Energy & Fuels最新文献

{"title":"Bio-Oil Production via Two-Stage and Direct Hydrothermal Liquefaction Process from High-Protein Monoraphidium sp. KMC4: A Comparative Study of Both Processes and an Insight into the Reaction Pathway","authors":"Pooja Singh,&nbsp; and ,&nbsp;Kaustubha Mohanty*,&nbsp;","doi":"10.1021/acs.energyfuels.5c0106110.1021/acs.energyfuels.5c01061","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01061https://doi.org/10.1021/acs.energyfuels.5c01061","url":null,"abstract":"<p >Hydrothermal liquefaction (HTL) technology is a process to produce substantial energy resources from potential algae feedstock. However, the high N and O content in wastewater-grown microalgae yields bio-oil with a significant number of heteroatoms, hindering its practical utilization. In this work, the bio-oil generated from direct high-temperature and two-stage hydrothermal liquefaction was compared for its elemental quality and yield. A bio-oil yield of 33.50% was achieved via direct HTL, with high N/C (0.05 mol/mol), H/C (1.36 mol/mol), and O/C (0.11 mol/mol) ratios. The implementation of two-stage hydrothermal liquefaction was applied to increase the H/C and to decrease the N/C of the feedstock, to increase the H/C and to decrease the N/C and the O/C of bio-oil. The aforementioned technology resulted in better bio-oil quality by the prior extraction of carbohydrates and protein components from algae biomass at lower pretreatment temperatures. The bio-oil from direct HTL had a significant number of nitrogen-based compounds (13.36%), i.e., amides, amines, and heterocyclic forms, while it was reduced to 1.98% in the two-stage hydrothermal liquefaction process, confirmed by GC-MS. Also, a reduction of 38% nitrogen in bio-oil was observed from direct HTL compared to two-stage HTL through elemental analysis. The GC-MS results aligned with the elemental analysis of bio-oil from the two-stage hydrothermal liquefaction. The bio-oil produced from two-stage HTL of pretreated microalgae exhibited improved properties, characterized by reduced N-heterocyclic compounds and better elemental composition. The study also formulated the hypothetical reaction pathway during the two-stage HTL. The findings obtained using the two-stage HTL greatly improved the bio-oil characteristics without the expense of reduced yield.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10465–10478 10465–10478"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ultrasonic Treatment Improves the Synergistic Modification Effect of EVA and Asphaltenes on Nanyang Crude Oil","authors":"Fei Yang,&nbsp;Baiwu Zhu,&nbsp;Chuanxian Li,&nbsp;Guangyu Sun,&nbsp;Yougang Wang,&nbsp;Bo Yao* and Xinyuan Li,&nbsp;","doi":"10.1021/acs.energyfuels.5c0056810.1021/acs.energyfuels.5c00568","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00568https://doi.org/10.1021/acs.energyfuels.5c00568","url":null,"abstract":"<p >The synergistic effect of asphaltenes and PPDs (Pour Point Depressants) on improving the low-temperature rheological properties of waxy crude oils has been extensively studied. Based on these studies, exploring a feasible method to improve the synergistic effect between PPDs and asphaltenes is greatly significant for the safe and economical transportation of waxy crude oils. This paper investigates the effects of different ultrasonic treatment durations (0–30 s, fixed at 20 kHz and 900 W) on the low-temperature fluidity of Nanyang crude oil with/without 100 ppm of EVA. The results of the pour point test, rheological test, DSC test, and microscopic observation show that ultrasonic treatment slightly improves the low-temperature fluidity of Nanyang crude oil without EVA PPDs. However, ultrasonic treatment has a very significant improvement effect on the low-temperature fluidity of Nanyang crude oil containing 100 ppm of EVA, and this effect is improved with the increase of ultrasonic treatment time. This indicates that ultrasonic treatment and EVA have a synergistic effect on the fluidity improvement of Nanyang crude oil. Combined with the results of the asphaltene dispersibility test, the mechanism of the synergistic effect of ultrasonic treatment and EVA on the fluidity improvement of Nanyang crude oil is discussed. Ultrasonic treatment improves the dispersibility of asphaltenes in Nanyang crude oil through cavitation and mechanical vibration, promotes the adsorption of asphaltenes by EVA, and improves the synergistic effect between EVA and asphaltenes. The discovery of this phenomenon enriches the research on the synergistic modification effect of PPDs and asphaltenes on waxy crude oil and provides insights into the application of ultrasonic treatment technology to improve the fluidity of waxy crude oil.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10304–10313 10304–10313"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211843","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Review and Perspectives on Enhancing the Hydrogen (H2) Storage Capacity and Stability in Geological Formations via Nanoparticle-Assisted Surfactant/Polymer Formulations","authors":"Erasto E. Kasala*,&nbsp;Jinjie Wang*,&nbsp;Asia Majid,&nbsp;Mbula Ngoy Nadege and Edwin E. Nyakilla,&nbsp;","doi":"10.1021/acs.energyfuels.5c0124910.1021/acs.energyfuels.5c01249","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01249https://doi.org/10.1021/acs.energyfuels.5c01249","url":null,"abstract":"<p >Despite numerous laboratory and simulation findings with great potential, nanoparticles (NPs), surfactants, and polymers used for enhancing hydrogen (H₂) storage capacity and stability in geological formations face significant challenges. Their long-term stability is compromised in the harsh conditions of sediment heterogeneity, overly high pressure and temperature, pH changes, sediment interactions, and fluctuation in salinity, which impede large-scale implementation. Incorporating NPs into surfactants and polymers yields a nanofluid revealing increased viscosity, enhanced dispersion, improved wettability, enhanced surface interaction, H₂ uptake, H₂ solubility, increased retention, and long-term stability─ultimately leading to long-term H₂ storage efficiency, all attributable to the synergistic effects of their components. In this research, the performance efficiency of NP-assisted surfactant/polymer formulations and the factors that impair their effectiveness were highlighted. Numerous NP-assisted surfactant/polymer formulations’ adsorption/absorption mechanisms, such as size-dependent interactions, surface charge effects, aggregation behavior, interfacial tension (IFT) modulation, H₂ bonding, and hydrophobic interactions on the aqueous phase, were illustrated. The synergistic interaction of NP-assisted surfactant or polymer to the IFT reduction, improved rheological properties, flow stability, H₂ adsorption, dispersion efficiency, phase retention, enhanced storage capacity, and long-term stability were also presented. Nevertheless, the extent of the synergy observed depends on the specific type and property of NPs, surfactants, or polymers used. In addition, the review highlighted the existing challenges, research gaps, and proposed potential interventions. The research uniquely bridges the gap between molecular-level interactions and field-scale applications, offering a novel synthesis of experimental and simulation data to propose actionable solutions for overcoming current limitations in H₂ storage technology. By focusing on the underexplored synergy of nanoparticle-surfactant/polymer systems in geological H₂ storage, this work advances the understanding of how nanoscale modifications can optimize macroscale storage efficiency and stability.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10165–10199 10165–10199"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effects of CO2-Induced Geochemical Reactions on Sandstone and Limestone Reservoirs in Mae Moh Basin: Insights from Subcore to Core Scale Analyses","authors":"Mathurot Tulapan,&nbsp;Vorasate Thanasaksukthawee,&nbsp;Chetsada Tapanya,&nbsp;Teerapat Tosuai,&nbsp;Jiatong Jiang,&nbsp;David Harbottle and Suparit Tangparitkul*,&nbsp;","doi":"10.1021/acs.energyfuels.5c0112910.1021/acs.energyfuels.5c01129","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01129https://doi.org/10.1021/acs.energyfuels.5c01129","url":null,"abstract":"<p >CO₂ capture and storage (CCS) is emerging as a key technology for climate change mitigation, particularly in emerging economies like Thailand, where fossil-based energy remains dominant, yet environmental concerns necessitate sustainable solutions. The Mae Moh Basin, home to a coal-fired power plant and its adjacent mine, has been considered as a potential CCS site. The current study investigates CO₂-induced geochemical reactions in the basin’s sandstone and limestone reservoirs, analyzing mineralogical and physical alterations across subcore to core scales using outcrop samples. Experimental results reveal that both sandstone and limestone undergo mineral dissolution, particularly carbonate dissolution in an acidified CO₂-rich environment. Reprecipitation of minerals was also observed, confirmed through microstructural imaging, X-ray diffraction, and morphological analyses. At the subcore scale, sandstone exhibited microcracks and expanded corrosion pits, while needle-like aragonite crystals reprecipitated on the limestone surface. These geochemical alterations led to increased porosity and permeability, though the effect remained limited due to the low-permeability nature of these tight reservoirs. Computerized tomography (CT) scanning further confirmed pore-space expansion, particularly in limestone, where carbonate dissolution was more pronounced. While CO₂-induced mineral dissolution suggests enhanced injectivity, uncontrolled permeability increases could pose risks of CO₂ migration, potentially affecting long-term containment security. The current findings provide detailed geochemical insights into the Mae Moh Basin’s reservoir properties, although further research─particularly geochemical-geomechanical coupling and field-scale assessments─is necessary to ensure the safe and effective deployment of CO₂ storage in the basin.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10518–10525 10518–10525"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.energyfuels.5c01129","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoding the Effect of Anion Identity on the Solubility of N-(2-(2-Methoxyethoxy)ethyl)phenothiazine (MEEPT)","authors":"Anton S. Perera,&nbsp;Yilin Wang,&nbsp;Sashen Ruhunage,&nbsp;Lily A. Robertson,&nbsp;T. Malsha Suduwella,&nbsp;Sean R. Parkin,&nbsp;Randy H. Ewoldt,&nbsp;Chad Risko* and Aman Preet Kaur*,&nbsp;","doi":"10.1021/acs.energyfuels.5c0047210.1021/acs.energyfuels.5c00472","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00472https://doi.org/10.1021/acs.energyfuels.5c00472","url":null,"abstract":"<p >Variations in the solubility of redox-active organic molecules (ROM) of interest for nonaqueous redox flow batteries (RFB), especially as the ROM state-of-charge changes during charge–discharge cycling, present significant molecular design challenges. The situation is further complicated as ROM solubility can be regulated by the choice of electrolyte salt and solvent that together with the ROM comprise the catholyte or anolyte (redox electrolyte) formulation, presenting materials design challenges. The ROM <i>N</i>-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT) is a viscous liquid at room temperature and is miscible in several organic solvents, including acetonitrile and propylene carbonate. The MEEPT radical cation (MEEPT^+•) paired with tetrafluoroborate (BF₄^–) in acetonitrile presents a 0.5 M solubility, a dramatic decrease when compared to the viscous liquid of neutral MEEPT. Here we present a joint experimental, regression modeling, and molecular dynamics (MD) simulations investigation to explore MEEPT–X (where X represents the counteranion) salt solubility variability as a function of concentration and counteranion chemistry in acetonitrile. We find a strong dependence of the salt solubility on the counteranion and relate these findings to explicit intermolecular interactions between MEEPT^+• and the counteranion in the electrolyte solution.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10649–10658 10649–10658"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Resolution Mass Spectrometry Reveals Heteroatom-Based Compositional Trends Linked to Jet Fuel Instability","authors":"Mark Romanczyk*,&nbsp;Jeffrey A. Cramer,&nbsp;Kristina M. Myers and Thomas N. Loegel,&nbsp;","doi":"10.1021/acs.energyfuels.5c0144410.1021/acs.energyfuels.5c01444","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01444https://doi.org/10.1021/acs.energyfuels.5c01444","url":null,"abstract":"<p >When exposed to high heat, the nitrogen- and oxygen-containing compounds (NCCs and OCCs, respectively) in fuels react to form oxidative deposits that may result in fuel failures. Due to the complexity of fuel, it is arduous to assign which class(es) of NCCs and OCCs exhibit the greatest propensities to form these adverse deposits. Hence, there is a burgeoning need to qualitatively characterize stable and thermally unstable jet fuels and compare their compositions. If links between compositions and fuel stability are realized, the harmful compounds can be identified and targeted for removal, consequently improving the fuel quality. The central aims of this work were to (1) qualitatively characterize ionized NCCs and OCCs derived from stable and unstable jet fuels, (2) compare and contrast the NCC and OCC compositions of stable and unstable fuels, (3) denote links between composition and thermally unstable fuels, and (4) utilize automated cluster optimization via serial variable down-selection and singular value decomposition to confirm manual assessments of data linkages. To complete the characterization, (+) and (−) electrospray ionization coupled to a high-resolution Orbitrap mass spectrometer was utilized. Upon measurement, the unstable fuels had greater abundances of OCCs with ≥2 oxygen atoms and ions with empirical formulas of C_<i>n</i>H_{(2<i>n</i>-1)}O₂, C_<i>n</i>H_{(2<i>n</i>-3)}O₂, and C_<i>n</i>H_{(2<i>n</i>-5)}O₂. Furthermore, although stable fuels contained a balanced distribution of different classes of NCCs, unstable fuels had a relatively large abundance of ions with a specific empirical formula of C_<i>n</i>H_2<i>n</i>-6N. Additional qualitative information was reported, including Kendrick Mass Defect plots. Overall, NCC and OCC compositional differences were noted when stable and unstable fuels were compared, highlighting the proficiency of the Orbitrap at characterization. Although it remains uncertain if these differences are responsible for fuel failure, the emergence of links between fuel compositions and thermal instability may prove critical at identifying the class(es) that pose the most harm to fuel.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10331–10345 10331–10345"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211886","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent Advances in Flow Through Porous Media for Energy Exploitation","authors":"Jianchao Cai*,&nbsp; and ,&nbsp;Steffen Berg*,&nbsp;","doi":"10.1021/acs.energyfuels.5c0215110.1021/acs.energyfuels.5c02151","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c02151https://doi.org/10.1021/acs.energyfuels.5c02151","url":null,"abstract":"","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 20","pages":"9181–9184 9181–9184"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104884","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Analysis of Hydrate Formation Kinetics and Wall-Climbing Growth Regulation Using Biofriendly Promoters: Synergistic Effects of Erioglaucine Disodium Salt and Sugar Alcohol","authors":"Kunlin Ma,&nbsp;Dongliang Li*,&nbsp;Jingsheng Lu,&nbsp;Decai Lin and Deqing Liang,&nbsp;","doi":"10.1021/acs.energyfuels.5c0099610.1021/acs.energyfuels.5c00996","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00996https://doi.org/10.1021/acs.energyfuels.5c00996","url":null,"abstract":"<p >The high toxicity, excessive foaming, and wall-climbing behavior of traditional promoters limit their large-scale use in hydrate-based gas storage and separation. Environmentally friendly and efficient hydrate management strategies are needed. We used a sapphire cell for comparative analysis of kinetic dynamics and wall-climbing morphology during hydrate formation under sugar alcohol (SA) and erioglaucine disodium salt (EDS). Microscopic analyses explored the mechanisms of EDS and SA on hydrate formation, with comparisons to amino acids. This is the first report on the synergistic effects of SA and EDS, both of which exhibit excellent biocompatibility and degradability, not only in significantly enhancing hydrate formation but also in regulating hydrate wall-climbing behavior. Three distinct modes of hydrate wall-climbing were observed at varying concentrations of EDS and SA. At a concentration of 4 ppm EDS + SA, hydrates exhibited an “antenna growth” mode, characterized by delayed promotion and a significantly prolonged induction time compared to the film formation time. In contrast, 200 ppm EDS + SA demonstrated a strong synergistic effect, drastically reducing both film formation and induction times. Microscopic characterizations revealed that while EDS + SA enhanced the selectivity of the hydrate for CO₂, it did not alter the hydrate cage structure. Optical microscopy results further demonstrate that EDS + SA can inhibit the capillary growth of hydrates and alter their crystal morphology. These findings suggest a mechanism in which a hydrophobic skeletal network promotes hydrate formation and regulates wall-climbing behavior. The EDS + SA combination holds promise for large-scale hydrate applications, offering efficient promotion and wall-climbing control.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10374–10393 10374–10393"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211798","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Insight into Underground Hydrogen Storage in Aquifers: Current Status, Modeling, Economic Approaches and Future Outlook","authors":"Babalola Aisosa Oni*,&nbsp;Ismail Akamu Adebayo,&nbsp;Victor Oyebamiji Ojo and Christopher Nkansah,&nbsp;","doi":"10.1021/acs.energyfuels.5c0148810.1021/acs.energyfuels.5c01488","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c01488https://doi.org/10.1021/acs.energyfuels.5c01488","url":null,"abstract":"<p >Aquifers are considered one of the most eco-friendly forms of underground hydrogen storage due to their widespread availability, natural porosity, minimal requirement for structural modification, and reduced environmental disruption compared to other options, such as salt caverns or depleted reservoirs. However, the number of active aquifer-based hydrogen storage projects is limited, as most current storage efforts focus on depleted fields and salt caverns. Unlike salt caverns, which require extensive mining and energy-intensive leaching processes or depleted reservoirs that may pose risks of residual hydrocarbons contaminating stored hydrogen, aquifers typically involve fewer invasive preparatory measures. Additionally, their wide geographical distribution makes them accessible without significant infrastructure development, reducing the carbon footprint associated with site preparation and operation. With careful monitoring to mitigate risks, such as microbial hydrogen consumption, aquifers offer a sustainable and less intrusive alternative for large-scale hydrogen storage. This is crucial for scaling up hydrogen as a primary energy carrier in global decarbonization efforts. While aquifers show high potential, their use for hydrogen storage remains underdeveloped, requiring significant research and development investment. Hydrogen’s interaction with aquifer materials poses risks, necessitating rigorous site assessments and mitigation strategies. Despite existing challenges, economic assessments indicate that aquifer costs are unpredictable due to a lack of reservoir characterization. This review further discusses the geological properties, H₂ loss pathway and mitigation strategies, sealing technologies, potential storage sites, challenges and economic analysis of H₂ storage in aquifers.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10274–10303 10274–10303"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tin Oxide with Trace Metallic Rhodium (0) Impurity for Overall Water Splitting Reaction: Impact of Rh Loading and Twin Boundaries","authors":"Ashawari Dewri,&nbsp;Gaurisankar Phukan,&nbsp;Salma A. Khanam,&nbsp;Donguk Kim,&nbsp;Young-Bin Park and Kusum K. Bania*,&nbsp;","doi":"10.1021/acs.energyfuels.5c0090310.1021/acs.energyfuels.5c00903","DOIUrl":"https://doi.org/10.1021/acs.energyfuels.5c00903https://doi.org/10.1021/acs.energyfuels.5c00903","url":null,"abstract":"<p >Tin oxide (SnO₂) loaded with a variable concentrations of metallic rhodium (Rh) was explored for the overall splitting of water (H₂O) in an alkaline medium. Three different catalysts, viz. Rh-SnO₂-I, Rh-SnO₂-II and Rh-SnO₂-III, with different Rh-to-Sn ratios, were evaluated for simultaneous oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) processes in 1 M KOH. The catalyst Rh-SnO₂-I, with low Rh loading, showed better OER activity with an onset potential of 1.45 V and an overpotential (<i>η</i>) of 240 mV, while the same for HER was found to be 470 mV. The Rh-SnO₂-II catalyst, with Rh loading slightly higher than that of Rh-SnO₂-I, showed OER activity with <i>η</i> = 250 mV and HER activity with <i>η</i> = 226 mV. The Rh-SnO₂-III catalyst, with the highest Rh content and twin boundaries, was found to show superior HER activity with <i>η</i> of 222 mV at a current density (J) of 10 mAcm^–2. The OER and HER activity in all cases were found to decrease at low pH. Tafel plot analysis and other comparative studies indicated that the loading of Rh into SnO₂ substantially altered the OER and HER activity. The lowest Tafel slope of 200 mVdec^–1 in OER was found in the case of Rh-SnO₂-I. Rh-SnO₂-III catalyst had the lowest Tafel slope value of 128 mVdec^–1 in HER. The current study implied that the introduction of Rh in SnO₂ can improve the HER activity and OER activity depending on the loading of Rh content. Density Functional Theory (DFT) calculations were used to understand the mechanism of overall water-splitting reactions. The study suggested that the water-splitting reaction would be more favorable if the hydrolysis process proceeded through the abstraction of hydrogen (H₂) at the Rh center. The formation of the Sn–H bond during the second H₂ molecule liberation was detected to be the rate-determining step.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 22","pages":"10594–10609 10594–10609"},"PeriodicalIF":5.2,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}