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Valence electron matching law for MXene-based single-atom catalysts

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Journal of Energy Chemistry 2025年第2期101卷 641-650页

作者： Pei Song Yuhang Zhou Zishan Luo Hang Zhang Xi Sun Sen Lu Zepeng Jia Hong Cui Weizhi Tian Rong Feng Lingxia Jin Hongkuan Yuan School of Mechanical Engineering Shaanxi University of Technology Shaanxi Key laboratory of Industrial Automation Shaanxi University of Technology Shaanxi Key laboratory of Catalysis College of Chemical & Environment Science Shaanxi University of Technology School of physical Science and Technology Southwest University

Single-atom catalysts（SACs） have attracted considerable interest in the fields of energy and environmental science due to their adjustable catalytic *** this study,we investigated the matching of valence electron numbers between single atoms and adsorbed intermediates（O,N,C,and H） in MXene-anchored SACs（M-Ti2C/M-Ti2CO2）.The density functional theory results demonstrated that the sum of the valence electron number（VM） of the interface-doped metal and the valence electron number（VA） of the adsorbed intermediates in M-Ti2C followed the 10-valence electron matching ***,based on the 10-valence electron matching law,we deduced that the sum of the valence electron number（k） and VMfor the molecular adsorption intermediate interactions in M-Ti2CO2adhered to the 11-valence electron matching *** repulsion between the interface electrons in M-Ti2CO2and H2O weakened the adsorption of intermediates,Furthermore,we applied the 11-valence electron matching law to guide the design of catalysts for nitrogen reduction reaction,specifically for N2→ NNH conversion,in the *** sure independence screening and sparsifying operator algorithm was used to fit a simple three-dimensional descriptor of the adsorbate（R2up to 0.970） for catalyst *** study introduced a valence electron matching principle between doped metals（single atoms） and adsorbed intermediates（atomic and molecular） for MXene-based catalysts,providing new insights into the design of high-performance SACs.

关键词： Density functional theory Nitrogen reduction reaction Sure independence screening and sparsifying operator Valence electron matching law

Gold-catalyzed intermolecular amination of allyl azides with ynamides: Efficient construction of 3-azabicyclo[3.1.0] scaffold

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Chinese chemical Letters 2025年第2期36卷 384-388页

作者： Chong-Yang Shi Jian-Xing Gong Zhen Li Chao Shu Long-Wu Ye Qing Sun Bo Zhou Xin-Qi Zhu College of Chemistry and chemical Engineering Yunnan Normal University Key laboratory of chemical Biology of Fujian Province State Key Laboratory of Physical Chemistry of Solid Surfacesand College of Chemistry and Chemical EngineeringXiamen University State Key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of Sciences Key laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong University

Gold-catalyzed amination reactions based on azides via α-imino gold carbene intermediates have attracted extensive attention in the past decades because this methodology leads to the facile and efficient construction of synthetically useful N-containing molecules, especially valuable N-heterocycles. However,successful examples of intermolecular generation of α-imino gold carbenes by using azides as amination reagents are rarely explored probably due to the weak nucleophilicity of azides. Herein, we disclose an efficient gold-catalyzed intermolecular aminative cyclopropanation of ynamides with the allyl azides, enabling flexible synthesis of a wide range of valuable 3-azabicyclo[3.1.0]hex–2-ene derivatives in good to excellent yields with excellent diastereoselectivities. Importantly, this protocol represents the first use of allyl azide as an efficient amination reagent in gold-catalyzed alkyne amination reactions.

关键词： Alkynes Amination Azides Gold Heterocycles

Engineering strategies of biomaterial-assisted exosomes for skin wound repair:Latest advances and challenges

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Chinese chemical Letters 2025年第1期36卷 99-109页

作者： Yang Xu Le Ma Yang Wang Chunmeng Shi Institute of Rocket Force medicine State Key Laboratory of Trauma and Chemical PoisoningThird Military Medical University(Army Medical University)Chongqing 400038China

The treatment of skin wounds,especially chronic wounds,remains a critical clinical challenge and places a heavy burden on patients and healthcare *** recent years,the engineering strategy of using biomaterial-assisted exosomes has emerged as a powerful tool for skin *** to treatments such as debridement and regular dressing changes,the design of biomaterial-assisted exosomes not only maintains the bioactivity of exosomes at the wound site but also provides an appropriate microenvironment for the repair of complex tissues,thereby accelerating wound *** review systematically introduces the general characteristics of exosomes and their functions in skin wound healing,highlights recent advances in classification of natural exosomes and engineering methods which enriching their functions in intercellular ***,various emerging and innovative approaches based on biomaterials delivery of exosomes are comprehensively *** review seeks to bring an in-depth understanding of bioactive dressings based on exosomes therapeutic strategies,aiming to facilitate new clinical application value.

关键词： Exosomes Biomaterials Hydrogel Delivery system Wound healing

Interface engineering of Pt/CeO2-{100} catalysts for enhancing catalytic activity in auto-exhaust carbon particles oxidation

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Chinese chemical Letters 2025年第2期36卷 195-200页

作者： Peng Zhang Yitao Yang Tian Qin Xueqiu Wu Yuechang Wei Jing Xiong Xi Liu Yu Wang Zhen Zhao Jinqing Jiao Liwei Chen State Key laboratory of Heavy Oil Processing Key Laboratory of Optical Detection Technology for Oil and GasCollege of ScienceChina University of Petroleum School of Chemistry and chemical In-situ Center for Physical SciencesFrontiers Science Center for Transformative MoleculesShanghai Jiao Tong University School of Chemistry and chemical Engineering Ningxia University School of Environmental Science and Engineering Yancheng Institute of Technology State Key laboratory of chemical Safety SINOPEC Research Institute of Safety Engineering Co.Ltd.

Herein,we fabricate an embedding structure at the interface between Pt nanoparticles （NPs） and CeO2-{100}nanocubes with surface defect sites （CeO2-SDS） through quenching and gas bubbling-assisted membrane reduction *** in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/*** a result,the distinctive geometric structure of Pt/CeO2-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T50and TOF values are 332°C and 2.915 h-1,*** with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO2-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO2-{100}support,and induce the formation of interfacial[Ce-Ox-Pt2]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular *** a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.

关键词： Catalytic oxidation Defective ceria Nanocube Pt NPs Soot particles

Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles

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Science China Chemistry 2025年第2期68卷 649-660页

作者： Ying-Qi Zhang Gan-Lu Qian Yun Liu Jia-Hui Li Xin Hong Zhou Xu Bo Zhou Long-Wu Ye State Key laboratory of physical Chemistry of Solid Surfaces Key Laboratory of Chemical Biology of Fujian Provinceand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Center of Chemistry for Frontier Technologies Department of ChemistryState Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027China Jiangsu Key laboratory of New Drug Research and Clinical Pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China State Key laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China State Key laboratory of Organometallic Chemistry Chinese Academy of SciencesShanghai 200032China

Herein,we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenoltethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic ***,the related dearomatized selenation and protonation are also achieved,affording the corresponding selenated and protonated spirocycles in high ***,the enantioselectivities of these products can be perfectly induced by Evans auxiliaries(99%ees).Significantly,this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives,but also constitutes the first asymmetric halogenation/selenation of *** calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.

关键词： alkynes cyclization dearomatization Evans chiral auxiliary spirocycles

Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina State Key laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina laboratory of physical-chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of BelarusMinsk 220072Belarus State Key laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and TechnologySchool of Marine Science and EngineeringHainan UniversityHaikou 570228HainanChina Department of chemical and Environmental Engineering University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina

Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Engineered iron-based metal-organic frameworks nanoplatforms for cancer theranostics: A mini review

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Chinese chemical Letters 2025年第2期36卷 80-93页

作者： Yunlong Li Xinyu Zhang Shuang Liu Chunsheng Li Qiang Wang Jin Ye Yong Lu Jiating Xu Key laboratory of Forest Plant Ecology Ministry of Education College of Chemistry Chemical Engineering and Resource Utilization Northeast Forestry University School of laboratory medicine Wannan Medical College Heilongjiang Provincial Key laboratory of Ecological Utilization of Forestry-Based Active Substances Northeast Forestry University

Up to now, numerous emerging methods of cancer treatment including chemodynamic therapy, photothermal therapy, photodynamic therapy, sonodynamic therapy, immunotherapy and chemotherapy have rapidly entered a new stage of development. However, the single treatment mode is often constrained by the complex tumor microenvironment. Recently, the nanomaterials and nanomedicine have emerged as promising avenues to overcome the limitation in cancer theranostics. Especially, metal-organic frameworks (MOFs) have gained considerable interests in cancer therapy because of their customizable morphologies, easy functionalization, large specific surface area, and good biocompatibility. Among these MOFs, iron-based MOFs (Fe-MOFs) are particularly promising for cancer treatment due to their properties as nano-photosensitizers, peroxidase-like activity, bioimaging contrast capabilities, and *** their structural regularity and synthetic tunability, Fe-MOFs can be engineered to incorporate organic molecules or other inorganic nanoparticles, thereby creating multifunctional nanoplatforms for single or combined theranostic modes. Herein, the minireview focuses on the recent advancements of the Fe-MOFs-based nanoplatforms for self-enhanced imaging and treatment at tumor sites. Furthermore,the clinical research development of Fe-MOFs-based nanoplatforms is discussed, addressing key challenges and innovations for the future. Our review aims to provide novice researchers with a foundational understanding of advanced cancer theranostic modes and promote their clinical applications through the modification of Fe-MOFs.

关键词： Bioimaging Cancer theranostics Catalytic therapy Engineered nanoplatforms Fe-based MOFs

Direct seawater splitting for hydrogen production:Recent advances in materials synthesis and technological innovation

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Green Energy & Environment 2025年第1期10卷 11-33页

作者： Yilin Zhao Zhipeng Yu Aimin Ge Lujia Liu Joaquim Luis Faria Guiyin Xu Meifang Zhu State Key laboratory for Modification of chemical Fibers and Polymer Materials Center for Advanced Low-dimension MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai201620China International Iberian Nanotechnology laboratory(INL) Avenida Mestre Jose VeigaBraga4715-330Portugal The MacDiarmid Institute for Advanced Materials and Nanotechnology School of Chemical and Physical SciencesVictoria University of WellingtonWellington6012New Zealand LSRE-LCM-laboratory of Separation and Reaction Engineering-laboratory of Catalysis and Materials Faculty of EngineeringUniversity of PortoRua Dr.Roberto Frias s/nPorto4200-465Portugal ALiCE-Associate laboratory in chemical Engineering Faculty of EngineeringUniversity of PortoRua Dr.Roberto Frias s/nPorto4200-465Portugal

Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil ***,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in ***,producing hydrogen on an industrial scale is challenging due to the high production *** present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater *** the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater *** the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater ***,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.

关键词： Seawater splitting Catalyst Membranes Mixed seawater systems Self-powered systems

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Unraveling atomistic and electronic origins of multiaxial magnetic anisotropy

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Science China(Physics,Mechanics & Astronomy) 2025年第2期68卷 175-182页

作者： Boyu Liu Xueyang Li Junsheng Feng Changsong Xu Hongjun Xiang Key laboratory of Computational physical Sciences(Ministry of Education) Institute of Computational Physical SciencesState Key Laboratory of Surface Physics and Department of PhysicsFudan UniversityShanghai200433China Shanghai Qi Zhi Institute Shanghai200030China School of Physics and Material Engineering Hefei Normal UniversityHefei230601China

Multiaxial magnetic anisotropy(MA)refers to the phenomenon that multiple axes of the magnetic crystal correspond to different energy *** with the common uniaxial magnetic anisotropy,multiaxial MA facilitates novel forms of applications in ***,by combining the first-principles-based spin Hamiltonian and tight-binding(TB)method,we reveal the microscopic origins,instead of the common phenomenological understanding,of biaxial MA and triaxial *** the example system of NiO,it is found that the multiple minima result from the fourth-order and the sixth-order single ion interactions,while the difference between[110]and[110]directions originates from a second-order bond-dependent anisotropic pair interaction(i.e.,the so-called Gamma interaction).Moreover,through the application of a newly developed general spin dependent TB approach,it is revealed that the triaxial MA arises from the special spin-orbital entangled Hund term,which is different from the orbital-independent Hund term in the usual Slater Koster TB *** work thus not only leads to a thorough understanding of the multiaxial MA in NiO,but also establishes a methodology that can be widely used to explore the microscopic origins of MA in different magnets.

关键词： multiaxial magnetic anisotropy origin of multiaxial magnetic mnisotropy effective spin Hamiltonian tight-binding model antiferromagnetism

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