IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-29 DOI: 10.1002/cssc.202500281

Yue Wang, Gustavo T Feliciano, Ashwani Kumar, Alexander A Auer, Harun Tüysüz

{"title":"Experimental and Theoretical Insights into the Role of Iron in the Rapidly Fabricated Ni/Fe Electrodes for the Oxygen Evolution Reaction.","authors":"Yue Wang, Gustavo T Feliciano, Ashwani Kumar, Alexander A Auer, Harun Tüysüz","doi":"10.1002/cssc.202500281","DOIUrl":"https://doi.org/10.1002/cssc.202500281","url":null,"abstract":"The development of low-cost electrocatalysts for the oxygen evolution reaction (OER) of water electrolysis is crucial for large-scale green hydrogen production. NiFe-based electrocatalysts have garnered significant attention due to their high OER activity; however, the need for a rapid and efficient electrode fabrication method and a clear understanding of the role of Fe in enhancing OER activity remain unresolved. Herein, we developed a highly active NiFe-based OER electrocatalyst self-supported on carbon fiber paper (CFP) using a versatile and rapid thermal shock method, requiring only 30 seconds of heat treatment. The as-prepared Fe1Ni1/CFP shows a current density of 493 mA/cm2 at 1.7 VRHE and a low overpotential of 247 mV at a current density of 10 mA/cm2, with excellent long-term durability in alkaline conditions. In-situ Raman spectroscopy, pH-dependence activity test, and electronic structure calculations revealed that Fe not only promotes the oxidation of adjacent Ni but also accelerates the deprotonation of -OH groups and stabilizes oxo-intermediates, thus displaying both direct and indirect effects and enhancing the overall OER performance. Our study provides a foundation for developing cost-effective electrocatalysts for green hydrogen production and other sustainable energy applications while enhancing our understanding of the role of Fe in NiO catalysts.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500281"},"PeriodicalIF":7.5,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172391","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Chelation Engineering Revitalizes Iron-Based Redox Flow Batteries. 螯合工程重振铁基氧化还原液流电池。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-29 DOI: 10.1002/cssc.202500697

Wendong Yang, Xue Long, Hua Jiang, Jinhua Guo, Jun Zhou, Jiangjiang Duan

引用次数: 0

Upcycling of Waste Poly(ethylene terephthalate) : Ammonolysis Kinetics of Model Bis(2-hydroxyethyl terephthalate) and Particle Size Effects in Polymeric Substrates. 废弃聚对苯二甲酸乙酯的升级回收：模型双（2-对苯二甲酸乙酯）氨解动力学和聚合物底物中的粒径效应。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202500509

Richard-Joseph L Peterson, Elanna P Neppel, Daniel Holmes, Robert Ofoli, John R Dorgan

{"title":"Upcycling of Waste Poly(ethylene terephthalate) : Ammonolysis Kinetics of Model Bis(2-hydroxyethyl terephthalate) and Particle Size Effects in Polymeric Substrates.","authors":"Richard-Joseph L Peterson, Elanna P Neppel, Daniel Holmes, Robert Ofoli, John R Dorgan","doi":"10.1002/cssc.202500509","DOIUrl":"https://doi.org/10.1002/cssc.202500509","url":null,"abstract":"Upcycling of poly(ethylene terephthalate) (PET) through ammonolysis is pursued. Model studies on bis(2-hydroxyethyl) terephthalate (BHET) reacting with ammonia in excess ethylene glycol (EG) to form terephthalamide (TPD) are presented. Sequential ester conversion is characterized by the pseudo reaction rate constants of = 1.02±0.09 h-1 and = 0.44±0.08 h-1 at 100 ⁰C; these values correspond to second order rate constants of = 0.60±0.05 L mol-1 h-1 and = 0.26±0.05 L mol-1 h-1. Reactions conducted over a range of temperatures yield preexponential factors of A1 = 758±120 L mol-1 h⁻¹ / A2 = 1033±220 L mol-1 h⁻¹ and activation energies of Ea1 = 22.1±1.5 kJ mol-1 / Ea2 = 26.5±2.1 kJ mol-1. Diffusional limitations are explored using particle sizes of 1800-2500 μm, 250-600 μm, and 150-250 μm. Conversion data from the particle size experiments is combined with the rate constants determined from the model studies to construct an effectiveness factor. Diffusional limitations are of profound importance; for particles of only 1 millimeter in average thickness, the conversion rate is decreased by a factor of ten! The comprehensive understanding of the ammonolysis of PET in EG provided can play an important role in improving material reuse and fostering a more circular economy.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500509"},"PeriodicalIF":7.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Single-Atom Mediated d-Band Engineering of Platinum Nanocatalysts for High-Efficiency Acidic Hydrogen Evolution. 高效酸性析氢铂纳米催化剂的单原子介导d波段工程。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202500640

Mi Luo, Bingbao Mei, Linyao Huang, Haiyong Wang, Chenguang Wang

{"title":"Single-Atom Mediated d-Band Engineering of Platinum Nanocatalysts for High-Efficiency Acidic Hydrogen Evolution.","authors":"Mi Luo, Bingbao Mei, Linyao Huang, Haiyong Wang, Chenguang Wang","doi":"10.1002/cssc.202500640","DOIUrl":"https://doi.org/10.1002/cssc.202500640","url":null,"abstract":"The rational construction of single-atom-mediated Pt catalysts with optimized electronic structures and robust stability remains a grand challenge for hydrogen evolution reaction (HER). Herein, we pioneer a spatial confinement coupled with a d-band engineering strategy to fabricate cobalt single-atom coordinated Pt nanocatalysts (Pt@Co-SAs/NC), achieving exceptional HER activity with ultralow Pt loading (0.94 wt%). The Pt@Co-SAs/NC exhibits an overpotential of 15 mV at 10 mA/cm2 (ƞ10) and 21.8-fold enhanced mass activity at 20 mV versus commercial Pt/C, surpassing most reported Pt-based systems. Synchrotron X-ray absorption spectroscopy (XAS) and theoretical studies reveal that the atomically dispersed CoN4 sites adjacent to Pt NPs serve as electronic modulators, inducing a 0.36 eV downshift of the Pt d-band center through interfacial charge redistribution. This electronic engineering weakens hydrogen adsorption strength (ΔGH* =-0.17 eV) while accelerating H2 desorption kinetics. Furthermore, the CoN4-anchored carbon matrix suppresses nanoparticle aggregation and ensures exceptional durability through strong metal-support interactions, maintaining 94.2% activity after 130 h operation. This work establishes an atomic-level electronic modulation paradigm for designing highly efficient, cost-effective, and durable electrocatalysts.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500640"},"PeriodicalIF":7.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Physics-based inverse modeling of battery degradation with Bayesian methods. 基于贝叶斯方法的电池退化物理逆建模。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202402336

Micha Philipp, Yannick Kuhn, Arnulf Latz, Birger Horstmann

{"title":"Physics-based inverse modeling of battery degradation with Bayesian methods.","authors":"Micha Philipp, Yannick Kuhn, Arnulf Latz, Birger Horstmann","doi":"10.1002/cssc.202402336","DOIUrl":"https://doi.org/10.1002/cssc.202402336","url":null,"abstract":"To further improve Lithium-ion batteries (LiBs), a profound understanding of complex battery processes is crucial. Physical models offer understanding but are difficult to validate and parameterize. Therefore, automated machine-learning methods (ML) are necessary to evaluate models with experimental data. Bayesian methods, e.g., Expectation Propagation + Bayesian Optimization for Likelihood-Free Inference (EP-BOLFI), stand out as they capture uncertainties in models and data while granting meaningful parameterization. An important topic is prolonging battery lifetime, which is limited by degradation, such as the solid-electrolyte interphase (SEI) growth. As a case study, we apply EP-BOLFI to parametrize SEI growth models with synthetic and real degradation data. EP-BOLFI allows for incorporating human expertise in the form of suitable feature selection, which improves the parametrization. We show that even under impeded conditions, we achieve correct parameterization with reasonable uncertainty quantification, needing less computational effort than standard Markov chain Monte Carlo methods. Additionally, the physically reliable summary statistics show if parameters are strongly correlated and not unambiguously identifiable. Further, we investigate Bayesian Alternately Subsampled Quadrature (BASQ), which calculates model probabilities, to confirm electron diffusion as the best theoretical model to describe SEI growth during battery storage.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402336"},"PeriodicalIF":7.5,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Controlling Secondary Crystallization with 1-Butanol for High-Efficiency Perovskite Solar Cells. 用1-丁醇控制高效钙钛矿太阳能电池的二次结晶。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202500860

Hao Li, Ying Shang, Wei Meng, Zhangyu Yuan, Kang An, Ning Li

引用次数: 0

Pyrene-derived iron complexes for efficient photocatalytic CO2 reduction. 芘衍生铁配合物用于高效光催化CO2还原。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202500720

Haoxiang Wang, Jianling Zhang, Yingzhe Zhao, Zhonghao Tan, Zhenhuan Wei, Meiling Li, Buxing Han

引用次数: 0

Strategic Engineering of Axially Coordinated Ligands in Fe-N-C Catalysts for Enhanced Oxygen Reduction Electrocatalysis. Fe-N-C催化剂轴向配体增强氧还原电催化的策略工程。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-28 DOI: 10.1002/cssc.202500855

Zongxuan Yang, Qingchen Wu, Hongwei Zhang, Cejun Hu, Xiaojun Bao, Pei Yuan

引用次数: 0

Surface Roughness Engineering for High-Salt-Tolerant Solar Evaporator with Enhanced Efficiency in Sustainable Desalination. 提高可持续海水淡化效率的高耐盐太阳能蒸发器表面粗糙度工程。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-27 DOI: 10.1002/cssc.202500714

Mengxue Zhang, Laigang Hu, Yang Guo, Wenhao Wu, Daohui Lin, Juan Wang, Kun Yang

{"title":"Surface Roughness Engineering for High-Salt-Tolerant Solar Evaporator with Enhanced Efficiency in Sustainable Desalination.","authors":"Mengxue Zhang, Laigang Hu, Yang Guo, Wenhao Wu, Daohui Lin, Juan Wang, Kun Yang","doi":"10.1002/cssc.202500714","DOIUrl":"https://doi.org/10.1002/cssc.202500714","url":null,"abstract":"The accumulation of dense crystal layers on solar evaporators compromises performances by reducing light absorption efficiency and obstructing water transport channels, ultimately diminishing evaporation rate. To mitigate this issue, spatially separated crystallization sites can be engineered on the evaporator surface to disrupt salt adhesion and prevent dense layers formation. In this study, we developed a 3D column-shaped wood evaporator (KAC-DW) by coating delignified wood (DW) with KOH-activated carbon (KAC). The KAC coating creates microstructured surface featuring abundant protrusions (~144 mm-2, each 20 μm in height), which effectively inhibit salt crystal adhesion. Under 1 kW m-2 solar radiation with a 15 wt% NaCl solution, the KAC-DW evaporator achieved an impressive water evaporation rate of 8.18 kg m-2 h-1 over 96 h (0 m s-1 wind speed)-more than double the performance of uncoated DW (3.91 kg m-2 h-1). This enhancement stems from two key mechanisms: (1) the KAC protrusions prevent dense crystal layer formation, preserving open surface channels for evaporation, and (2) they promote the growth of loose salt crystals, thereby expanding the effective evaporation area and further boosting the evaporation rate.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500714"},"PeriodicalIF":7.5,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Ruthenium/Carbon Nanocomposites for Efficient Hydrogen Electrocatalysis: Impacts of Halide Residues. 用于高效氢电催化的钌/碳纳米复合材料：卤化物残留物的影响。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-27 DOI: 10.1002/cssc.202500802

Bingzhe Yu, Qiming Liu, Chaochao Dun, Davida Briana DuBois, Bryan Hou, Dingjie Pan, John Tressel, Kiley Mayford, Colton Jones, Xiao Wang, Qingfeng Ge, Frank Bridges, Shaowei Chen

{"title":"Ruthenium/Carbon Nanocomposites for Efficient Hydrogen Electrocatalysis: Impacts of Halide Residues.","authors":"Bingzhe Yu, Qiming Liu, Chaochao Dun, Davida Briana DuBois, Bryan Hou, Dingjie Pan, John Tressel, Kiley Mayford, Colton Jones, Xiao Wang, Qingfeng Ge, Frank Bridges, Shaowei Chen","doi":"10.1002/cssc.202500802","DOIUrl":"https://doi.org/10.1002/cssc.202500802","url":null,"abstract":"Ruthenium has emerged as a promising substitute for platinum towards the hydrogen evolution/oxidation reaction (HER/HOR). Herein, ruthenium/carbon composites are prepared by magnetic induction heating (300 A, 10 s) of RuCl3, RuBr3 or RuI3 loaded on hollow porous carbon cages (HNC). The HNC-RuCl3-300A sample consists of Ru nanoparticles (dia. 1.96 nm) and abundant Cl residues, HNC-RuBr3-300A possesses a larger nanoparticle size (ca. 19.36 nm) and lower content of Br residues, whereas HNC-RuI3-300A, contains only bulk-like Ru agglomerates with a minimal amount of I residues, due to reduced Ru-halide bonding interactions. Among these, HNC-RuCl3-300A exhibits the best HER activity in alkaline media, with a low overpotential of only -26 mV to reach 10 mA cm-2, even outperforming Pt/C, and can be used as the cathode catalyst for anion exchange membrane water electrolyzer (along with commercial RuO2 as the anode catalyst), producing 0.5 A cm-2 at 1.88 V for up to 100 h, a performance markedly better than that with Pt/C. HNC-RuCl3-300A also exhibits the best HOR activity, with a half-wave potential (+18 mV) even lower than that of Pt/C (+35 mV). These activities are ascribed to the combined contributions of small Ru nanoparticles and Ru-to-halide charge transfer that weaken H adsorption.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500802"},"PeriodicalIF":7.5,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

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