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Phase-engineering modulation of Mn-based oxide cathode for constructing super-stable sodium storage

Journal of Energy chemistry 2024年第1期88卷 421-427,I0010页

作者： Quanqing Zhao Ruru Wang Ming Gao Bolin Liu Jianfeng Jia Haishun Wu Youqi Zhu Chuanbao Cao Key Laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032ShanxiChina Metals and chemistry research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China research center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The Mn-based oxide cathode with enriched crystal phase structure and component diversity can provide the excellent chemistry structure for Na-ion ***,the broad application prospect is obstructed by the sluggish Na^(+)kinetics and the phase transitions upon ***,we establish the thermodynamically stable phase diagram of various Mn-based oxide composites precisely controlled by sodium content tailoring strategy coupling with co-doping and solid-state *** chemical environment of the P2/P'3 and P2/P3 biphasic composites indicate that the charge compensation mechanism stems from the cooperative contribution of anions and *** from the no phase transition to scavenge the structure strain,P2/P'3 electrode can deliver long cycling stability(capacity retention of 73.8%after 1000 cycles at 10 C)and outstanding rate properties(the discharge capacity of 84.08 mA h g^(-1)at 20 C)than P2/P3 ***,the DFT calculation demonstrates that the introducing novel P'3 phase can significantly regulate the Na^(+)reaction dynamics and modify the local electron configuration of *** effective phase engineering can provide a reference for designing other high-performance electrode materials for Na-ion batteries.

关键词： Sodium ion battery Oxide cathode Phase engineering Phase diagram Na~+kinetic

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Surface structural transformation of Ni2P@C electrocatalysts for overall alkaline water splitting

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Progress in Natural Science:materials International 2024年第1期34卷 102-107页

作者： Kun Yang Xinjuan Liu Jun Xu Yun Gong Shuling Shen Jinchen Fan Xiaojie Zhang Yuhua Xue School of materials and chemistry University of Shanghai for Science and Technology National&Local Joint Engineering research center for Mineral Salt Deep Utilization Huaiyin Institute of Technology

Understanding the surface restructuring, including atomic rearrangement and chemical composition adjustments,is urgent to accelerate electrocatalytic reactions. Herein, we focus on the surface restructuring and active species for phosphide especially Ni2P during the water splitting process by combination of in-situ Raman and ex-situ X-ray photoelectron spectroscopy. Results confirm that NiOOH and NiOO* are formed during OER, while Niδ+-Hadactive sites are formed during HER. In situ-formed NiOOH/Ni2P@C and Niδ+/Ni2P@C show enhanced water splitting（1.514 V at 10 mA/cm2） and NO3RR(86% and 668 μmol h-1cm-2for NH3Faraday efficiency and yield)activities. In-depth investigation of the surface dynamic changes can provide guidance for establishing the relation of structure-electrocatalytic activity.

关键词： Dynamic surface restructuring Phase structural transition In-situ Raman spectra Ni_2P@C Overall water splitting

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Superwetting Ag/α-Fe_(2)O_(3) anchored mesh with enhanced photocatalytic and antibacterial activities for efficient water purification

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Green Energy & Environment 2024年第1期9卷 89-103页

作者： Jiakai Li Changpeng Lv Jiajia Song Xiaoling Zhang Xizhen Huang Yingzhuo Ma Haijie Cao Na Liu department of chemistry Tsinghua UniversityBeijing100084China Anhui Provincial Engineering Laboratory of Silicon-based materials Engineering Technology Research Center of Silicon-based Materials(Anhui)School of Material and Chemical EngineeringBengbu UniversityBengbu233030China Institute of materials for Energy and Environment College of Materials Science and EngineeringQingdao UniversityQingdao266071China

Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water ***,it is still a challenge to fabricate multifunctional and environmentally friendly materials,which can be stably applied to purify the actual complicated ***,a Ag/Ag/α-Fe_(2)O_(3) heterostructure anchored copper mesh was intentionally synthesized using a facile two-step hydrothermal *** resultant mesh with superhydrophilicity and underwater superoleophobicity was capable of separating various oil/water mixtures with superior separation efﬁciency and high permeationﬂux driven by ***ﬁting from the joint effects of the smaller band gap of Ag/α-Fe_(2)O_(3) heterojunction,inherent antibacterial capacity of Ag/α-Fe_(2)O_(3) and Ag nanoparticles,favorable conductive substrate,as well as the hierarchical structure with superwettability,such mesh presented remarkably enhanced degradation capability toward organic dyes under visible light irradiation and antibacterial activity against both Escherichia coli(***)and Staphylococcus aureus(***)compared with the pure Ag/α-Fe_(2)O_(3) coated ***,the mesh exhibited bifunctional water puriﬁcation performance,in which organic dyes were eliminated simultaneously from water during oil/water separation in oneﬁltration *** importantly,this mesh behaved exceptional chemical resistance,mechanical stability and long-term ***,this material with multifunctional integration may hold promising potential for steady water puriﬁcation in practice.

关键词： Superwetting Ag/α-Fe_(2)O_(3)heterostructure Enhanced photocatalytic and antibacterial activities Water purification Long-term reusability

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Interfacial engineering of the layered oxide cathode materials for sodium-ion battery

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Nano research 2024年第3期17卷 1441-1464页

作者： Quanqing Zhao Ruru Wang Ming Gao Faheem KButt Jianfeng Jia Haishun Wu Youqi Zhu Key Laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China Metals and chemistry research Institute China Academy of Railway Sciences Corporation LimitedBeijing 100081China department of Physics Division of Science and TechnologyUniversity of EducationLahore 54770Pakistan research center of materials Science Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green ApplicationsBeijing Institute of TechnologyBeijing 100081China

The layered metal oxides are reviewed as the hopeful cathode materials for high-performance sodium-ion batteries(SIBs)due to their large theoretical capacity,favorable two-dimensional(2D)ion diffusion channel,and simple ***,their cycling stability,rate capability,and thermal stability are still significantly concerned and highlighted before further practical *** chemical,mechanical and electrochemical stability of the cathode–electrolyte interfaces upon cycling is of great ***,the unique structural and electrochemical properties of the layered oxide cathode materials for SIB are *** mechanism of bulk/surface degradation induced by oxygen evolution,phase transition,microcrack,and electrolyte decomposition is thoroughly ***,the interfacial engineering to construct stable interface through various effective methods is fully *** future outlook and challenges for interfacial engineering in this filed are also *** review should shed light on the rational design and construct of robust interface for applications of superior layered oxide cathodes in SIB and may suggest future research directions.

关键词： interfacial engineering sodium-ion battery layered oxide electrolyte interface

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Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo5}motifs for enhanced proton conductivity

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Nano research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China Hebei Key Laboratory of Organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China State Key Laboratory of Supramolecular Structure and materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction

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Photoredox catalytic alkylarylation of alkynes with arylsulfonylacetate as bifunctional reagent

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Science China chemistry 2024年第6期67卷 2022-2028页

作者： Chonglong He Min Wang Yulong Wang Lirong Zhao Youkang Zhou Keyuan Zhang Shenyu Shen Yaqiong Su Xin-Hua Duan Le Liu School of chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an710049China

Difunctionalization of alkynes represents a powerful and straightforward approach to the synthesis of complex ***,the radical difunctionalization of alkynes mediated by bifunctional reagents remains challenging and underexplored,despite significant progress having been made in alkene ***,we report a novel arylsulfonylacetate skeleton in which aryl rings are attached to acetates through SO_(2),serving as a powerful bifunctional reagent for the alkylarylation of alkynes via vinyl-radical intermediate under photoredox *** modular bifunctional reagent enables the simultaneous incorporation of a wide range of functional groups,including(hetero)aryl ring and alkyl carboxylate into alkynes,resulting in synthetically valuable all-carbon tetrasubstituted alkene *** transformation is distinguished by its redox-neutral nature,readily accessible starting materials,compatibility with diverse functional groups and its capacity to facilitate convergent *** utility of this approach was further demonstrated by the late-stage functionalization of complex molecules and the preparation of fluorescent molecules and anti-cancer drugs.

关键词： bifunctional reagent photoredox catalysis Smiles rearrangement alkylarylation tetrasubstituted acyclic all-carbon olefins

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Coupling interface constructions of hollow Co-Mo mixed multiple oxidation states heterostructure for high-performance aprotic Li-O_(2) battery

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Nano research 2024年第5期17卷 4100-4107页

作者： Xingzi Zheng Mengwei Yuan Jingshen Xu Zihan Li Caiyun Nan Genban Sun Beijing Key Laboratory of Energy Conversion and Storage materials College of ChemistryBeijing Normal UniversityBeijing 100875China center for Advanced materials research Beijing Normal UniversityZhuhai 519087China

Constructing interfaces in heterostructures is effective for modulating the electronic properties of *** hollow CoMoO_(4)-Co_(3)O_(4) heterostructure(HCMCH)was prepared as a bifunctional electrocatalyst for Li-O_(2) *** different components in CoMoO_(4)-Co_(3)O_(4) heterostructure presented the efficient coupling and enhanced the electrocatalytic activity for aprotic oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),in which it improved the obviously reduced overpotential of 300 mV(compared with the pure Ketjen black(KB)electrode),enhanced reversibility of 80%capacity retention after 6 full cycles and the superior cyclability of more than 200 cycles with an optimized *** battery performance of the HCMCH was not only associated with the unique hollow structure and rich active sites but also with coupling interface constructions synergetic effects attaching to the improving conductivity and optimized the discharge *** results suggested that this HCMCH electrocatalyst was a promising candidate for the Li-O_(2) battery and it gave a novel insight for high performance electrocatalyst designing.

关键词： Li-oxygen battery heterostructure electrocatalyst coupling interface

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Ni-Catalyzed Enantioselective Difunctionalization of Alkynes to Azepine Derivatives Bearing a Quaternary center and an Unprotected Imine

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Chinese Journal of chemistry 2024年第8期42卷 873-878页

作者： Jian Long Zhiwu Lu Xiao-Lin Li Peng Xue Wen-Bo Liu Engineering research center of Organosilicon Compounds&materials(Ministry of Education)and College of chemistry and Molecular Sciences Wuhan UniversityWuhanHubei430072 China

Comprehensive Summary,The azepine ring is a prominent structural scaffold in biologically significant molecules. In this study, we present a Ni(II)-catalyzed asymmetric difunctionalization of alkynes, involving intermolecular regioselective arylation and intramolecular nitrile addition, enabling the synthesis of enantioenriched azepine derivatives. This reaction simultaneously installs an all-carbon quaternary stereocenter and introduces an unprotected imine functionality, showing great promise for subsequent transformations. The reaction exhibits good tolerance toward various functional groups, resulting in high yields and enantioselectivities. The synthetic utility of this methodology is further demonstrated through gram-scale synthesis and product derivatization. This research offers an efficient approach to the synthesis of seven-membered nitrogen heterocycles.

关键词： Nickel Asymmetric catalysis N-Heterocycles Alkyne functionalization Quaternary centers

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Bridging molecular photosensitizer and catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction

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Journal of Environmental Sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong Anhui Engineering research center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China School of chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246011China School of chemistry and materials Science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and ***,their low durability and recyclability limit practical *** this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous *** characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular ***,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly *** work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts.

关键词： durability selectivity catalyst

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Weak interaction-steered evolution of polyoxovanadate-based metal-organic polyhedra from transformation via interlock to packing

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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

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