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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

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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

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Optimizing 3d spin polarization of CoOOH by in situ Mo doping for efficient oxygen evolution reaction

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Carbon Energy 2024年第1期6卷 236-244页

作者： Zhichao Jia Yang Yuan Yanxing Zhang Xiang Lyu Chenhong Liu Xiaoli Yang Zhengyu Bai Haijiang Wang Lin Yang Key Laboratory of Green Chemical Media and Reactions School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsMinistry of EducationHenan Normal UniversityXinxiangHenanChina School of Physics Henan Normal UniversityXinxiangHenanChina Oak Ridge National Laboratory Electrification and Energy Infrastructures DivisionOak RidgeTennesseeUSA Department of Mechanical and Energy Engineering Key Laboratory of Energy Conversion and Storage TechnologiesSouthern University of Science and TechnologyShenzhenGuangdongChina

Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.

关键词： electrocatalyst in situ raman Mo-doped CoOOH oxygen evolution reaction

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Ultrahigh-performance mesoporous ZnMn2O4 microspheres as anode materials for lithium-ion batteries and their in situ raman investigation

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Nano Research 2018年第7期11卷 3814-3823页

作者： Xiaobin Zhong1 Xiaoxiao wang Huiyuan Wang Zhizheng Yang Yuxiong Jiang Jianfeng Li Zhongqun Tian MOE Key Laboratory of Spectrochemical Analysis and Instrumentation State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China Key Laboratory of Automobile Materials Ministry of Education College of Materials Science and Engineering Jilin University Changchun 130012 China

Currently, lithium-ion batteries play a key role in energy storage; however, their applications are limited by their low energy density. Here, we design a facile method to prepare mesoporous ZnMn2O4 microspheres with ultrahigh rate performance and ultralong cycling properties by finely tuning the solution viscosity during synthesis. When the current density is raised to 2 A·g^-1, the discharge capacity is maintained at 879 mA·h·g^-1 after 500 cycles. The electro- chemical properties of mesoporous ZnMn2O4 microspheres are better than that for most reported ZnMn2O4. To understand the electrochemical processes on the mesoporous ZnMn2O4 microspheres, in situ raman spectroscopy is used to investigate the electrode surface. The results show that mesoporous ZnMn2O4 microspheres have a great potential as an alternative to commercial carbon anode materials.

关键词： ZnMn2O4 mesoporous microspheres viscosity in situ raman ultralong cycling stability

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in situ raman Spectroscopic Study and Adsorption Engineering for COOH* Intermediates during CO2 Electroreduction Reaction

In situ Raman Spectroscopic Study and Adsorption Engineering...

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第二十届全国光散射学术会议（CNCLS20）

作者： Hao Yang Yu-wen Hu Yexiang Tong Jian Chen School of Materials Science and Engineering Sun Yat-sen University School of Chemistry Sun Yat-sen University Instrumental analysis and Research center

The challenge in the artificial CO reduction to fuel is achieved high selective electrocatalysts.Here,we propose a simple strategy to modified CuO/CuO heterostructure nanowires with metal nanoparticles for the intermediates adsorption engineering of COOH* during CO reduction reaction.The CuO/CuO@ nanowires modified by Ni nanoparticles exhibit superior catalytic performance with high faradic efficiency(95% for CO).Theoretical and experimental analyses show that the hybridization of CuO/CuO nanowires and Ni nanoparticles could not only adjust the d-band center of electrocatalysts to enhance the intrinsic catalytic activity but also improve the adsorption of COOH* intermediates and suppressing the hydrogen evolution reaction to promote the CO conversion efficiency during CO reduction reaction.in situ raman spectroscopic study further confirm the existence of COOH* species and the engineering intermediates adsorption.This work offers new insights for facile designing of non-precious transition metal compound heterostructure for CO reduction reaction through adjusting the reaction pathway.

关键词： Cu2O nanowires heterostructure intermediates in situ raman CO2 reduction reaction

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