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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

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in situ raman spectroscopy reveals the mechanism of titanium substitution in P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2): Cathode materials for sodium batteries

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Journal of Energy Chemistry 2021年第2期30卷 323-328,I0011页

作者： Xiao-Bin Zhong Chao He Fan Gao Zhong-Qun Tian Jian-Feng Li School of Mechanical and Power Engineering North University of ChinaTaiyuan 030051ShanxiChina State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Layered P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 is a promising cathode material. It exhibits a high capacity and suitable operating voltage and undergoes a phase transition from P2 to O2 during charge/discharge.Researchers have used Ti substitution to improve the cathode, yet the chemical principles that underpin elemental substitution and functional improvement remain unclear. To clarify these principles, we used in situ raman spectroscopy to monitor chemical changes in P2–Na2/3 Ni1/3 Mn1/3 Ti1/3 O2 and P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 during charge/discharge. Based on the change in the A_(1g) and E_g peaks during charge/discharge, we concluded that Ti substitution compressed the transition metal layer and expanded the planar oxygen layer in the unit cell. Titanium stabilized the P2 phase structure, which improved the cycling stability of P2–NaNMT. Our results provide clear theoretical support for future research on modifying electrodes by elemental substitution.

关键词： in situ raman spectroscopy P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2) Titanium substitution

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Electrokinetic-mechanism of water and furfural oxidation on pulsed laser-interlaced Cu_(2)O and CoO on nickel foam

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Journal of Energy Chemistry 2024年第4期91卷 145-154页

作者： Yewon Oh Jayaraman Theerthagiri M.L.Aruna Kumari Ahreum Min Cheol Joo Moon Myong Yong Choi Department of Chemistry(BK21 FOUR) Research Institute of Natural SciencesGyeongsang National UniversityJinju 52828Republic of Korea Department of Chemistry The Oxford College of ScienceBengaluruKarnataka 560102India Core-Facility Center for Photochemistry&Nanomaterials Gyeongsang National UniversityJinju 52828Republic of Korea

The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.

关键词： Pulsed laser irradiation in liquids Water and furfural oxidation in situ raman spectroscopy CoO/NiO/nickel foam Cu_(2)O/Nio/nickel foam 2-furoic acid

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Synergetic Contributions from the Components of Flexible 3D Structured C/Ag/ZnO/CC Anode Materials for Lithium-Ion Batteries

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Energy & Environmental Materials 2023年第6期6卷 227-235页

作者： Huang Xiao Shuangpeng Li Jiaying Zhou Chenyu Zhao Yi Yuan Xiaohong Xia Yuwen Bao Manon Lourenço Kevin Homewood Yun Gao Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and MinistrySchool of Materials Science&EngineeringHubei UniversityWuhan 430062China

Low electronic conductivity and large volume changes during the(de)lithiation process are the two main challenges for ZnO anode materials used for lithium-ion batteries(LIB).Here,a free-standing,flexible,and binder-free LIB electrode composed of ZnO nanorods and carbon cloth(CC)is fabricated.This is then decorated with Ag nanoparticles and finally coated by an amorphous carbon layer to form the hybrid electrode:(C@(Ag&ZnO)).The voids among the nanorods are sufficient to accommodate the volume expansion of the ZnO while the flexible CC,which acts as the current collector,relieves the volume change-induced stress.The Ag nanoparticles are effective in improving the conductivity.This composite electrode shows excellent LIB performance with a stable long cycling life over 500 cycles with a reversible capacity of 1093 mAh g^(-1)at a current density of 200 mA g^(-1).It also shows good rate performance with reversible capacity of 517 mAh g^(-1)under a high-current density of 5000 mA g^(-1).in situ raman spectroscopy is conducted to investigate the contributions of the amorphous carbon layer to the capacity of the whole electrode and the synergy between the CC and ZnO nanorods.

关键词： binder-free in situ raman spectroscopy lithium-ion batteries ZnO nanorods

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Electronic and Nano-structural Modulation of Co(OH)_(2) Nanosheets by Fe-Benzenedicarboxylate for Efficient Oxygen Evolution

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Chemical Research in Chinese Universities 2023年第2期39卷 219-223页

作者： XIAO Long WU Huirong ZHANG Yong SUN Hao ZHANG Wenchao LYU Fenglei DENG Zhao PENG Yang Soochow Institute for Energy and Material Innovations College of EnergySoochow UniversitySuzhou215006P.R.China School of Chemistry and Life Science Suzhou University of Science and TechnologySuzhou215009P.R.China

Oxygen evolution reaction(OER)plays a key role in the electrochemical conversion and storage processes,but the sluggish kinetics of OER strongly impedes its large-scale applications.We herein reported the in situ growth of Fe-benzenedicarboxylate(Fe-BDC)on Co(OH)_(2) nanoplates[Fe-BDC/Co(OH)_(2)]that showed remarkably enhanced OER activity than the pristine Co(OH)_(2).The incorporation of Fe species could enhance the intrinsic OER activity of Co and BDC could increase the electrochemically active surface area(ECSA),thus resulting in dramatically enhanced OER activity.in situ raman spectroscopy characterization disclosed that Fe-CoOOH reconstructed from Fe-BDC/Co(OH)_(2) was the real active site for OER.This work highlights the significance of rational tailoring of the nanostructure and electronic structure of Co(OH)_(2) and provides more opportunities for its widespread applications.

关键词： Co(OH)_(2)nanoplate Oxygen evolution reaction Electronic structure Nanostructure in situ raman spectroscopy

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In situ study of calcite-Ⅲ dimorphism using dynamic diamond anvil cell

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Chinese Physics B 2022年第9期31卷 421-427页

作者：赵霞梅升华郑直高悦陈姜智刘月高孙建国李艳孙建辉 CAS Key Laboratory for Experimental Study under Deep-sea Extreme Conditions Institute of Deep-sea Science and EngineeringChinese Academy of Sciences(CAS)Sanya 572000China University of Chinese Academy of Sciences Beijing 100049China Department of Mechanical Engineering National University of Singapore(NUS)Singapore 117575Singapore

The phase transitions among the high-pressure polymorphic forms of CaCO_(3)(cc-Ⅰ,cc-Ⅱ,cc-Ⅲ,and cc-Ⅲb)are investigated by dynamic diamond anvil cell(dDAC)and in situ raman spectroscopy.Experiments are carried out at room temperature and high pressures up to 12.8 GPa with the pressurizing rate varying from 0.006 GPa/s to 0.056 GPa/s.In situ observation shows that with the increase of pressure,calcite transforms from cc-Ⅰto cc-Ⅱat~1.5 GPa and from cc-Ⅱto cc-Ⅲat~2.5 GPa,and transitions are independent of the pressurizing rate.Further,as the pressure continues to increase,the cc-Ⅲb begins to appear and coexists with cc-Ⅲwithin a pressure range that is inversely proportional to the pressurizing rate.At the pressurizing rates of 0.006,0.012,0.021,and 0.056 GPa/s,the coexistence pressure ranges of cc-Ⅲand cc-Ⅲb are 2.8 GPa-9.8 GPa,3.1 GPa-6.9 GPa,2.7 GPa-6.0 GPa,and 2.8 GPa-4.5 GPa,respectively.The dependence of the coexistence on the pressurizing rate may result from the influence of pressurizing rate on the activation process of transition by reducing the energy barrier.The higher the pressurizing rate,the lower the energy barrier is,and the easier it is to pull the system out of the coexistence state.The results of this in situ study provide new insights into the understanding of the phase transition of calcite.

关键词： calcite-Ⅲ dimorphism dynamic diamond anvil cell in situ raman spectroscopy pressurizing rate

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Anodic and cathodic process of hypophosphite on a Ni-Ag electrode

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Chinese Journal of Chemistry 2000年第5期18卷 703-709页

作者：曾跃于尚慈李则林周绍民 Department of Chemistry Hunan Normal University ChangshaHunan 410006 China State Key Laboratory for Physical Chemistry of the Solid Surface Department of ChemistryXiamen UniversityXiamenFujian 361005 China

The reduction and the oxidation of hypophosphite on a Ni-Ag electrode have been studied to provide the information about the phosphorus incorporation mechanisms during the electro-less deposition and the electrodeposition of Ni-P alloys. In the electrooxidation process, an absorbency band around 240 nm, which was ascribed to tbe formation of an intermediate PHO2, was observed by in situ UV-Vis subtractive reflectance spectroscopy. Accordingly, the electrooxidation of hypophosphite might undergo an H abstraction of hypophosphite from the PH bond to form the phosphorus-centred radical PHO2, which was subsequently electrooxidized to the final product, phosphite. In the reduction process Ni-phosphine compound N-(PH3), was observed byin situ surface raman spectroscopy. The results from the raman experiments show that, in the NiSO4-free solution, hypophosphite was reduced only to Ni-phosphine compound, while in the case where NiSO4 coexisted in tbe solutions, the Ni-phosphine compound, as an intermediate, was oxidised by Ni2+ to elemental phosphorus in alloys with nickel acting as the catalyst.

关键词： in situ raman spectroscopy in situ UV-Vis spectroscopy hypophosphite electrooxidation electroreduction

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