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Lattice-mismatch-induced formation of defect-rich Pd-Cu alloy nanocages for enhanced formic acid oxidation activity

Science China Chemistry 2025年第2期68卷 481-491页

作者： Zhaojun Liu Zhengyan Wang Zhaoyu Wang Hao Yuan Yuke Bai Xiaoxiao Wang Zerui Mu Chunxia Wu Kai Liu Zhun Hu Chuanbo Gao Sate Key Laboratory of Multiphase Flow in Power Engineering Frontier Institute of Science and TechnologyXi’an Jiaotong UniversityXi’an 710049China institute of Industrial Catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China

Crystallographic defects in noble metal nanocrystals are recognized as highly active catalytic sites,significantly enhancing activities in many important *** their importance,synthesizing noble metal nanocrystals with a high density of defects poses a considerable synthetic ***,we present a novel lattice mismatch-induced formation mechanism to create high-density defects in noble metal *** approach takes advantage of lattice mismatch to enable nonepitaxial nucleation and growth of a noble metal on a foreign metal substrate,forming abundant noble metal crystallites with random lattice orientations not dictated by the substrate *** these crystallites grow extensively,they merge,forming numerous grain boundaries and yielding defect-rich noble metal ***-rich alloy nanocrystals can also be synthesized through a subsequent vacancy-diffusion alloying *** take defective PdCu alloy nanocages as an example and demonstrate the effectiveness of crystallographic defects in enhancing catalytic performance of noble metal *** nanocages exhibit superior activity in the electrocatalytic formic acid oxidation reaction,which is 1.6 times greater than their defect-free *** strategy offers a new avenue for creating defect-rich noble metal nanocrystals as highly efficient catalysts for a wide array of catalytic applications.

关键词： noble metal nanocrystals defects non-epitaxial growth electrocatalysis formic acid oxidation reaction

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Structural engineering of high-entropy alloys for advanced electrocatalytic reactions

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Tungsten 2025年第1期7卷 1-31页

作者： Qiao Xie Ying-Jie Yu Hai-Jun Zhang Ya-Ping Deng Wen Lei The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and Technology Department of chemical Engineering Waterloo Institute for Sustainable Energy Waterloo Institute for Nanotechnology University of Waterloo

High-entropy alloys(HEAs) have emerged as promising candidates to replace traditional precious metal catalysts,owing to their unique chemical and physical *** review commences by revisiting the fundamental concepts of HEAs,including their synthesis methods and structural control strategies in *** underscores the critical role of meticulously manipulating both macroscopic and microscopic structures of the HEAs to optimize their catalytic performance.A deep understanding of the structure-activity relationship in HEAs across various configurations is pivotal in developing more effective *** review methodically encapsulates the research progress of structural control strategies for HEAs in achieving efficient energy conversion,with the aim of gaining a better understanding of the relationship between structure and *** review concludes by summarizing the current achievements and challenges,and suggestions for potential future directions of HEAs in the fields of energy conversion and environmental purification.

关键词： Electrocatalytic Energy conversion High-entropy alloys Structural modulation

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Molecular-based porous polymers with precise sites for photoreduction of carbon dioxide

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Chinese chemical Letters 2025年第1期36卷 201-213页

作者： Wei-Jia Wang Kaihong Chen College of Biological and chemical Engineering Zhejiang University of Science and TechnologyHangzhou 310023China The institute of Green Chemistry and Engineering School of Chemistry and Chemical EngineeringNanjing UniversitySuzhou 215163China

Photocatalytic CO_(2)reduction reaction(CO_(2)RR)is one of the promising strategies for sustainably producing solar *** precise identification of catalytic sites and the enhancement of photocatalytic CO_(2)conversion is imperative yet quite *** critical review summarizes recent advances in porous photo-responsive polymers,including covalent organic frameworks(COFs),covalent triazine frameworks(CTFs),and conjugated microporous polymers(CMPs),those can be rationally designed from the molecular level for visible-light-driven photocatalytic CO_(2)***,special emphasis is placed on how the well-defined active sites on these polymers can influence their properties and photocatalytic *** precise regulation and control of microenvironments and electronic properties of metal active centers are crucial for boosting catalytic efficiency and selectivity,as well as for the design of better photocatalysts for CO_(2)reduction.

关键词： Carbon dioxide reduction Photocatalysis Porous polymers Well-defined catalytic sites Molecular level

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Breaking Solvation Dominance Effect Enabled by Ion-Dipole Interaction Toward Long-Spanlife Silicon Oxide Anodes in Lithium-Ion Batteries

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Nano-Micro Letters 2025年第4期17卷 367-380页

作者： Shengwei Dong Lingfeng Shi Shenglu Geng Yanbin Ning Cong Kang Yan Zhang Ziwei Liu Jiaming Zhu Zhuomin Qiang Lin Zhou Geping Yin Dalong Li Tiansheng Mu Shuaifeng Lou State Key Laboratory of Space Power-Sources School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China School of Marine Science and technology Harbin Institute of Technology at WeihaiWeihai 264200People’s Republic of China Chongqing Research institute of HIT Chongqing 401135People’s Republic of China

Micrometer-sized silicon oxide(SiO)anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy ***,an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO *** functional theory calculations validate a robust ion-dipole interaction between lithium ions(Li^(+))and succinonitrile(SN).The cosolvent fluoroethylene carbonate(FEC)optimizes the Li^(+)solvation structure in the SN-based electrolyte with its weakly solvating *** dynamics simulations investigate the regulating mechanism of ion-dipole and cation-anion *** unique Li^(+)solvation structure,enriched with FEC and TFSI^(-),facilitates the formation of an inorganic-organic composite solid electrolyte interphase on SiO ***-CT further detects the inhibiting effect on the SiO volume *** a result,the SiO|LiCoO_(2) full cells exhibit excellent electrochemical performance in deep eutectic-based *** work presents an effective strategy for extending the cycle life of SiO anodes by designing a new SN-based deep eutectic electrolyte.

关键词： Lithium-ion batteries Micrometer-sized silicon oxide Ion-dipole interaction Long-term cycling

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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 EngineeringDalian University of TechnologyDalian 116024 State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

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： MFI zeolite ZSM-5 Nanosheets Scale-up synthesis Aromatic alkylation

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

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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 SciencesDalian 116023China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

The methanol-to-olefins(MTO)reaction offers an alternative pathway for the production of low-carbon olefins from non-oil *** research has been impeded by a lack of comprehensive understanding of its underlying mechanism,despite the significant progress made 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 ***,the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of in-situ^(13)C MAS NMR and 2D correlation ***,recent technological advancements in hyperpolarization(HP)methods,including HP^(129)Xe NMR and dynamic nuclear polarization(DNP),have significantly improved the sensitivity of ssNMR,enabling detailed structural and kinetic analysis as well as the detection of trace *** this feature article,we summarized recent advancements in(in-situ)ssNMR spectroscopy applied to MTO reaction processes,encompassing mechanistic investigations at various stages and the intricate host–guest *** 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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Constructing Ti_(3)C_(2)T_(x)-MXene-based gradient woodpile structure by direct ink writing 3D printing for efficient microwave absorption

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International Journal of Minerals,Metallurgy and Materials 2025年第3期32卷 657-667页

作者： Changtian Zhu Pei Liu Jin Chen Zixuan Ding Guohui Tang Qingqing Gao Yinxu Ni Kai Xu Zhilei Hao Gaojie Xu Fenghua Liu School of Materials Science and chemical Engineering Ningbo UniversityNingbo 315211China Ningbo institute of Materials technology&Engineering Chinese Academy of SciencesNingbo 315201China

As a novel 2D material,Ti_(3)C_(2)T_(x)-MXene has become a major area of interest in the field of microwave absorption(MA).However,the MA effect of common Ti_(3)C_(2)T_(x)-MXene is not prominent and often requires complex processes or combinations of other ma-terials to achieve enhanced *** this context,a kind of gradient woodpile structure using common Ti_(3)C_(2)T_(x)-MXene as MA ma-terial was designed and manufactured through direct ink writing(DIW)3D *** minimum reflection loss(RL_(min))of the Ti_(3)C_(2)T_(x)-MXene-based gradient woodpile structures with a thickness of less than 3 mm can reach-70 dB,showing considerable improve-ment compared with that of a completely filled *** addition,the effective absorption bandwidth(EAB)reaches 7.73 *** study demonstrates that a Ti_(3)C_(2)T_(x)-MXene material with excellent MA performance and tunable frequency band can be successfully fab-ricated with a macroscopic structural design and through DIW 3D printing without complex material hybridization and modification,of-fering broad application prospects by reducing electromagnetic wave radiation and interference.

关键词： Ti_(3)C_(2)T_(x)-MXene electromagnetic wave absorption macro-design impedance matching 3D printing ink

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Auxiliary ligand-induced assembly of atomically precise silver clusters

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Science China Chemistry 2025年第2期68卷 580-589页

作者： Yeqin Feng Xuemeng Jing Fangyu Fu Mengyun Zhao Manzhou Chi Hongjin Lv Guo-Yu Yang MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

Establishing the correlation between inter-cluster assembly and auxiliary ligands at the atomic level is crucial for the development of metal cluster *** this work,we report the successful preparation and characterization of three Ag clusters,discrete 0-D Ag_(51)S_(6)Cl_(3)(i PrS)_(21)(TsO)_(15)CH_(3)CN(0-D Ag_(51),i PrS–=isopropanethiolate,TsO–=toluenesulfonate),1-D{Ag_(38)S_(4)-(i PrS)_(18)(PhCOO)_(12)}n(1-D Ag_(38),PHCOO–=benzoate),and 2-D{Ag_(2)0(SO_(4))Cl_(2)(i PrS)10(NO_(3))6}n(2-D Ag_(20)),using a delicate auxiliary-ligand-induced *** analyses reveal that the types of auxiliary ligands can readily affect the structure and dimensionality of resulting Ag *** addition of different surface auxiliary ligands from TsO–to PhCOO–and then to NO_(3)–leads to the formation of 0-D Ag_(51) to 1-D Ag_(38) and then to 2-D Ag_(2)0 clusters under otherwise identical reaction conditions,*** resulting Ag clusters exhibited structure-related optical/luminescence properties and distinct bathochromic shifts as revealed by the temperature-dependent luminescence and single-crystal X-ray diffraction studies.

关键词： silver(I)clusters auxiliary ligand effect silver cluster synthesis luminescence

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Metrological traceable calibration of organic carbon and elemental carbon based on laboratory-generated reference materials

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Journal of Environmental Sciences 2025年第3期149卷 524-534页

作者： Yue Liu Junjie Liu Ji Xiao Jing Ye Lixu Guo Caiqing Yan Center for Environmental Metrology National Institute of Metrology ChinaBeijing 100029China College of Chemistry and chemical Engineering Taiyuan University of TechnologyTaiyuan 030024China Environment Research institute Shandong UniversityQingdao 266237China

Carbonaceous aerosol,including organic carbon(OC)and elemental carbon(EC),has significant influence on human health,air quality and climate *** measurement of carbonaceous aerosol is essential to reduce the uncertainty of radiative forcing estimation and source *** accurate separation of OC and EC is controversial due to the charring of ***,the development of reference materials(RM)for the validation of OC/EC separation is an important basis for further *** RMs were mainly based on ambient air sampling,which could not provide traceability of OC and EC *** develop traceable RMs with known OC/EC contents,our study applied an improved aerosol generation and mixing technique,providing uniform deposition of particles on quartz *** generate OC aerosol with similar pyrolytic property of ambient aerosol,both water soluble organic carbon(WSOC)and water insoluble organic carbon(WIOC)were used,and amorphous carbon was selected for EC *** RMs were analyzed using different *** homogeneity within the filter was validated,reaching below 2%.The long-term stability of RMs has been validated with RSD ranged from 1.7%–3.2%.Good correlationwas observed between nominal concentration of RMswithmeasured concentration by two protocols,while the difference of EC concentration was within 20%.The results indicated that the newly developed RMs were acceptable for the calibration of OC and EC,which could improve the accuracy of carbonaceous aerosol ***,the laboratory-generated EC-RMs could be suitable for the calibration of equivalent BC concentration by Aethalometers.

关键词： Carbonaceous aerosol Split point Reference material Laboratory-generated Traceability

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Efficient remediation of different concentrations of Cr-contaminated soils by nano zero-valent iron modified with carboxymethyl cellulose and biochar

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Journal of Environmental Sciences 2025年第1期147卷 474-486页

作者： Lihong Xie Qiyan Ma Qingjun Chen Yiyang Liu Pengfei Guo Jinlan Zhang Guilan Duan Aijun Lin Tingting Zhang Shangyi Li Department of Environmental Science and Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China China National Petroleum and chemical Planning institute Beijing 100013China State Key Laboratory of Urban and Regional Ecology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

Nano zero-valent iron(nZVI)is widely used in soil remediation due to its high ***,the easy agglomeration,poor antioxidant ability and passivation layer of Fe-Cr coprecipitates of nZVI have limited its application scale in Cr-contaminated soil remediation,especially in high concentration of Cr-contaminated ***,we found that the carboxymethyl cellulose on nZVI particles could increase the zeta potential value of soil and change the phase of *** with the presence of biochar,97.0%and 96.6%Cr immobilization efficiency through CMC-nZVI/BC were respectively achieved in high and low concentrations of Cr-contaminated soils after 90-days *** addition,the immobilization efficiency of Cr(VI)only decreased by 5.1%through CMC-nZVI/BC treatment after 10 weeks aging in air,attributing to the strong antioxidation *** for the surrounding Crcontaminated groundwater,the Cr(VI)removal capacity of CMC-nZVI/BC was evaluated under different reaction conditions through column experiments and COMSOL ***-nZVI/BC could efficiently remove 85%of Cr(VI)in about 400 hr when the initial Cr(VI)concentration was 40 mg/L and the flow rate was 0.5 mL/*** study demonstrates that uniformly dispersed CMC-nZVI/BC has an excellent remediation effect on different concentrations of Cr-contaminated soils.

关键词： Carboxymethyl cellulose Nanoscale zero-valent iron Biochar Cr-contaminated soils

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