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Applications of in-situ solid-state nuclear magnetic resonance in methanol to olefins reaction

Science China Chemistry 2025年第1期68卷 134-151页

作者： Jing Niu Shutao Xu Yingxu Wei Zhongmin Liu National Engineering research Center of Lower-Carbon catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of Sciences State Key Laboratory of catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The methanol-to-olefins（MTO） reaction offers an alternative pathway for the production of low-carbon olefins from non-oil feedstocks. Fundamental research has been impeded by a lack of comprehensive understanding of its underlying mechanism,despite the significant progress made in industry. In-situ solid-state nuclear magnetic resonance（ss NMR） spectroscopy has emerged as a pivotal tool, offering crucial insights into key species under real-time operando conditions. Furthermore, the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of in-situ13C MAS NMR and 2D correlation spectroscopy. Moreover, recent technological advancements in hyperpolarization（HP） methods, including HP129Xe NMR and dynamic nuclear polarization（DNP）, have significantly improved the sensitivity of ss NMR, enabling detailed structural and kinetic analysis as well as the detection of trace species. In this feature article, we summarized recent advancements in（in-situ） ss NMR spectroscopy applied to MTO reaction processes,encompassing mechanistic investigations at various stages and the intricate host–guest interactions. These theoretical insights into the dynamic evolution of MTO reactions lay a solid foundation for the optimization of catalytic processes and the development of efficient catalysts, thereby advancing the techniques towards more sustainable and economical production route for olefins.

关键词： MTO zeolites in-situ ssNMR reactive intermediates reaction mechanism

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Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

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Journal of Energy Chemistry 2025年第1期100卷 760-769页

作者： Lin Peng Yu Bai Hang Li Meixiu Qu Zhenhua Wang Kening Sun Advanced research institute of Multidisciplinary Science Beijing Institute of Technology Beijing Key Laboratory of Chemical Power Source and Green catalysis School of Chemistry and Chemical Engineering Beijing Institute of Technology

Lithium-sulfur （Li-S） batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox ***,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P （Vp-B-Ni2P）,thereby enhancing the bidirectional sulfur *** study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides （LiPSs） as well as expediting the bidirectional conversion kinetics of sulfur ***,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation ***,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg *** work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.

关键词： Lithium sulfur batteries

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Constructing 2D bismuth-based heterostructure for highly efficient photocatalytic CO2 reduction

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Tungsten 2025年第1期7卷 71-79页

作者： Ruo-Hang Xu Hao-Yu Jiang Dan-Dan Cui Kun-Rong Du Hong-Run Zhang Sheng-Jie Xu Ya-Qi Li Zhi-Zhen Ren Liang Wang Wei-Chang Hao Yi Du School of Physics and BUAA-UOW Joint research Centre Beihang University Shenzhen institute of Beihang University Centre for catalysis and Clean Energy School of Environment and Science Griffith University

Reforming carbon dioxide（CO2） into fuels and valuable chemicals using solar energy holds significant potential for emission reduction and addressing energy supply *** recombination of photocarriers remains a major obstacle,however,to enhancing solar energy conversion efficiency in the photocatalytic reaction *** two-dimensional materials,constructing heterogeneous structures has emerged as an effective strategy to enhance the separation of photoexcited carriers by leveraging the internal electric field at the heterogeneous ***,we present a facile strategy for preparing Bi4NbO8Br/Bi2WO6plate-on-plate Z-scheme junctions with a strong internal electric field by in situ *** unique heterostructure facilitates efficient separation and transport of photoexcited charges by harnessing the internal electric field induced by chemical bonding at the lateral ***,the Bi4NbO8Br/Bi2WO6heterostructure exhibits enhanced CO2photoreduction properties,along with a CO yield rate of approximately 35 μmol·g-1·h-1under full light *** work offers novel insights into the synthesis of unique hetero structures intended to enhance the efficiency of photocatalytic CO2reduction.

关键词： Bi4NbO8Br/Bi2WO6 CO2 reduction Heterostructures Photocatalysts

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Fabrication of carbon-supported Al2O3 nanoparticles via spontaneous cross-linking to enhance selective hydrogenation of furfural

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Journal of Energy Chemistry 2025年第1期100卷 612-620页

作者： Weiwei Yu Xinbao Zhang Hongyu Chen Yanan Wang Shaoguo Li Fucun Chen Zhenni Liu Xiujie Li Xiangxue Zhu State Key Laboratory of catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=***,a novel Al2O3/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al2O3nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and *** obtained carbon-supported Al2O3hybrid catalyst has a high ratio （31%） of Al species in pentahedral-coordinated *** introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active *** the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al2O3/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-***,Al2O3/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on *** work provides an innovative and facile strategy for fabrication of carbon-supported Al2O3hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.

关键词： Selective hydrogenation Furfural Furfuryl alcohol Cross-linking Carbon supported Al 2 O 3 MPV route

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences institute of catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare Earth Resource research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

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Structural designs and mechanism insights into electrocatalytic oxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第1期100卷 792-814页

作者： Jing Lei Huijie Zhang Jian Yang Jia Ran Jiqiang Ning Haiyan Wang Yong Hu Key Laboratory of the Ministry of Education for Advanced catalysis Materials Department of Chemistry Zhejiang Normal University Jinhua Advanced research institute Department of Optical Science and Engineering Fudan University College of Chemistry and Materials Engineering Zhejiang A&F University

Biomass conversion offers an efficient approach to alleviate the energy and environmental *** oxidation of 5-hydroxymethylfurfural(HMF) has attracted tremendous attention in the latest few years for the mild synthesis conditions and high conversion efficiency to obtain 2,5-furan dicarboxylic acid(FDCA), but there still remain problems such as limited yield, short cycle life,and ambiguous reaction mechanism. Despite many reviews highlighting a variety of electrocatalysts for electrochemical oxidation of HMF, a detailed discussion of the structural modulation of catalyst and the underlying catalytic mechanism is still lacking. We herein provide a comprehensive summary of the recent development of electrochemical oxidation of HMF to FDCA, particularly focusing on the mechanism studies as well as the advanced strategies developed to regulate the structure and optimize the performance of the electrocatalysts, including heterointerface construction, defect engineering,single-atom engineering, and in situ reconstruction. Experimental characterization techniques and theoretical calculation methods for mechanism and active site studies are elaborated, and challenges and future directions of electrochemical oxidation of HMF are also prospected. This review will provide guidance for designing advanced catalysts and deepening the understanding of the reaction mechanism beneath electrochemical oxidation of HMF to FDCA.

关键词： Structural design

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Ni-catalyzed cross-electrophile alkyl-alkyl coupling reactions

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Science China Chemistry 2025年

作者： Li-Xu You Lan Tian Chun-Ling Guo Shun-Xi Li Yu-Cheng Liu Yu-Long Li Wei Shu College of Chemistry and Environmental Engineering Key Laboratory of Green Catalysis of Higher Education Institutes of Sichuan Sichuan University of Science and Engineering Guangming Advanced research institute Shenzhen Grubbs Institute Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and Technology

Introducing saturated carbon-carbon bonds into organic molecules significantly increases the three-dimensional configuration,thus altering the physical and chemical properties as well as the functions of molecules. Transition-metal-catalyzed carboncarbon cross-couplings represent one of the most straightforward, efficient and modular alternatives to build saturation in a single step. However, the efficient construction of alkyl-alkyl bonds remains a formidable challenge due to the precise manipulation of multiple alkyl metallic intermediates as well as associated competitive side reactions and selectivity control. Over the past years, Ni-catalyzed cross-coupling under reductive conditions has gained more and more attention for alkyl-alkyl crosscoupling partially attributing to the low-valent state of metal centers under reducing conditions, which suppresses the competitive β-hydride elimination process, thus facilitating the formation of alkyl-alkyl bonds. In this review, the initiative and progress of Ni-catalyzed cross-electrophile alkyl-alkyl cross-coupling, including the efforts in racemic and enantioselective formation of alkyl-alkyl bonds, have been summarized and discussed. Moreover, the challenges and further opportunities in this area have also been discussed.

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Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS

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Science China Chemistry 2025年

作者： Yuanjie Xu Zemin An Yu Tang institute of Molecular Engineering Plus Institute of Molecule Catalysis and In Situ/Operando Studies College of Chemistry Fuzhou University

X-ray photoelectron spectroscopy(XPS) is a crucial surface analysis technique that has become a key tool in the study of heterogeneous catalysis. Detecting surface chemistry under conditions that closely mimic actual industrial catalytic processes is essential for understanding the mechanisms involved. In the past decade, near ambient pressure X-ray photoelectron spectroscopy(NAP-XPS) has been increasingly utilized to study the surface chemistry of catalysts during heterogeneous catalytic processes, offering insights into structure-performance correlations. This review begins with a brief overview of NAP-XPS instrumentation. Next, we discuss the application of NAP-XPS in the study of thermal catalysis reactions, followed by a summary of the research on catalyst restructuring under reaction conditions. Additionally, we address the challenges and future perspectives for the development and application of NAP-XPS. catalysis is inherently dynamic, requiring an understanding of the real-time behavior of catalysts under varying conditions. Therefore, future improvements in the ability to probe reaction intermediates with higher spatial and temporal resolution under conditions that closely mimic industrial environments are needed.

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Simulations of electron zebra stripes in the inner radiation belt using a composite empirical electric field model

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Science China Earth Sciences 2025年第1期68卷 27-38页

作者： Ziyang WANG Ying LIU Qiugang ZONG Hong ZOU Yuguang YE Xuzhi ZHOU Chao YUE Shan WANG institute of Space Physics and applied Technology Peking University State Key Laboratory of Lunar and Planetary Science Macau University of Science and Technology

The phenomenon termed “zebra stripes” manifests as regular patterns in the energy-space(L shell) spectrum of energetic electrons(ranging from tens to hundreds ke V) within the inner radiation belt. These structures exhibit drift-periodic behavior and commonly arise from large-scale electric field perturbations near the substorm onsets. In this study, we introduce a composite electric field model and replicate the formation, structure, and evolution of zebra stripes using a bounce-averaged test particle code under this electric field model. High-resolution measurements of energetic electrons obtained from the Van Allen Probes and the recently launched Macao Science Satellites-1 are used as initial conditions and served to validate our test particle simulations. Comparative analyses between observed data and simulations demonstrate our test particle method's efficacy in capturing zebra stripes' general behavior. Moreover, the composite model proves capable of reproducing realistic variations in the electric field within the inner radiation belt to a certain extent. Nevertheless, subtle differences emerge in the flux strength and the positions of stripes. These disparities primarily stem from limitations inherent in the electric field model and the initial conditions of the simulation. Acknowledging that the model represents an average case, it is conceivable that real-world scenarios may deviate from the average, thereby introducing variations in the observed phenomena.

关键词： Zebra stripes Inner radiation belt Large-scale electric fields Van Allen Probes Macao Science Satellite

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First observation results of Macao Science Satellite-1 on lightning-induced electron precipitation

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Science China Earth Sciences 2025年第1期68卷 1-10页

作者： Yongping WANG Yixin SUN Qiugang ZONG Gaopeng LU Xudong GU Ze-Jun HU Bin LI Key Laboratory for Polar Science Ministry of Natural Resources Polar Research Institute of China institute of Space Physics and applied Technology Peking University State Key Laboratory of Lunar and Planetary Science Macau University of Science and Technology School of Earth and Space Sciences University of Science and Technology of China School of Electronic Information Wuhan University

The Medium-energy Electron Spectrometers(MES) is a space-borne instrument onboard Macao Science Satellite-1(MSS-1) dedicated to monitoring the typical charged particle radiation characteristics in the satellite orbit and the process of their occurrence and development, including short bursts of lightning-induced electron precipitation(LEP).This paper presents the first results of the LEP measurements by the MSS-1.47 LEP events are identified with the routine operation for 3 months since satellite launch, all within the range of 1.5

关键词： Lightning-induced electron precipitation Inner radiation belts Energetic electrons Macao Science Satellite-1

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