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Chinese chemical Letters 2024年第2期35卷 527-533页

作者： Yan-Hu Wang Ke-Wei Tong Chao-Qin Chen Jing Du Peng Yang college of chemistry and chemical engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China college of chemistry and Materials Science Testing and Analysis CenterHebei Normal UniversityShijiazhuang 050024China

A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak *** contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular *** this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence *** only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.

关键词： Polyoxometalates Polyoxovanadates Metal-organic polyhedron Interlock Weak intermolecular forces

Homogenous coating of Li^(+)conductive Li_(5)AlO_(4)on single-crystalline nonstoichiometric Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)for rechargeable lithium-ion batteries

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Journal of Energy chemistry 2024年第8期95卷 651-659,I0014页

作者： Guoyu Ding Shizhou Wang Jinhan Li Ziyan Wu Jiayu Chen Jiayong Du Xinhui Huang Kuiming Liu Yudong Zhang Zhonghan Wu Yiyang Peng Qiancheng Zhao Meng Yu Fangyi Cheng Key Laboratory of advanced Energy Materials chemistry(ministry of education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of advanced chemical Power Sources Nankai UniversityTianjin 300071China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China

Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate *** this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li_(5)AlO_(4)-coated single-crystalline slightly Li-rich Li_(1.04)Ni_(0.92)Al_(0.04)O_(2).The symbiotic formation of Li_(5)AlO_(4)from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li_(5)AlO_(4)that permits high Li^(+)*** from mitigated undesirable side reactions and phase evolution,the Li_(5)AlO_(4)-coated single-crystalline Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)delivers a high specific capacity of220.2 mA h g^(-1)at 0.1 C and considerable rate capability(182.5 mA h g^(-1)at 10 C).Besides,superior capacity retention of 90.8%is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full ***,the particulate morphology of Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li_(0.98)Ni_(0.97)Al_(0.05)O_(2)features intragranular cracks and irreversible lattice *** results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

关键词： Aluminum segregation Surface coating Nonstoichiometric oxides Molten synthesis Cathode materials

Anodic Electrosynthesis of Amide from Alcohol and Ammonia

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CCS chemistry 2024年第1期6卷 125-136页

作者： Yuxuan Lu Yingying Li Bo Zhou Jingcheng Wu Ling Zhou Yuping Pan Zhongcheng Xia Ming Yang Yandong Wu Zhenran Yuan Rixin Peng Zhijie Kong Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082 Shenzhen Institute of Hunan University Shenzhen 518057 School of chemistry and chemical engineering Jishou UniversityJishouHunan 416000

Amide is essential in biologically active compounds,synthetic materials,and building ***,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N ***,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient *** have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic *** C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with *** work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.

关键词： electrocatalysis electrocatalysts biomass upgrading elctrochemical oxidation coupling amide production

Experimental and theoretical investigation of sulfur-doped g-C_(3)N_(4)nanosheets/FeCo_(2)O_(4)nanorods S-scheme heterojunction for photocatalytic H_(2)evolution

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Nano research 2024年第9期17卷 8007-8016页

作者： Haitao Wang Lianglang Yu Jiahe Peng Jing Zou Weiping Gong Jizhou Jiang School of chemistry and Environmental engineering School of Environmental Ecology and Biological EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Guangdong Provincial Key Laboratory for Electronic Functional Materials and Devices Huizhou UniversityHuizhou 516007China

g-C_(3)N_(4)emerges as a promising metal-free semiconductor photocatalyst due to its cost-effectiveness,facile synthesis,suitable visible light response,and robust thermal ***,its practical application in photocatalytic hydrogen evolution reaction(HER)is impeded by rapid carrier recombination and limited light absorption *** this study,we successfully develop a novel g-C_(3)N_(4)-based step-scheme(S-scheme)heterojunction comprising two-dimensional(2D)sulfur-doped g-C_(3)N_(4)nanosheets(SCN)and one-dimensional(1D)FeCo_(2)O_(4)nanorods(FeCo_(2)O_(4)),demonstrating enhanced photocatalytic HER *** engineered SCN/FeCo_(2)O_(4)S-scheme heterojunction features a well-defined 2D/1D heterogeneous interface facilitating directed interfacial electron transfer from FeCo_(2)O_(4)to SCN,driven by the lower Fermi level of SCN compared to FeCo_(2)O_(4).This establishment of electron-interacting 2D/1D S-scheme heterojunction not only facilitates the separation and migration of photogenerated carriers,but also enhances visible-light absorption and mitigates electron-hole pair *** structure analysis and density functional theory calculations corroborate that the carrier migration in the SCN/FeCo_(2)O_(4)photocatalyst adheres to a typical S-scheme heterojunction mechanism,effectively retaining highly reactive photogenerated ***,the optimized SCN/FeCo_(2)O_(4)heterojunction exhibits a substantially high hydrogen production rate of 6303.5μmol·g^(-1)·h^(-1)under visible light excitation,which is 2.4 times higher than that of the ***,the conjecture of the S-scheme mechanism is confirmed by in situ XPS *** 2D/1D S-scheme heterojunction established in this study provides valuable insights into the development of high-efficiency carbon-based catalysts for diverse energy conversion and storage applications.

关键词： g-C_(3)N_(4) FeCo_(2)O_(4) S-scheme heterojunction photocatalytic hydrogen evolution reaction(HER)

Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano research 2024年第8期17卷 7163-7173页

作者： Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan Key Laboratory of advanced Energy catalytic and Functional Material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Key Laboratory of Materials Physics of ministry of education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Key Laboratory of chemical Reaction engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China center for High Pressure Science and Technology advanced research PudongShanghai 201203China Key Laboratory of advanced Energy Materials chemistry(ministry of education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

Unveiling the geometric site dependent activity of spinel Co_(3)O_(4)for electrocatalytic chlorine evolution reaction

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Journal of Energy chemistry 2024年第5期92卷 95-103页

作者： Linke Cai Yao Liu Jingfang Zhang Qiqi Jia Jiacheng Guan Hongwei Sun Yu Yu Yi Huang Key Laboratory of Pesticide&chemical Biology of ministry of education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina Key Laboratory of Green chemical engineering Process of ministry of education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina college of Materials Science and engineering Fuzhou UniversityFuzhou 350108FujianChina School of chemistry and chemical engineering Anhui UniversityHefei 230601AnhuiChina

Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost ***,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied *** by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity *** work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

关键词： Chlorine evolution reaction Geometry effects Active chlorine Electronic configuration optimization Spinel oxides

Green synthesis of luminescent La-MOF nanoparticle from waste poly(ethylene terephthalate) for high-performance in Fe(Ⅲ) detection

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Rare Metals 2024年第8期43卷 3833-3843页

作者： Zhi Gong Zhi-Kui Dai Zhi-Yue Dong Qiu-Xuan Liu Valentin AMilichko Hua-Jian Liu Jie Liu Ran Niu Jiang Gong Key Laboratory of Material chemistry for Energy Conversion and Storage Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringMinistry of EducationHuazhong University of Science and TechnologyWuhan 430074China School of chemical engineering and Pharmacy Wuhan Institute of TechnologyWuhan 430073China Collaborative Innovation center for advanced Organic chemical Materials Co-constructed by the Province and ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules and College of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China School of Physics and engineering ITMO UniversitySt.Petersburg197101Russia School of Materials Science and engineering Hubei UniversityWuhan430062China Guangdong Provincial Key Laboratory of Technique and Equipment for Macromolecular advanced Manufacturing School of Mechanical and Automotive EngineeringKey Laboratory of Polymer Processing EngineeringMinistry of EducationSouth China University of TechnologyGuangzhou 510641China

Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,***,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy ***,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly(-ethylene terephthalate)(PET) bottles and La(NO_(3))_(3)·_(6)H_(2)*** goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt(Na_(2)BDC) and ethylene glycol by ball ***,BDC reacts with La^(3+)to form *** as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred ***,La-MOF nanoparticles display high selectivity and sensitivity for Fe^(3+)*** quenching constant and limit of detection are 5.29×10^(3)(mol·L^(-1))^(-1) and 0.147 μmol·L^(-1),respectively,thus surpassing many advanced Fe^(3+) *** to the result of density functional theory,the high Fe^(3+) detection performance of La-MOF is related to the complexing of Fe^(3+)with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La^(3+).It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.

关键词： Metal-organic framework Waste polyester Mechanochemistry milling Fluorescence sensor

耦合异质结和Pd纳米颗粒的高效电荷接力促进CO2光还原为C2H6（英文）

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Science China Materials 2024年第9期67卷 2949-2956页

作者：方姣姣朱成洋方林灿陈雨凯胡慧玲吴艳陈庆庆毛俊杰 Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal University Jiangsu Key Laboratory of advanced catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterSchool of Petrochemical EngineeringChangzhou University

太阳能驱动CO2转换制备高附加值产品是实现碳中和的路径之一,但具有挑战性.CO2光转化实现多碳产物的关键是打破C-C耦合难和多电子转移效率低的瓶颈.本文报道了一种由Pd修饰的BiOCl包裹CuBi2O4组成的电荷接力系统,利用PdNPs和异质结的协... 详细信息

太阳能驱动CO2转换制备高附加值产品是实现碳中和的路径之一,但具有挑战性.CO2光转化实现多碳产物的关键是打破C-C耦合难和多电子转移效率低的瓶颈.本文报道了一种由Pd修饰的BiOCl包裹CuBi2O4组成的电荷接力系统,利用PdNPs和异质结的协同作用实现CO2-C2H6的高效光转换.在无牺牲剂条件下,C2H6产率达到167.1μmol g-1h-1,电子选择性为81.1%.光谱研究表明,BiOCl纳米片作为电荷中继站,将光生电子从自身和CuBi2O4纳米棒定向转移到Pd纳米颗粒（PdNPs）上进行C-C耦合.PdNPs与异质结的协同作用显著提高了电荷的分离和转移效率.原位表征和理论模拟均表明,由PdNPs和异质结组成的电荷接力系统产生的富电子PdNPs,优化了CO2到C2H6反应路径,降低了中间体*CHOCO的能垒.这项工作为发展高效的CO2光催化材料提供了思路.

关键词： charge relay Pd nanoparticles heterojunction CO2 photoreduction C2H6

Towards wafer-scale growth of two-dimensional cerium dioxide single crystal with high dielectric performance

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Nano research 2024年第9期17卷 8592-8599页

作者： Zhuofeng Shi Muhammad Imran Xiaohui Chen Xin Liu Yaqi Zhu Zhaoning Hu Saiyu Bu Jialin Zhang Chunhu Li Xiaodong Zhang Li Lin college of chemistry and chemical engineering Qingdao UniversityQingdao 266000China School of Materials Science and engineering Peking UniversityBeijing 100871China center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Key Laboratory of Marine chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

Owing to the atomically thin nature,two-dimensional(2D)oxide materials have been widely reported to exhibit exciting transport and dielectric properties,such as fine gate controllability and ultrahigh carrier mobility,that outperform their bulk ***,unlike the successful synthesis of bulk oxide single crystals,reliable methods for synthesizing large-area single crystal of 2D oxide,that would suppress the negative influence from defective grain boundaries,remain unavailable,especially for nonlayered ***,we report that the lattice symmetry between the substrate and cerium dioxide(CeO_(2))would allow for the aligned nucleation and epitaxial growth of CeO_(2)on sapphire substrates,enabling the wafer-sized growth of CeO_(2)single *** careful tuning of the growth temperature and oxygen flow rate contributed to the harvesting of CeO_(2)wafer with reduced thickness and enhanced growth *** removal of grain boundaries improved the dielectric performance in terms of high dielectric strength(Ebd≈8.8 MV·cm^(-1)),suppressed leakage current,along with high dielectric constants(εr≈24).Our work demonstrates that with fine dielectric performance and ease of synthesizing wafer-sized single crystals,CeO_(2)can function as potential candidate as gate insulator for 2D-materials based nanoelectronics,and we believe the reported protocol of aligned nucleation can be extended to other 2D oxides.

关键词： dielectric materials two-dimensional materials chemical vapor deposition cerium dioxide

MXenes/CNTs-based hybrids:Fabrications,mechanisms,and modification strategies for energy and environmental applications

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Nano research 2024年第5期17卷 3429-3454页

作者： Jizhou Jiang Fangyi Li Lei Ding Chengxun Zhang Arramel Xin Li School of Environmental Ecology and Biological engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Nano center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Emerging two-dimensional(2D)layered metal carbide and nitride materials,commonly termed MXenes,are increasingly recognized for their applications across diverse fields such as energy,environment,and *** the past few years,MXenes/carbon nanotubes(CNTs)-based hybrids have attracted extensive attention as an important catalyst in energy and environmental fields,due to their superior multifunctions and mechanical *** review aims to address the fabrication strategies,the identification of the enhancement mechanisms,and recent progress regarding the design and modification of MXenes/CNTs-based hybrids.A myriad of fabrication techniques have been systematically summarized,including mechanical mixing,spray drying,three-dimensional(3D)printing,self-assembly/in-situ growth,freeze drying,templating,hydrothermal methods,chemical vapor deposition(CVD),and ***,the identification of the enhancement mechanisms was thoroughly discussed from the two dimensions of theoretical simulations and in-situ ***,the recent advancements in profound applications of MXenes/CNTs-based hybrids have also been carefully revealed,including energy storage devices,sensors,water purification systems,and microwave *** also underscore anticipated challenges related to their fabrication,structure,underlying mechanisms,modification approaches,and emergent ***,this review offers insights into prospective directions and the future trajectory for these promising *** is expected that this review can inspire new ideas or provide new research methods for future studies.

关键词： MXenes/carbon nanotubes(CNTs)-based hybrids fabrication applications modification strategies