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Nano-Micro Letters 2024年第12期16卷 42-58页

作者： Yongji Xia Le Wang Guiyang Gao Tianle Mao Zhenjia Wang Xuefeng Jin Zheyu Hong Jiajia Han Dong-Liang Peng Guanghui Yue state key Lab of physical chemistry of solid surface Fujian Key Laboratory of Surface and Interface Engineering for High Performance MaterialsCollege of MaterialsXiamen UniversityXiamen 361005People’s Republic of China

Lithium-oxygen batteries(LOBs)with high energy density are a promising advanced energy storage ***,the slow cathodic redox kinetics during cycling causes the discharge products to fail to decompose in time,resulting in large polarization and battery failure in a short ***,a self-supporting interconnected nanosheet array network NiCo_(2)O_(4)/MnO_(2)with a Mott-Schottky heterostructure on titanium paper(TP-NCO/MO)is ingeniously designed as an efficient cathode catalyst material for *** heterostructure can accelerate electron transfer and influence the charge transfer process during adsorption of intermediate by triggering the interface disturbance at the heterogeneous interface,thus accelerating oxygen reduction and oxygen evolution kinetics and regulating product decomposition,which is expected to solve the above *** meticulously designed unique structural advantages enable the TP-NCO/MO cathode catalyst to exhibit an astounding ultra-long cycle life of 800 cycles and an extraordinarily low overpotential of 0.73 *** study utilizes a simple method to cleverly regulate the morphology of the discharge products by constructing a Mott-Schottky heterostructure,providing important reference for the design of efficient catalysts aimed at optimizing the adsorption of reaction intermediates.

关键词： Mott-Schottky heterostructure Lithium-oxygen batteries Electrocatalysts Electrodeposition

Li_(2)ZnTi_(3)O_(8)as the host–separator modifier with efficient polysulfides trapping and fast Li^(+)diffusion for lithium-sulfur batteries

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Nano Research 2024年第7期17卷 6087-6094页

作者： Mao Qian Yakun Tang Lang Liu Yue Zhang Xiaohui Li JiaJia Chen state key laboratory of chemistry and Utilization of Carbon Based Energy Resources Xinjiang UniversityUrumqi 830017China state key laboratory of physical chemistry of solid surfaces Xiamen UniversityXiamen 361005China

The diffusion and loss of lithium polysulfides(LiPSs)in lithium-sulfur batteries(LSBs)reduce the sulfur utilization rate and the catalytic conversion efficiency of sulfur species,resulting in early battery ***_(2)ZnTi_(3)O_(8)(LZTO),characterized by its stable spinel structure,exhibits high Li+conductivity and holds great potential as an effective adsorbent for *** study proposes a collaborative design concept of LZTO host–separator modifier,which offers a complementary and matching approach in the cathode side,effectively addressing the challenges associated with dissolution and inadequate conversion of *** functional theory(DFT)calculation substantiates the pronounced chemical affinity of LZTO towards *** importantly,the high efficiency ion transport channels are achieved in separator coating due to the presence of the LZTO ***,the catalytic efficacy of LZTO is validated through meticulous analysis of symmetric batteries and Tafel ***,the LZTO host–separator modifier-based cell displays satisfactory rate capability(1449 and 1166 mAh·g^(−1)at 0.1 and 0.5 C)and an impressively capacity(606 mAh·g^(−1)after 500 cycles at 1 C).The coordinated strategy of host–separator modifier is supposed to have wide applications in LSBs.

关键词： Li_(2)ZnTi_(3)O_(8) lithium-sulfur batteries host-separator modifier catalytic conversion diffusion and loss of LiPSs

Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

Quantitative lithium substitution of carboxyl hydrogens in polyacrylic acid binder enables robust SiO electrodes with durable lithium storage stability

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Journal of Energy chemistry 2024年第10期97卷 352-360页

作者： Weihua Wang Wenyi Li Siyi Jing Huiping Yang Huiqun Wang Ling Huang Yuxiang Mao Xikun Pang Yudai Huang Li Zhang state key laboratory of physical chemistry of solid surfaces Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy Materials (iChEM) Xiamen University state key laboratory of chemistry and Utilization of Carbon-Based Energy Resources College of Chemistry Xinjiang University

The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide（SiO） *** the classic polyacrylic acid（PAA） binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO ***,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant ***,a modified PAA-Lix（0.25 ≤x≤1） binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with *** appropriate lithium substitution（x=0.25） not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Lixmolecular chains through the ion-dipole *** such,the PAA-Li0.25/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g-1after 100cycles at 0.1 C) and rate performance(1000.6 mA h g-1at 1 C),significantly outperforming the electrode using pristine PAA *** work paves the way for quantitative regulation of binders at the molecular level.

关键词： Adhesion strength Charge repulsion effect Polyacrylic acid binder Quantitative lithium substitution SiO anode

Healing the structural defects of spinel MnFe2O4 to enhance the electrocatalytic activity for oxygen reduction reaction

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Journal of Energy chemistry 2024年第10期97卷 12-19页

作者： Manting Tang Yue Zou Zhiyong Jiang Peiyu Ma Zhiyou Zhou Xiaodi Zhu Jun Bao Shi-Gang Sun National Synchrotron Radiation laboratory University of Science and Technology of China state key laboratory of physical chemistry of solid surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University iChEM (Collaborative Innovation Center of chemistry for Energy Materials) University of Science and Technology of China

Spinel metal oxides containing Mn,Co,or Fe（AB2O4,A/B=Mn/Fe/Co） are one of the most promising nonPt electrocatalysts for oxygen reduction reaction（ORR） in alkaline ***,the low conductivity of metal oxides and the poor intrinsic activities of transition metal sites lead to unsatisfactory ORR *** this study,eutectic molten salt（EMS） treatment is employed to reconstruct the atomic arrangement of MnFe2O4electrocatalyst as a prototype for enhancing ORR *** analyses by using XAFS,soft XAS,XPS,and electrochemical methods reveal that the EMS treatment reduces the oxygen vacancies and spinel inverse in MnFe2O4effectively,which improves the electric conductivity and increases the population of more catalytically active Mn2+sites with tetrahedral ***,the enhanced Mn-O interaction after EMS treatment is conducive to the adsorption and activation of O2,which promotes the first electron transfer step（generally considered as the ratedetermining step） of the ORR *** a result,the EMS treated MnFe2O4catalyst delivers a positive shift of 40 mV in the ORR half-wave potential and a two-fold enhanced mass/specific *** work provides a convenient approach to manipulate the atomic architecture and local electronic structure of spinel oxides as ORR electrocatalysts and a comprehensive understanding of the structureperformance relationship from the molecular/atomic scale.

关键词： Eutectic molten salt Oxygen reduction reaction Oxygen vacancies Spinel inverse Spinel MnFe2O4

Switching on/off phosphorescent or non-radiative channels by aggregation-induced quantum interference

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Aggregate

Aggregate 2024年第1期5卷 175-184页

作者： Yi Kong Yu-Chen Wang Xunkun Huang WanZhen Liang Yi Zhao department of chemistry State Key Laboratory of Physical Chemistry of Solid SurfacesiChEMFujian Provincial Key Laboratory of Theoretical and Computational Chemistryand College of Chemistry and Chemical EngineeringXiamen UniversityXiamenPeople’s Republic of China

Pure organic materials with persistent and efficient room-temperature phosphorescence have recently aroused great research interest due to their vast potential in *** crucial design principle for such materials is to suppress as much as possible the non-radiative decay of the triplet exciton while maintaining a moderate phosphorescent radiative ***,molecular engineering often exhibits similar regulation trends for the two ***,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay *** systematically analyze various constructive and destructive transition pathways in aggregates with different molecular packing types and establish clear relationships between the luminescence characters and the signs of the singlet and triplet excitonic *** is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic *** importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion *** work lays the theoretical foundation for future experimental realization of quantum interference effects in phosphorescence.

关键词： excitonic coupling intersystem crossing organic aggregates organic room temperature phosphorescence quantum interference

Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of chemistry for Energy Materials state key laboratory of physical chemistry of solid surfaces and department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

High-rate lithium-ion battery performance of a ternary sea urchin-shaped CoNiO_(2)@NiP_(6)Mo_(18)/CNTs composites

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Journal of Energy chemistry 2024年第9期96卷 516-525页

作者： Li-ping Cui Shuang Sun Kai Yu Shu Zhang Mei-lin Wang Jia-jia Chen Bai-bin Zhou key laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina state key laboratory of physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005FujianChina

Bimetallic oxides are attractive anode materials for lithium-ion batteries(LIBs)due to their large theoretical ***,the low conductivity,short cycle life,and poor rate capability are the bottlenecks for their further *** overcome above issues,the basket-like polymolybdate(NiP_(6)Mo_(18))and carbon nanotubes(CNTs)were uniformly embedded on the urchin-shaped CoNiO_(2)nanospheres to yield a ternary composites CoNiO_(2)@NiP_(6)Mo_(18)/CNTs via electrostatic *** multi-level morphology of urchin spinules accelerates the diffusion rate of Li^(+);CNT improves the conductivity and enhances cycle stability of the material;and heteropoly acid contributes more redox activity ***,CoNiO_(2)@NiP_(6)Mo_(18)/CNTs as an anode of LIBs exhibits a high initial capacity(1396.7 mA h g^(−1)at 0.1 A g^(−1)),long-term cycling stability(750.2 mA h g^(−1)after 300 cycles),and rate performance(450.3 mA h g^(−1)at 2 A g^(−1)),which are superior to reported metallic oxides anode of *** density functional theory(DFT)and kinetic mechanism suggest that CoNiO_(2)@NiP_(6)Mo_(18)/CNTs delivers an outstanding pseudocapacitance and rapid Li^(+)diffusion behaviors,which is due to the rich surface area of the urchin-like CoNiO_(2)with the uniform embeddedness of NiP_(6)Mo_(18)and *** study provides a new idea for optimizing the performance of bimetallic oxides and developing high-rate lithium-ion battery composites.

关键词： Bi-metal oxides Transition metal oxides Polyoxometalates Nanocomposite LIBs

Parallelogram 3d-4f-5d heterometallic clusters based on trilacunary tungstoantimonates with excellent proton conductivity

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Chinese Chemical Letters 2024年第3期35卷 528-531页

作者： Haiying Wang Han Xu Chaolong Chen Yingjie Zhu Yikang Zhang Dongdi Zhang Jingyang Niu Henan key laboratory of Polyoxometalate chemistry College of Chemistry and Molecular SciencesHenan UniversityKaifeng 475004China School of Pharmaceutical Science&Yunnan key laboratory of Pharmacology for Natural Products Kunming Medical UniversityKunming 650500China Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Two 3d-4f-5d heterometallic cluster-containing polyoxometalates,formulated as Na_(22){(SbW_(9)O_(33))_(4)[La_(3)W_(6)MO_(18)(H_(2)O)_(8)(CH_(3)COO)_(4)]_(2)}·nH_(2)O(abbreviated as La_(6)M_(2),M=Co/Mn)were synthesized and structurally ***-crystal X-ray diffraction analyses reveal that the polyanions of La_(6)Co_(2)and La_(6)Mn_(2)consist of the uncommon 3d-4f-5d clusters{La_(6)W_(12)Co_(2)}and{La_(6)W_(12)Mn_(2)},which are encapsulated by four trilacunary Keggin tungstoantimonates to form the parallelogram-shaped title ***,the polyanions can be extended into a two-dimensional(2D)frame by the linkage of peripheral Na+*** inner space of the 2D layer was filled with water molecules and thus an H-bonded network was formed,which is expected to exhibit a fascinating proton *** study of water-assisted proton conduction demonstrated that La_(6)Co_(2)and La_(6)Mn_(2)were temperature-and humiditydependent proton conductors,respectively,and the proton conductivities could reach 1.3×10^(-2)and 2.3×10^(-2)S/cm at 65℃and 90%RH conditions.

关键词： Polyoxometalate Parallelogram Heterometallic 3d-4f-5d cluster Proton conductivity

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao You Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun Zheng Nanfeng Zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China department of chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden department of chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation