Chemphyschem最新文献_第8页

Microkinetic Modelling of Electrochemical Oxygen Evolution Reaction on Ir(111)@N-Graphene Surface

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-05 DOI: 10.1002/cphc.202400907

Adyasa Priyadarsini, Bhabani S. Mallik

{"title":"Microkinetic Modelling of Electrochemical Oxygen Evolution Reaction on Ir(111)@N-Graphene Surface","authors":"Adyasa Priyadarsini, Bhabani S. Mallik","doi":"10.1002/cphc.202400907","DOIUrl":"10.1002/cphc.202400907","url":null,"abstract":"We have explored the thermodynamics and microkinetic aspects of oxygen evolution catalysis on low loading of Ir(111) on nitrogen-doped graphene at constant potential. The electronic modification induced by N-doping is the reason for the reduced overpotential of OER. The N-induced defect in the charge density is observed with increasing charge-depleted region around the Ir atoms. The lattice contraction shifts the d-band center away from the Fermi level, which increases the barrier for OH* and O* formation on Ir(111) supported on NGr (Ir(111)@NGr). Thus, highly endothermic O* formation reduces the OOH* formation, which is the potential determining step. For comparison, all electronic and binding energy calculations were also performed against Ir NP supported on Gr (Ir(111)@Gr). The stepwise potential-dependent activation barrier (<math></math>\u0000) was obtained using the charge extrapolation method. The third step remains the RDS in all ranges of water oxidation potentials. The potential dependent <math></math>\u0000 is further applied to the Eyring rate equation to obtain the current density (<math></math>\u0000) and correlation between <math></math>\u0000 and pH dependence, i. e., OH− concentration. The microkinetic <math></math>\u0000 progression leads to a Tafel slope value of 30 mV dec−1 at pH=14.0, requiring <math></math>\u0000.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":"26 7","pages":""},"PeriodicalIF":2.3,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

A First Principle Study to Understand the Importance of Edge-exposed and Basal Plane Defective MoS₂ Towards Nitrogen Reduction Reaction.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-05 DOI: 10.1002/cphc.202400866

Yuan-Hui Xiao, Xin-Wei Wu, Lai-Ke Chen, Zi-Wei Ma, Jian-De Lin, Rajkumar Devasenathipathy, De-Yin Wu, Zhong-Qun Tian

{"title":"A First Principle Study to Understand the Importance of Edge-exposed and Basal Plane Defective MoS2 Towards Nitrogen Reduction Reaction.","authors":"Yuan-Hui Xiao, Xin-Wei Wu, Lai-Ke Chen, Zi-Wei Ma, Jian-De Lin, Rajkumar Devasenathipathy, De-Yin Wu, Zhong-Qun Tian","doi":"10.1002/cphc.202400866","DOIUrl":"10.1002/cphc.202400866","url":null,"abstract":"Nitrogen reduction reaction (NRR) as a promising approach to ammonia synthesis has received much attention in recent years. Molybdenum disulfides (MoS2), as one of the most potential candidates for NRR, are extensively investigated. However, the inert basal plane limits the application of MoS2. Herein, by using density functional theory (DFT) calculations, we constructed edge-exposed MoS2 and different kinds of basal plane defects, including anti-site, sulfur vacancy and pore defects, to systematically investigate their influence on the NRR performance. The thermodynamically calculated results revealed that the NRR on edge-exposed MoS2, anti-site defects, sulfur vacancy with three sulfur atoms missing (S3V) and porous defect (D) exhibit great catalytic activity with low limiting potentials. The calculated limiting potentials are -0.43 and -0.47 V at armchair and zigzag edge MoS2, -0.42 and -0.44 V at anti-site defects, -0.49 and -0.67 V at S3V and D. However, by inspecting the thermodynamic properties of the hydrogen evolution reaction, we proposed that the zigzag-end MoS2 and anti-site defects exhibit a better NRR selectivity compared to armchair-end MoS2, S3V and D. Electronic structure calculations reveals that the edge-exposed and basal plane defective MoS2 can improve the conductivity of the material by reducing the band gap. Donation-backdonation mechanism can effectively promote the activation of nitrogen molecule. Our results pave the way to understanding the defective effects of the MoS2 inertness plane for NRR and designing high-performance NRR catalysts.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202400866"},"PeriodicalIF":2.3,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254776","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Insight into the Coupling of HgS and CuO with Metal-Organic Frameworks Support in Electrocatalytic Oxygen Evolution Reaction.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-05 DOI: 10.1002/cphc.202400956

Mitali Hupele, Ritu Raj, Shikha Rai, Tapasi Sen, Krishna Kanta Haldar

{"title":"Insight into the Coupling of HgS and CuO with Metal-Organic Frameworks Support in Electrocatalytic Oxygen Evolution Reaction.","authors":"Mitali Hupele, Ritu Raj, Shikha Rai, Tapasi Sen, Krishna Kanta Haldar","doi":"10.1002/cphc.202400956","DOIUrl":"10.1002/cphc.202400956","url":null,"abstract":"This study investigates the coupling of mercury sulfide (HgS) and copper oxide (CuO) nanoparticles with metal-organic frameworks (MOFs) as a support material for enhancing the electrocatalytic oxygen evolution reaction (OER). The integration of HgS and CuO into the MOF framework aims to leverage the unique electronic and structural properties of both the nanoparticles and the MOFs to improve catalytic performance. Metal-organic frameworks (MOFs), particularly ZIF-67, are investigated for their potential to catalyze water-splitting reactions due to their high porosity and large specific surface areas. The strategic incorporation of HgS and CuO into ZIF-67 significantly enhances its electrocatalytic properties, resulting in remarkable performance metrics: a low overpotential of 246 mV at 10 mA/cm2, a Tafel slope of 123 mV/dec, an expanded electrochemical active surface area (ECSA) of 23.56 cm2, and a reduced charge transfer resistance of 34.86 Ω. This integration enhances porosity and increases active surface area, which is crucial for improved catalytic performance. This investigation introduces an innovative methodology for fabricating highly efficient electrocatalysts, positioning HgS/CuO/ZIF-67 as a promising candidate for oxygen evolution reactions in alkaline media. The findings highlight the potential of this novel nanocomposite in future clean energy applications, particularly in the realm of water-splitting technologies.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202400956"},"PeriodicalIF":2.3,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143188275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Mechanistic Insights into the Photocatalytic Indigo Carmine Dye Decolorization by Co₃O₄/TiO₂.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-04 DOI: 10.1002/cphc.202400688

Mirjam E de Graaf, Nejc Godec, Bram T Kappé, Roos L Grote, Jitte Flapper, Eline M Hutter, Bert M Weckhuysen

{"title":"Mechanistic Insights into the Photocatalytic Indigo Carmine Dye Decolorization by Co3O4/TiO2.","authors":"Mirjam E de Graaf, Nejc Godec, Bram T Kappé, Roos L Grote, Jitte Flapper, Eline M Hutter, Bert M Weckhuysen","doi":"10.1002/cphc.202400688","DOIUrl":"10.1002/cphc.202400688","url":null,"abstract":"TiO2 is widely studied as an efficient UV-light photocatalyst for organic compound degradation through reactive oxygen species (ROS) generation. TiO2 can be modified to show photocatalytic activity under visible light illumination by combining with visible-light absorbing metal oxides. Here, we investigated Co3O4/TiO2 composite materials as visible-light absorbing photocatalysts, with various weight loadings of Co3O4, for the decolorization of wastewater pollutant indigo carmine. Under green LED light, 1.4 wt% Co3O4/TiO2 showed the highest decolorization rate compared to other weight loadings and bare TiO2. While UV-Vis spectroscopy indicated that Co3O4/TiO2 composite materials and bare TiO2 cause similar dye decolorization behavior, NMR spectroscopy showed that after 24 h, reaction products were present in the reaction mixture for 1.4 wt% Co3O4/TiO2, while TiO2 showed no reaction products. The lack of photocatalytic activity of Co3O4/zeolite and other Co3O4/oxide composite materials suggests a synergistic effect between Co3O4 and TiO2, where a small amount of Co3O4 enables TiO2 to utilize visible light without compromising the surface area available for ROS creation. Lastly, we emphasize the need to be cautious when drawing conclusions regarding the dye degradation, since we showed that decolorization does not necessarily equate to full degradation, using a unique combination of UV-Vis and nuclear magnetic resonance spectroscopy.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202400688"},"PeriodicalIF":2.3,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143188278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

2H,3H-Decafluoropentane Endorsed Localized High Concentration Electrolyte for Low-Temperature Lithium-Metal Batteries. 2H,3H-decafluoropentane endorsed localized high concentration electrolyte for low temperature lithium-metal batteries（用于低温锂金属电池的局部高浓度电解质）。

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-04 DOI: 10.1002/cphc.202400920

Jie Wang, Yubin Liu, Haikuo Lei, Wenbin Sun, Xiaoyu Huang, Yanli Ruan

{"title":"2H,3H-Decafluoropentane Endorsed Localized High Concentration Electrolyte for Low-Temperature Lithium-Metal Batteries.","authors":"Jie Wang, Yubin Liu, Haikuo Lei, Wenbin Sun, Xiaoyu Huang, Yanli Ruan","doi":"10.1002/cphc.202400920","DOIUrl":"10.1002/cphc.202400920","url":null,"abstract":"A lithium-metal battery's electrochemical performance is affected by the kinetics of desolvation and ion transport at low temperatures. Here, we propose a low-temperature lithium-metal battery electrolyte. 1,2-Dimethoxyethane (DME) is used as the solvent, 2H,3H-decafluoropentane (HFC) as the diluent, and a high concentration of lithium bis(fluorosulfonyl)imide (LiFSI) as the solute. The addition of HFC diluent increases the number of anions bound to lithium ions and decreases the number of solvents in the solvation structure, which is conducive to the desolvation process at low temperatures. In addition, the anion-dominated solvation structure is conducive to the formation of an inorganic rich solid electrolyte interface (SEI), which effectively enhances the compatibility of LHCE-HFC electrolyte with lithium metal. The LHCE-HFC achieves ultra-high coulombic efficiency of lithium metal anode in Li||Cu batteries (99.31 %) and Li||Li batteries (1080 h) that have strong fluorine content in the interface. The Li||LiFePO4 (LFP) cells provide a discharge-specific capacity of 92.1 mAh g-1 at 0.2 C at -20 °C and capacity retention of 89.6 % after 200 cycles.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202400920"},"PeriodicalIF":2.3,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143188270","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Cover Feature: Multi-Layer Kesterite-Based Photocathodes for NH3 Photosynthesis from N2 Reduction Reaction (ChemPhysChem 3/2025)

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-04 DOI: 10.1002/cphc.202580302

Juliana Ferreira de Brito, Marina Medina, Hugo Leandro Sousa Santos, Mileny dos Santos Araujo, Marcos Antônio Santana Andrade Jr., Lucia Helena Mascaro

引用次数: 0

Front Cover: Absorption and Excited-State Coherences of Cryogenically Cold Retinal Protonated Schiff Base in Vacuo (ChemPhysChem 3/2025)

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-04 DOI: 10.1002/cphc.202580301

Nikolaj Klinkby, Anne P. Rasmussen, Anders G. S. Lauridsen, Prof. Lars H. Andersen

引用次数: 0

Valence Electron Count-Based Density Functional Theory to Investigate Structural Stability, Optoelectronic and Thermoelectric Properties of New p-Type Half-Heusler Zryau (Y=B, Al) Alloys.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-03 DOI: 10.1002/cphc.202400921

Radja Nour El Imene Bennoui, Walid Adli, Y Al-Douri, Fadila Belkharroubi, Fatima Sidjilani, Abdelkader Bentayeb, Friha Khelfaoui, Nawal Belmiloud, Sid Ahmed Bendella, Lakhdar Alagui, Anis Samy Amine Dib, Mohammed Noureddine Belkaid

{"title":"Valence Electron Count-Based Density Functional Theory to Investigate Structural Stability, Optoelectronic and Thermoelectric Properties of New p-Type Half-Heusler Zryau (Y=B, Al) Alloys.","authors":"Radja Nour El Imene Bennoui, Walid Adli, Y Al-Douri, Fadila Belkharroubi, Fatima Sidjilani, Abdelkader Bentayeb, Friha Khelfaoui, Nawal Belmiloud, Sid Ahmed Bendella, Lakhdar Alagui, Anis Samy Amine Dib, Mohammed Noureddine Belkaid","doi":"10.1002/cphc.202400921","DOIUrl":"10.1002/cphc.202400921","url":null,"abstract":"The full-potential linearized augmented plane wave (FP-LAPW) method within the framework of density functional theory (DFT) and semi-classical Boltzmann transport theory under the constant relaxation time approximation has been employed to investigate the structural, mechanical, optoelectronic and thermoelectric properties of novel half-Heusler (HH) ZrYAu alloys (where Y=B or Al) with a valence electron count (VEC) of 8. Our results indicate that both compounds are mechanically stable in structure Type 1 and possess negative formation energies. Additionally, ZrBAu and ZrAlAu display semiconducting behavior, with ZrBAu showing a direct band gap, 0.753 eV (0.774 eV) at point Γ→X and ZrAlAu exhibiting an indirect band gap, 0.431 eV (0.482 eV) at point Γ→Γ, using the generalized gradient approximation (GGA) and Modified Becke and Johnson-generalized gradient approximation (mBJ-GGA), respectively. Based on optical properties, both ZrBAu and ZrAlAu exhibit high optical conductivity within the visible spectrum. In terms of visible light absorption, ZrBAu primarily absorbs blue light, while ZrAlAu absorbs yellow, blue-green and violet light. However, both compounds are effective absorbers of UV light. Regarding thermoelectric performance, the thermoelectric parameters reveal that ZrBAu and ZrAlAu demonstrate significant p-type thermoelectric power. These half-Heusler alloys have a high-power factor, making them promising candidates for thermoelectric applications.","PeriodicalId":9819,"journal":{"name":"Chemphyschem","volume":" ","pages":"e202400921"},"PeriodicalIF":2.3,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143078734","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Charge Transfer Effect on Relaxation Mechanism in Hydrated Pyrrole-Water Systems Following N-2s Ionization.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-03 DOI: 10.1002/cphc.202400962

Ravi Kumar, Kankana Bhattacharjee, Aryya Ghosh, Nayana Vaval

引用次数: 0

Cyclically Generated Phase Segregation Synergizing with Si Enhances Lithium-Ion Storage Capability.

IF 2.3 3区化学

Chemphyschem Pub Date : 2025-02-03 DOI: 10.1002/cphc.202401007

Haoyuan Zhu, Zaoyan Yu, Yushuai Song, Shun Liu, Luzheng Zhao, Jiancong Guo, Wenruo Li, Xu Han, Zhongsheng Wen

引用次数: 0