battery technologies are pivotal for the performance of electric ***-air batteries are considered as potential power batteries for electric vehicles due to their high ***-air battery researches can be classified into three categories:primary batteries,mechanically rechargeable batteries,and chemically rechargeable *** majority of current studies aim at developing and improving chemically rechargeable and mechanically rechargeable Zn-air *** have tried to use catalytic materials design and device design for Zn-air batteries to make it possible for their applications in electric *** review will highlight the state-of-the-art in primary batteries,mechanically rechargeable batteries,and chemically rechargeable batteries,revealing the prospects of Zn-air batteries for electric vehicles.

关键词： Energy storage Electric vehicles Bifunctional oxygen catalysts Mechanically rechargeable Zn-air batteries Chemically rechargeable Zn-air batteries

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Threshold friction velocity influenced by soil particle size within the Columbia Plateau, northwestern United States

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Journal of Arid Land 2024年第8期16卷 1147-1162页

作者： meng Ruibing meng Zhongju Brenton SHARRATT ZHANG Jianguo cai Jiale CHEN Xiaoyan College of Desert Control Science and Engineering Inner Mongolia Agricultural UniversityHohhot 010018China Key Laboratory of Aeolian Physics and Desertification Control Engineering from Inner Mongolia Autonomous Region Inner Mongolia Agricultural UniversityHohhot 010018China Key Laboratory of Desert Ecosystem Conservation and Restoration State Forestry and Grassland Administration of ChinaInner Mongolia Agricultural UniversityHohhot 010018China USDA-Agricultural Research Service Washington State UniversityWashington 99164USA College of Resources and Environment Northwest A&F UniversityYangling 712100China Inner Mongolia Autonomous Region Academy of Social Sciences Hohhot 010010China

Wind erosion is a geomorphic process in arid and semi-arid areas and has substantial implications for regional climate and *** the Columbia Plateau of northwestern United States,the emissions from fine particles of loessial soils often contribute to the exceedance of inhalable particulate matter(PM)with an aerodynamic diameter of 10μm or less(PM10)according to the air quality ***,little is known about the threshold friction velocity(TFV)for particles of different sizes that comprise these *** this study,soil samples of two representative soil types(Warden sandy loam and Ritzville silt loam)collected from the Columbia Plateau were sieved to seven particle size fractions,and an experiment was then conducted to determine the relationship between TFV and particle size *** results revealed that soil particle size significantly affected the initiation of soil movement and TFV;TFV ranged 0.304-0.844 and 0.249-0.739 m/s for different particle size fractions of Ritzville silt loam and Warden sandy loam,***10 and total suspended particulates(TSP)emissions from a bed of 63-90μm soil particles were markedly higher for Warden sandy loam than for Ritzville silt *** with the lower TFV of Warden sandy loam,dust emissions from fine particles(<100μm in diameter)of Warden sandy loam thus may be a main contributor to dust in the region's atmosphere,since the PM10 emissions from the soil erosion surfaces and its ensuing suspension within the atmosphere constitute an essential process of soil erosion in the Columbia *** and implementing strategic land management practices on sandy loam soils is therefore necessary to control dust emissions in the Columbia Plateau.

关键词： particle size threshold friction velocity inhalable particulate matter total suspended particles Warden sandy loam Ritzville silt loam Columbia Plateau

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