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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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Potential dependence in electrocatalysis: a theoretical perspective

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Science China Chemistry 2025年第1期68卷 21-25页

作者： Leyu Liu Zhaoming Xia Zeyu Wang Yinjuan Chen Hai Xiao department of Chemistry Tsinghua University Fundamental Science Center of Rare Earths Ganjiang Innovation Academy Chinese Academy of Sciences Key Laboratory of Advanced Catalytic Materials and technology Advanced Catalysis and Green Manufacturing Collaborative Innovation Center Changzhou University

Electrocatalysis is a key technology for the new energy era and sustainable development, serving as the interface for interconversion of electrical and chemical energies, which spans a wide spectrum of applications in sustainable energy and environmental engineering. Electrocatalytic reactions including electrochemical CO2reduction reaction （eCO2RR）, hydrogen evolution reaction （HER）, and oxygen evolution/reduction reactions （OER/ORR）, hold essential promise for renewable energy technologies as well as complement the biogeochemical carbon and oxygen cycles.

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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology State Key Laboratory of catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： Aspect ratio

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High-throughput screening of CO_(2) cycloaddition MOF catalyst with an explainable machine learning model

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Green Energy & Environment 2025年第1期10卷 132-138页

作者： Xuefeng Bai Yi Li Yabo Xie Qiancheng Chen Xin Zhang Jian-Rong Li Beijing Key Laboratory for Green catalysis and Separation and department of Chemical Engineering College of Materials Science&EngineeringBeijing University of TechnologyBeijing100124China

The high porosity and tunable chemical functionality of metal-organic frameworks(MOFs)make it a promising catalyst design ***-throughput screening of catalytic performance is feasible since the large MOF structure database is *** this study,we report a machine learning model for high-throughput screening of MOF catalysts for the CO_(2) cycloaddition *** descriptors for model training were judiciously chosen according to the reaction mechanism,which leads to high accuracy up to 97%for the 75%quantile of the training set as the classification *** feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding.12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100℃ and 1 bar within one day using the model,and 239 potentially efficient catalysts were *** them,MOF-76(Y)achieved the top performance experimentally among reported MOFs,in good agreement with the prediction.

关键词： Metal-organic frameworks High-throughput screening Machine learning Explainable model CO_(2)cycloaddition

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Comparative Evaluation and Performance Analysis of Heat Exchangers Featured with Peened Surface

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Journal of Thermal Science 2025年第1期34卷 50-61页

作者： DINESHBABU Chinnadurai SHIVA SANKARAN Nallasamy VENKATESH RAJA Krishnan VENKATESH Rathinavelu department of Mechanical Engineering Kongunadu College of Engineering and Technology department of Mechanical Engineering Selvam College of Technology department of Mechanical Engineering Sona College of Technology department of Mechanical Engineering Saveetha School of EngineeringSaveetha Institute of Medical and Technical Sciences (SIMATS)Saveetha University

Heat exchangers have the potential for various engineering applications,and their performance is enriched by surface *** proposed system enriches the heat exchanger's performance by adapting a peened stainless steel（SS） surface blasted with copper,grinding,sand,and *** influences peened SS surface modified with a copper blast,grinding,sandblast,and iron blast on the surface morphology of shell and tube heat exchanger surface（STHE） is analyzed via tungsten heated cathode electron gun featured scanning electron microscope and observed coarse grain *** SS surface featured STHE performance is experimentally evaluated by different flow rates（30,60,90,and 120 L/min） underwater fluid medium functioned by the temperature ranges of 25-75℃ and its results are compared with computational fluid dynamic（CFD）/heat transfer research（HTRI） analyzed *** 60 L/min flow rate was spotted as an optimum value for both shell and tube side *** STHE is operated with a 60 L/min flow rate under the different peened surfaces and evaluated its Stanton number,Nusselt number,logarithmic mean temperature difference（LMTD）,overall heat transfer coefficient,number of transfer units（NTU）,effectiveness,and exergy *** iron blasted SS peened surface was observed to have better SHTE performance like Stanton number（0.0012）,Nusselt number（2180）,reduced LMTD of 31℃,improved overall heat transfer co-efficient of 2400 W/（m2·K）,better NTU of 0.5532,good effectiveness value of 0.451 62,and hiked exergy efficiency of 10% respectively.

关键词： penned surface performance analysis shell and tube heat exchanger stainless steel

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Electrochemical sensor for dopamine detection based on multiwalled carbon nanotube/molybdenum disulfide quantum dots with machine learning integration and anti-interference capability

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Tungsten 2025年第1期7卷 137-151页

作者： Geethukrishnan Onkar Apte Kiran Kumar Tadi Energy Electrodics and Electrocatalysis (EEE) Lab Department of Chemistry School of Advanced Sciences Vellore Institute of Technology School of Computer Science and Engineering Vellore Institute of Technology

The precise detection and measurement of dopamine（DA）,a crucial neurotransmitter in the human body,plays a significant role in diagnosing,preventing,and treating neurological diseases associated with its levels.A highly sensitive DA electrochemical sensor was constructed by combining molybdenum disulfide quantum dots（MSQDs） with multiwalled carbon nanotubes（MWCNTs）.The MSQDs were synthesized using the shear exfoliation *** sensors consist of MSQDs with Mo-S edge catalytic centers for the DA redox reaction,and MWCNTs amplify the sensor *** linearity of the sensor for the detection of DA was tested in the presence of ascorbic acid(AA,50 μmol·L-1) and uric acid(UA,200 μmol·L-1),and exhibited linearity from 2 to 966 μmol·L-1of DA with 0.097 μA(mol·L-1)-1sensitivity and a low limit of detection of0.6 μmol·L-1（the ratio between signal and noise,S/N=3）.Moreover,the sensitivity and selectivity of the sensor were also studied using *** is no increase in amperometric current after adding the most potentially interfering *** sensor was successfully applied to recover DA in human blood sera ***,machine learning algorithms were operated to aid in the near-precise detection of DA in the heterogeneous mixture containing AA and *** algorithms facilitate the identification and quantification of DA amidst coexisting interferents,including AA,that are commonly present in biological matrices.

关键词： Biosensor Complex mixture Dopamine Machine learning MoS2 Multiwalled carbon nanotubes

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A low redox potential and long life organic anode material for sodium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 557-564页

作者： Zhi Li Yang Wei Kang Zhou Xin Huang Xing Zhou Jie Xu Taoyi Kong Junwei Lucas Bao Xiaoli Dong Yonggang Wang department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and Innovative Materials Institute of New Energy Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Fudan University department of Chemistry Boston College School of Materials Science and Engineering Anhui University of Technology

Sodium-ion batteries （SIBs） with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ***,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials（>1 V）.Organic electrodes with low redox potential that can be used as anode are ***,a novel organic anode material （tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na4TDC） has been developed with low redox potential （<0.7 V） and excellent cyclic *** three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per ***,the Na4TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg *** pairing with a thick Na3V2（PO4）3cathode (20.6 mg cm-2),the as-fabricated full cell exhibited high operating voltage （2.8 V）,excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na4TDC anode material for SIBs.

关键词： Organic anode material Low redox potential Composite anode Sodium-ion batteries

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Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and Innovative Materials Fudan University State Key Laboratory of catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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Regression analysis of squeezing-induced hybrid nanofluid flow in Darcy-Forchheimer porous medium

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Applied Mathematics and Mechanics(English Edition) 2025年第1期46卷 193-208页

作者： K.MUHAMMAD M.SARFRAZ department of Humanities and sciences School of Electrical Engineering and Computer Science National University of Sciences and Technology department of Mathematics Quaid-i-Azam University

This article presents a mathematical model addressing a scenario involving a hybrid nanofluid flow between two infinite parallel plates. One plate remains stationary, while the other moves downward at a squeezing velocity. The space between these plates contains a Darcy-Forchheimer porous medium. A mixture of water-based fluid with gold(Au) and silicon dioxide(Si O2) nanoparticles is formulated. In contrast to the conventional Fourier's heat flux equation, this study employs the Cattaneo-Christov heat flux equation. A uniform magnetic field is applied perpendicular to the flow direction, invoking magnetohydrodynamic(MHD) effects. Further, the model accounts for Joule heating, which is the heat generated when an electric current passes through the fluid. The problem is solved via NDSolve in MATHEMATICA. Numerical and statistical analyses are conducted to provide insights into the behavior of the nanomaterials between the parallel plates with respect to the flow, energy transport, and skin *** findings of this study have potential applications in enhancing cooling systems and optimizing thermal management strategies. It is observed that the squeezing motion generates additional pressure gradients within the fluid, which enhances the flow rate but reduces the frictional drag. Consequently, the fluid is pushed more vigorously between the plates, increasing the flow velocity. As the fluid experiences higher flow rates due to the increased squeezing effect, it spends less time in the region between the plates. The thermal relaxation, however, abruptly changes the temperature, leading to a decrease in the temperature fluctuations.

关键词： Nanofluidics

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Propagating subduction initiation of the Caroline Plate at the Mussau Trench

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Science China Earth sciences 2025年第1期68卷 253-269页

作者： Chun-Feng LI Yongkang DENG Tao WU Dongdong DONG Guoliang ZHANG Jiazheng ZHANG Yutao LIU Yaqing LI Fugui TANG Lulu ZHANG department of Marine sciences Zhejiang University Laboratory of Marine Mineral Resources Laoshan Laboratory Key Lab of Marine Geology and Environment Institute of Oceanology Chinese Academy of Sciences Key Lab of Ocean and Marginal Sea Geology South China Sea Institute of Oceanology Chinese Academy of Sciences Science & technology on Integrated Information System Lab Institute of Software Chinese Academy of Sciences

New seismic imaging from the Mussau Trench confirms that, under horizontal compression on an oceanic plate boundary, it is within the young and weak oceanic plate that a trench will develop, and it is the young plate, not so long after its birth, that starts to subduct toward the old plate. The Mesozoic Pacific Plate cannot easily bend, under the joint horizontal compression and vertical gravity pull, even with a pre-existing weak zone in place and with a large age offset across the plate boundary. The bending of the Caroline Plate near the northern end of the Mussau Trench started only after a long-time span of trench migration, and/or after a prolonged transition from initial compression to trench development. Highly contrasting trench deformation and sedimentary accretion between two parallel seismic sections support an evident migration of underthrusting or significant longitudinal heterogeneity along the trench. The swift transition from underthrusting to non-thrusting can be explained by a counter-clockwise rotation of the Caroline Plate. That miniature accretionary wedges develop even before the subduction initiates imply strong compression and uplifting before the underthrusting can kick-start. Rotation of the Caroline Plate have been halted as the Mussau Trench is seismically rather quiet and the Lyra Trough to the east shows relaxational extension.

关键词： Mussau Trench Subduction initiation Seismic reflection Caroline Plate

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