Chinese Journal of Chemical Physics最新文献_第2页

Frequently Encountered Factors Which Obstruct Evaluation of Intrinsic Kinetics of Hydrogen Electrocatalytic Reaction 阻碍氢电催化反应本征动力学评价的常见因素

4区化学

Chinese Journal of Chemical Physics Pub Date : 2025-01-01 DOI: 10.1063/1674-0068/cjcp2503029

引用次数: 0

Kinetics of CH ₂ OO Reactions with Fluorinated Compounds: Temperature-Dependent Study of CF ₃ CH=CHCF ₃ and Upper Limit Determination for SF ₆ 甲烷与氟化化合物反应动力学：cf3ch = chcf3的温度依赖性研究和sf6的上限测定

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Chinese Journal of Chemical Physics Pub Date : 2025-01-01 DOI: 10.1063/1674-0068/cjcp2509131

引用次数: 0

Tuning Mechanism of Optical Bandgap in CsPbBr_xCl_3−x Single-Crystal Microplatelets via Halide Hybridization 卤化物杂交CsPbBrxCl3−x单晶微血小板光学带隙调谐机制

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Chinese Journal of Chemical Physics Pub Date : 2025-01-01 DOI: 10.1063/1674-0068/cjcp2505063

引用次数: 0

Solvent-dependent Photophysical Dynamics of Nitro-substituted Triphenylamine: Insights from Spectroscopies and DFT Calculations 硝基取代三苯胺的溶剂依赖光物理动力学：来自光谱和DFT计算的见解

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Chinese Journal of Chemical Physics Pub Date : 2025-01-01 DOI: 10.1063/1674-0068/cjcp2503031

引用次数: 0

Donor-Acceptor Engineering in Ca-doped NiOOH as a Stable Electrocatalyst for Urea Oxidation Reaction 掺钙NiOOH作为尿素氧化反应稳定电催化剂的供体-受体工程研究

4区化学

Chinese Journal of Chemical Physics Pub Date : 2025-01-01 DOI: 10.1063/1674-0068/cjcp2508111

Naiyuan Duan, Tianxin Hou, Tiezhu Liu, Runlong Yang, Dongdong Wang, Yang Yang, Qianwang Chen

{"title":"Donor-Acceptor Engineering in Ca-doped NiOOH as a Stable Electrocatalyst for Urea Oxidation Reaction","authors":"Naiyuan Duan, Tianxin Hou, Tiezhu Liu, Runlong Yang, Dongdong Wang, Yang Yang, Qianwang Chen","doi":"10.1063/1674-0068/cjcp2508111","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2508111","url":null,"abstract":"The thermodynamic barrier of the anodic oxygen evolution reaction in water electrolysis for green hydrogen production is high, significantly increasing energy consumption and hydrogen production costs. Replacing oxygen evolution reaction with the urea oxidation reaction (UOR) can substantially reduce the voltage, offering advantages in energy efficiency and cost. However, catalysts for urea oxidation face challenges of declining activity during prolonged operation, which severely limits catalyst lifespan and hinders the industrial application of urea oxidation reaction as an alternative to oxygen evolution reaction. Here we show that a calcium-doping strategy enabling spontaneous electron transfer to nickel atoms effectively avoid catalyst deactivation induced by over-oxidation. This electron-buffering mechanism, confirmed through X-ray photoelectron spectroscopy binding energy shifts and stability tests, sustains active Ni3+ sites during prolonged urea oxidation operation. Density functional theory calculations elucidate the catalytic activity enhancement mechanism driven by calcium doping, revealing fundamental electronic and energetic modifications at the atomic scale. The catalyst Ca-NiOOH achieves a current density of 100 mA·cm−2 at 1.46 V for 400 h without significant decay. The longevity of catalysts for urea oxidation reaction is significantly enhanced.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147900388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unraveling ethylene carbonate-propylene carbonate disparity at electrode interface using femtosecond sum frequency generation vibrational spectroscopy 用飞秒和频产生振动光谱分析电极界面上的碳酸乙烯-碳酸丙烯差异

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Chinese Journal of Chemical Physics Pub Date : 2024-11-04 DOI: 10.1063/1674-0068/cjcp2408102

Zhuo Wang, Xiaoxuan Zheng, Zijian Ni, Shuji Ye

{"title":"Unraveling ethylene carbonate-propylene carbonate disparity at electrode interface using femtosecond sum frequency generation vibrational spectroscopy","authors":"Zhuo Wang, Xiaoxuan Zheng, Zijian Ni, Shuji Ye","doi":"10.1063/1674-0068/cjcp2408102","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2408102","url":null,"abstract":"Ethylene carbonate (EC) is an important electrolyte used in lithium-ion batteries due to its excellent electrochemical performance. However, propylene carbonate (PC) differs from EC by only one methyl substituent and exhibits markedly poorproperties. The EC-PC disparity is still poorly understood at the molecular level. In this study, we demonstrated that femtosecond broadband sum frequency generation vibrational spectroscopy (SFG-VS) with simultaneous measurement of multiple polarization combinations provides a powerful probe for investigating the physicochemical processes at the electrode-electrolyte interface during the charge-discharge cycles of lithium batteries. Using monolayer graphene as the working electrode, we observed the distinct reaction outcomes of EC and PC on the electrode surface. The interfacial reaction of EC occurred only in the first charge-discharge cycle, while the interfacial reaction of PC was ongoing along with the charge-discharge cycles, which explains why EC is a better electrolyte choice than PC. This study provides direct experimental evidence in elucidating the differences in interfacial performance between EC and PC, facilitating a deeper understanding of battery interface reactions and guiding the design of high-performance lithium-ion batteries.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"37 6","pages":"729-736"},"PeriodicalIF":0.0,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147910245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 3

Removing Fermi resonance through deuterated molecules with single C–H bond in C–H stretching region of Raman spectra 通过拉曼光谱C-H拉伸区单键氘化分子去除费米共振

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Chinese Journal of Chemical Physics Pub Date : 2024-11-04 DOI: 10.1063/1674-0068/cjcp2408117

Nisar Ullah, Zhirun Jiao, Jialin Bai, Zhiqiang Wang, Ruiting Zhang, Lin Ma, Ke Lin

引用次数: 8

Mechanistic study of initial quenching process in photocatalytic α-keto acids radical acylation: A general strategy for enhancing quantum efficiency 光催化α-酮酸自由基酰化初始猝灭过程的机理研究：提高量子效率的一般策略

4区化学

Chinese Journal of Chemical Physics Pub Date : 2024-09-16 DOI: 10.1063/1674-0068/cjcp2407098

Zhicong Lin, Jialu Li, Chenli Chen, Linan Zhou, Jialong Jie, Hongmei Su

{"title":"Mechanistic study of initial quenching process in photocatalytic α-keto acids radical acylation: A general strategy for enhancing quantum efficiency","authors":"Zhicong Lin, Jialu Li, Chenli Chen, Linan Zhou, Jialong Jie, Hongmei Su","doi":"10.1063/1674-0068/cjcp2407098","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2407098","url":null,"abstract":"The photocatalytic decarboxylation of α-keto acids to generate acyl radicals under mild conditions represents a novel strategy in organic synthesis. However, the quantum efficiency of this process has been underexplored, limiting its practicality. To improve quantum efficiency, detailed analysis of mechanisms and kinetic data for key steps are essential. In this work, using time-resolved emission and absorption spectroscopy, we conducted a mechanistic study focusing on the excited-state properties of representative photocatalysts and their quenching efficiencies during the initial quenching process ([Ir(dFCF3ppy)2(dtbbpy)]+ (IrIII), Eosin Y (EY), Rose Bengal (RB), and 4CzPN). Our findings revealed that RB is active in its triplet states (3RBH*), with lifetimes of 103 ns (in air) and 3.4 µs (in anaerobic conditions), while EY and 4CzPN are active in their singlet states (1EYH* and 14CzPN*), with lifetimes of 2.9 ns and 5.1 ns, respectively. We measured the second-order rate constants for quenching by electron transfer from α-keto acids: 1EYH*, 2.3 × 109 (mol/L)-1 · s−1; 3RBH*, 3.2 × 108 (mol/L)-1 · s−14CzPN*, 2.8 × 108 (mol/L)-1 · s−1. With our previously reported data for Mil, we established the quenching efficiency relationships for these photocatalysts with α-keto acids concentration. Our steady-state chromatography experiments determined the quantum efficiencies for consumption of α-keto acids (IrIII &gt; RBH &gt; EYH &gt; 4CzPN), correlating these efficiencies with the initial quenching process. The results suggest that IrIII/RBH under anaerobic conditions could be optimal for high quantum efficiency. This study provides a foundation for designing new photocatalytic α-keto acid radical acylation systems with enhanced quantum efficiency.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"37 6","pages":"878-892"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147889069","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect of pH on (bi)phosphate adsorption at Pd(111) electrode pH对Pd（111）电极吸附（bi）磷酸盐的影响

4区化学

Chinese Journal of Chemical Physics Pub Date : 2024-09-16 DOI: 10.1063/1674-0068/cjcp2404053

Ke-Yu He, Zhen Wei, Bai-Quan Zhu, Meng-Ke Zhang, Jun Cai, Yan-Xia Chen

{"title":"Effect of pH on (bi)phosphate adsorption at Pd(111) electrode","authors":"Ke-Yu He, Zhen Wei, Bai-Quan Zhu, Meng-Ke Zhang, Jun Cai, Yan-Xia Chen","doi":"10.1063/1674-0068/cjcp2404053","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2404053","url":null,"abstract":"Phosphoric acid/phosphate solutions are commonly used as buffer solutions in the fundamental studies in electrochemistry. Information on the nature of adsorbed (bi)phosphate as well as the domain structures is of great importance in unveiling the impact on electrochemical processes occurring at electrode electrolyte interface. In this work, the pH effect on the adsorption of phosphate related species on Pd(111) electrode has been investigated by cyclic voltammetry over a broad pH range from 1 to 14. After carefully analyzing the related onset desorption potential of (bi)phosphate adsorbate to the thermodynamic equilibrium potential of the corresponding electrode reactions, three different phosphate related adsorbates have been identified, which are highly pH-dependent. Our analysis reveals that the dominant phosphate anions in bulk solution undergo deprotonation upon adsorption. At pH&lt;1.5, the main adsorbate on Pd(111) is H2PO4λ1−; in solutions with 1.5 &lt; pH &lt; 7, the main adsorbate changes into HPO4λ2−. At higher pHs, PO4λ3− on electrode surface dominates. The exact charging value of λi, which represents the true valence of the (bi)phosphate adsorbate, could be determined using theoretical calculations. In addition, our results can not rule out the possibility of co-adsorbed H3PO4 molecules on Pd(111) at pH &lt; 1.5, which needs to be proved by infrared spectroscopy in the future.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"38 3","pages":"281-290"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147900918","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 1

Fabrication and STM characterization of spiral MoS2-graphene/SiC heterostructure 螺旋mos2 -石墨烯/SiC异质结构的制备及STM表征

4区化学

Chinese Journal of Chemical Physics Pub Date : 2024-09-16 DOI: 10.1063/1674-0068/cjcp2406080

Wenyuan Wang, Chenxi Huang, Li Wang, Jun Fu, Xiaodong Zhang, Wenrui Lai, Dianyu Jin, Hualing Zeng, Xiang Shao, Qi Chen

{"title":"Fabrication and STM characterization of spiral MoS2-graphene/SiC heterostructure","authors":"Wenyuan Wang, Chenxi Huang, Li Wang, Jun Fu, Xiaodong Zhang, Wenrui Lai, Dianyu Jin, Hualing Zeng, Xiang Shao, Qi Chen","doi":"10.1063/1674-0068/cjcp2406080","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2406080","url":null,"abstract":"Two-dimensional (2D) heterostructures comprising of differently stacking atomic layers are attractive owing to its flexible composition as well as the emerging new physicochemical properties. However, so far many 2D vertical heterojunctions are constructed through transfer methods, inevitably introducing interfacial impurities and thus hindering detailed atomic-level studies. In this work, we have developed a clean two-step fabrication strategy by combining ultrahigh vacuum (UHV) molecular beam epitaxy (MBE) growth with ambient chemical vapor deposition (CVD). We firstly grew single crystalline graphene film on a SiC substrate under UHV condition, and then synthesized MoS2 films on the graphene-SiC surface through CVD under inert atmosphere, thus successfully realized the construction of a well-defined MoS2-graphene/SiC heterojunction with clean surface. Particularly, we observed the MoS2 can not only grow into monolayer flakes but also form spiral structures, the latter showing layer-by-layer stacks with reduced bandgap down to ∼1.0 eV.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"38 4","pages":"471-478"},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147892123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0