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In situ tracking of the lithiation and sodiation process of disodium terephthalate as anodes for rechargeable batteries by Raman spectroscopy

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Nano Research 2024年第1期17卷 245-252页

作者： Xiu-Mei Lin Chong Han Xin-Tao Yang Jia-Sheng Lin Wei-Qiang Yang Hong-Xu Guo Yao-Hui Wang Jin-Chao Dong Jian-Feng Li Department of Chemistry and Environment Science Fujian Province University Key Laboratory of Analytical ScienceMinnan Normal UniversityZhangzhou 363000China College of Energy College of Chemistry and Chemical EngineeringCollege of MaterialsState Key Laboratory of Physical Chemistry of Solid SurfacesiChEMXiamen UniversityXiamen 361005China Institute of Optical and Electronic Technology China Jiliang UniversityHangzhou 310018China

Organic compounds represent an appealing group of electrode materials for rechargeable batteries due to their merits of biomass,sustainability,environmental friendliness,and processability.Disodium terephthalate(Na_(2)C_(8)H_(4)O_(4),Na_(2)TP),an organic salt with a theoretical capacity of 255 mAh·g^(-1),is electroactive towards both lithium and sodium.However,its electrochemical energy storage(EES)process has not been directly observed via in situ characterization techniques and the underlying mechanisms are still under debate.Herein,in situ Raman spectroscopy was employed to track the de/lithiation and de/sodiation processes of Na2TP.The appearance and then disappearance of the–COOLi Raman band at 1625 cm^(-1) during the de/lithiation,and the increase and then decrease of the–COONa Raman band at 1615 cm^(-1) during the de/sodiation processes of Na2TP elucidate the one-step with the 2Li+or 2Na+transfer mechanism.We also found that the inferior cycling stability of Na2TP as an anode for sodium-ion batteries(SIBs)than lithium-ion batteries(LIBs)could be due to the larger ion radium of Na+than Li+,which results in larger steric resistance and polarization during EES.The Na2TP,therefore,shows greater changes in spectra during de/sodiation than de/lithiation.We expect that our findings could provide a reference for the rational design of organic compounds for EES.

关键词： disodium terephthalate(Na_(2)C_(8)H_(4)O_(4) Na2TP) in situ Raman spectroscopy de/lithiation de/sodiation mechanisms

Composite laminar membranes for electricity generation from water evaporation

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Nano Research 2024年第1期17卷 307-311页

作者： Xiao Wang Gang Yuan Han Zhou Yu Jiang Shuo Wang Jiaojiao Ma Chongyang Yang Sheng Hu State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China

Harvesting clean energy from water evaporation has been extensively investigated due to its sustainability.To achieve high efficiency,energy conversion materials should contain multiple features which are difficult to be simultaneously obtained from single-component materials.Here we use composite laminar membranes assembled by nanosheets of graphene oxide and mica,and find a sustained power density induced by water evaporation that is two orders of magnitude larger than that from membranes made by either of the components.The power output is attributed to selective proton transport driven by water evaporation through the interlayer nanochannels in the membranes.This process relies on the synergistic effects from negatively charged and hydrophilic mica surfaces that are important for proton selectivity and water transport,and the tunable electrical conductivity of graphene oxide that provides optimized internal resistance.The demonstrated composite membranes offer a strategy of enhancing power generation by combining the advantages from each of their components.

关键词： graphene oxide mica water evaporation electrical double layer surface charge ion selectivity

Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction

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Journal of Energy Chemistry 2024年第1期88卷 194-201,I0005页

作者： Saihang Zhang Senchuan Huang Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou National Engineering Research Center of Light Alloy Net Forming&State Key Laboratory of Metal Matrix Composites Center of Hydrogen ScienceSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersCollege of Chemistry and MaterialsFudan UniversityShanghai 200433China

High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.

关键词： Oxygen evolution reaction Nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis Electrocatalysts

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纳米氧化铜片用于高效电化学还原一氧化氮

Science China Materials 2024年第6期67卷 1876-1881页

作者：邵加奇魏鹏飞王硕宋延鹏付云凡李荣坦张小敏汪国雄包信和 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 116023China University of Chinese Academy of Sciences Beijing 100049China

一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生... 详细信息

一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生产速率分别达到1.1 A cm^(-2)和7356μmol cm^(-2)h^(-1).在电流密度超过400 m A cm-2时,氨法拉第效率在50小时保持在80%以上.准原位X射线光电子能谱和原位X射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被电化学还原成单质铜.与铜纳米颗粒相比,氧化铜纳米片展现出较高的电化学表面积和一氧化氮电还原的内在活性.

关键词： electrocatalytic NORR ammonia synthesis electro-catalysis CuO nanosheets

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 applications.One 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 rate.However,molecular engineering often exhibits similar regulation trends for the two processes.Here,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay channels.We 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 couplings.It is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic couplings.Most importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion symmetry.This 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

Catalytic conversion of mixed polyolefins under mild atmospheric pressure

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The Innovation 2024年第2期5卷 98-106页

作者： Binzhi Zhao Hui Tan Jie Yang Xiaohui Zhang Zidi Yu Hanli Sun Jialiang Wei Xinyi Zhao Yufeng Zhang Lili Chen Dali Yang Jin Deng Yao Fu Zheng Huang Ning Jiao State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China The Institute for Advanced Studies Wuhan UniversityWuhan 430072China Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Urban Pollutant ConversionAnhui Province Key Laboratory of Biomass Clean EnergyiChEMUniversity of Science and Technology of ChinaHefei 230026China State Key Laboratory of Organometallic Chemistry Chinese Academy of SciencesShanghai 200032China

The chemical recycling of polyolefin presents a considerable challenge,especially as upcycling methods struggle with the reality that plastic wastes typically consist of mixtures of polyethylene(PE),polystyrene(PS),and polypropylene(PP).We report a catalytic aerobic oxidative approach for polyolefins upcycling with the corresponding carboxylic acids as the product.This method encompasses three key innovations.First,it operates under atmospheric pressure and mild conditions,using O_(2) or air as the oxidant.Second,it is compatible with high-density polyethylene,low-density polyethylene,PS,PP,and their blends.Third,it uses an economical and recoverable metal catalyst.It has been demonstrated that this approach can efficiently degrade mixed wastes of plastic bags,bottles,masks,and foam boxes.

关键词： mixed Catalytic oxidative

超低密度的单原子钴位点高效去除抗生素（英文）

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Science China Materials 2024年

作者：葛骁王杰周冬琴王小治吴宇恩 College of Environmental Science and Engineering Yangzhou University Department of Chemistry Hefei National Laboratory for Physical Sciences at the Microscale iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) University of Science and Technology of China

单原子位点催化剂(SSCs)由于能够产生丰富的活性物质来清除类芬顿体系中的污染物,而显示出广阔的潜力.然而,在高级氧化工艺中,实现金属原子100%的利用率和减少金属浸出以满足环境安全标准是困难的.在此基础上,利用强极化力获得了Co原子...

单原子位点催化剂(SSCs)由于能够产生丰富的活性物质来清除类芬顿体系中的污染物,而显示出广阔的潜力.然而,在高级氧化工艺中,实现金属原子100%的利用率和减少金属浸出以满足环境安全标准是困难的.在此基础上,利用强极化力获得了Co原子含量极低(～0.17%)的催化剂,提高了金属原子利用率,降低了抗生素消除过程中金属浸出的风险.正如预期,该催化剂具有有限的Co位点,伴随着丰富的缺陷和大量从大孔到中孔再到微孔分布的骨架,实现了快速的四环素降解(0.07133 min-1)和优异的归一化速率常数(kper-site,2.4726×105min-1M-1).实验和理论结果均表明,充分暴露具有丰富C-N缺陷的Co位点,可以提高Co活性位点的电子密度,降低过硫酸盐(PDS)的吸附能,从而优化Co原子对PDS活化的利用.该研究为设计高性能、环境友好的水修复用SSCs提供了有价值的见解.

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Exploring the Cation Regulation Mechanism for Interfacial Water Involved in the Hydrogen Evolution Reaction by In Situ Raman Spectroscopy

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Nano-Micro Letters 2024年第3期16卷 303-312页

作者： Xueqiu You Dongao Zhang Xia‑Guang Zhang Xiangyu Li Jing‑Hua Tian Yao‑Hui Wang Jian‑Feng Li School of Ocean Information Engineering Fujian Provincial Key Laboratory of Oceanic Information Perception and Intelligent ProcessingJimei UniversityXiamen 361021People’s Republic of China State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis and InstrumentationiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyXiamen UniversityXiamen 361005People’s Republic of China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsCollege of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007People’s Republic of China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005People’s Republic of China

Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.Unfortunately,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial environment.Here,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation techniques.Direct spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively direction.When comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+

关键词： In situ Raman Interfacial water Hydrogen evolution reaction Cations

Core-shell nanoparticle enhanced Raman spectroscopy in situ probing the composition and evolution of interfacial species on PtCo surfaces

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Nano Research 2024年第6期17卷 4687-4692页

作者： Jing Liu Han-Liang Zhong Xiangyu Li Mu-Fei Yue Wei-Min Yang Xueqiu You Jing-Hua Tian Yao-Hui Wang Jian-Feng Li Fujian Provincial Key Laboratory of Oceanic Information Perception and Intelligent Processing School of Ocean Information EngineeringJimei UniversityXiamen 361021China College of Chemistry Fuzhou UniversityFuzhou 350108China State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis and InstrumentationiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Shenzhen Research Institute of Xiamen University Shenzhen 518000China

The composition and evolution of interfacial species play a key role during electrocatalytic process.Unveiling the structural evolution and intermediate during catalytic process by in situ characterization can shed new light on the electrocatalytic reaction mechanism and develop highly efficient catalyst.However,directly probing the interfacial species is extremely difficult for most spectroscopic techniques due to complicated interfacial environment and ultra-low surface concentration.Herein,electrochemical core-shell nanoparticle enhanced Raman spectroscopy is utilized to probe the composition and evolution processes of interfacial species on Au@Pt,Au@Co,and Au@PtCo core-shell nanoparticle surfaces.The spectral evidences of interfacial intermediates including hydroxide radical(OH*),superoxide ion(O_(2)^(−)),as well as metal oxide species are directly captured by in situ Raman spectroscopy,which are further confirmed by the both isotopic experiment and density functional theory calculation.These results provide a mechanistic guideline for the rational design of highly efficient electrocatalysts.

关键词： in situ Raman core-shell nanoparticle PtCo interfacial species composition and evolution